Magnetic Field Reversal Effect in Inter-Landau Level Absorption, and Stimulated Spin-Flip Raman Scattering in n-Type InSb by Gervais F. Favrot, Jr. B.A., Williams College (1970) Submitted to the Department of Physics in partial fulfillment of the requirements for the degree of Doctor of Philosophy at the MASSACHUSETTS INSTITUTE OF TECHNOLOGY September, 1998 © 1998 Gervais F. Favrot, Jr. All rights reserved. The author hereby grants to MIT permission to reproduce and to distribute publicly paper and electronic copies of this thesis document in whole or in part. Signature of Author Department of Physics September, 1998 Certified by Don Heiman Professor of Physics, Northeastern University Supervisor -Thesis Certified by Peter A. lif Professor of Physics Thesis Supery or I Accepted by I , / MASSACHUSETTS INSTITUTE OCT 09108 LIBRARIES Thom . Greytak Professf'r of Physics Chairman, Departmental Committee on Graduate Students Magnetic Field Reversal Effect in Inter-Landau Level Absorption, and Scattering in n-Type InSb Raman Stimulated Spin-Flip by Gervais F. Favrot, Jr. Submitted to the Department of Physics in September 1998 in partial fulfillment of the requirements for the degree of Doctor of Philosophy ABSTRACT This thesis is a theoretical and experimental study of inter-Landau level Three main topics are considered: (i) The first transitions in n-type InSb. observation was made of a magnetic field reversal effect in a spin-conserving (ii) Advancements were made in the inter-Landau level absorption transition. (iii) Experiments theory of intraband absorption and scattering processes. were carried out on the spin-flip Raman laser to examine crystal anisotropy. An important feature of this research is the prediction and observation of a level inter-Landau in the effect reversal field magnetic striking magnetoabsorption in n-InSb. The magnitude of the absorption associated with two transitions is observed to change by a factor of nearly 3 upon reversal of The effect results from the inversion asymmetry of magnetic field direction. The transitions which show the effect the tetrahedral zincblende structure. are the double cyclotron resonance and the double cyclotron resonance combined with spin-flip. The reversal effect involves the interference between two matrix elements which contribute to the absorption, one having tetrahedral symmetry, and the The tetrahedral matrix element results from the other spherical symmetry. The isotropic matrix element is associated inversion-asymmetry mechanism. with the wave vector-dependent electric quadrupole EQ and magnetic dipole MD The isotropic matrix element changes sign on reversal of q, and absorption. the one for inversion asymmetry changes sign on reversal of B, so the interference term changes sign on reversal of either q or B. Stimulated spin-flip Raman (SFR) scattering has been studied in applied For 10-gm pumping, the SFR laser output is magnetic fields up to 18 T. dominated by structure associated with linear intraband absorption and shows significant anisotropy with regard to crystal orientation in the applied Calculations have been made for the transition matrix elements and field. intraconduction-band anisotropic the for coefficients absorption transitions warping-induced The theory includes magneto-optical transitions. model. Brown and and the effects of band nonparabolicity in the Pidgeon Reasonable agreement between theory and experiment is obtained. Thesis Supervisor: D. Heiman, Professor of Physics, Northeastern University Thesis Supervisor: Peter A. Wolff, Professor of Physics TABLE OF CONTENTS LIST OF TABLES 3 5 7 11 1. INTRODUCTION 13 2. THEORY OF INTER-LANDAU LEVEL TRANSITIONS 2.1 Overview 2.2 Formulation of the Effective Mass Theory for Magnetoabsorption 2.3 Calculation of Magneto-optical Absorption Coefficients 17 22 ABSTRACT TABLE OF CONTENTS LIST OF FIGURES 2.3.1 Magnetoabsorption in the Pidgeon and Brown Model 2.3.2 Decoupled Model: Semiquantitative Treatment of Magnetoabsorption 37 42 68 3. MAGNETOABSORPTION AND FIELD-REVERSAL EFFECT IN n-InSb 3.1 Background 3.2 Experimental Conditions 3.3 Results 3.4 Discussion 4. SPIN-FLIP RAMAN LASER 4.1 Introduction Theory of Inter-Landau Light Scattering 4.2.1 Scattering Cross Section 4.2.2 Scattering in the Decoupled Representation 4.2.3 Scattering in the Pidgeon and Brown Model 4.3 Experimental Background 4.4 Experimental Conditions 4.5 Results and Discussion 4.2 89 90 92 98 112 133 137 139 140 150 166 168 170 5. CONCLUSION 181 6. REFERENCES 187 APPENDICES A. Extended Pidgeon and Brown Hamiltonian B. Irreducible Spherical Tensors C. Rotation of the PB Hamiltonian D. Kane and Yafet Models E. Magneto-optical Matrix Elements for Scattering and Absorption F. Matrix Elements of exp(iq.r) for MD and EQ Transitions G. Decoupling of the PB Hamiltonian H. Effective Scattering Operator to Order k2 ACKNOWLEDGEMENTS 195 221 229 263 275 279 281 293 317 LIST OF FIGURES 2.1 2.2 Energy bands and Landau levels for InSb. Inversion-asymmetry function F (a,3,y): (a) Magnitude versus a and 1, and 2.3 2.4 (b) 18F0 versus angle in planes of high symmetry. Inversion-asymmetry function F (a,3,y): (a) Magnitude versus a and 0, and (b) j 16F1 versus angle in planes of high symmetry. Inversion-asymmetry function F2(a,13,y): (a) Magnitude versus a and 0, and (b) 18F 2 2.5 versus angle in planes of high symmetry. Inversion-asymmetry function F (a,3,y): (a) Magnitude versus a and 1, and (b) 14F 3 1 versus angle in planes of high symmetry. Warping function W0 (a,1,y): (a) Magnitude versus a and 13, and (b) 13, and (b) of high symmetry. (a) Magnitude versus a and 13, and (b) of high symmetry. (a) Magnitude versus a and 13, and (b) 18W 3 versus angle in planes of high symmetry. 2.10 Warping function W4 (a,3,y): (a) Magnitude versus a and 13, and (b) 2.6 SWoI versus angle in planes of high symmetry. 2.7 2.8 2.9 Warping function W (a,c,y): (a) Magnitude versus a and 18W I versus angle in planes Warping function W2 (a,1,y): 18W 2 I versus angle in planes Warping function W3(a,x,y): 18W 4 1 versus angle in planes of high symmetry. 2.11 oc(a ) ED cyclotron resonance, peak absorption versus magnetic field for n-InSb. y(HWHM)=15 cm -1, and B 11[111], [110] and [001]. 2.12 oc+() ED combined resonance, peak absorption versus magnetic field for n-InSb. y(HWHM)=15 cm -1, and B 11[111], [110] and [001]. 2.13 as(r) MD (with some EQ) spin resonance, peak absorption versus magnetic field for n-InSb, with B II [111], [110] and [001]. 2.14 2oc(oL) EQ resonance, peak absorption versus magnetic field for n-InSb, with y(HWHM)=15 cm - 1. Theoretical curves are given for the decoupled approximation and the spherical PB approximation. 2.15 2 oc+co (t) EQ/MD resonance, peak absorption versus magnetic field cs1 for n-InSb, with y(HWHM)=15 cm - 1. The dashed curve is from the decoupled model, neglecting g" and y0 . 2.16 2oc(it) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 =65 a.u.; peak absorption versus magnetic field for n-InSb. Absorption is for B II [001] and is approximately proportional to I F 2. 2.17 2Oc(a_) ED absorption due to inversion asymmetry parameters C' and G, matched to 68 =65 a.u.; peak absorption versus magnetic field for n-InSb. Absorption proportional to jF3 is for B ll [111] 56 and is approximately 57 2. 2.18 2oc(a+) ED absorption due to inversion asymmetry parameters C' and G, matched to 68=65 a.u.; peak absorption versus magnetic field for n-InSb. Absorption is for B II [110] and is approximately proportional to IF1 2. 58 2.19 2oc+o)s() ED absorption due to inversion asymmetry parameters C' and G, matched to 8 =65 a.u.; peak absorption versus magnetic field for n-InSb. Absorption is for B0ll [110] and is approximately proportional to IF 1 2 2.20 2oc+o (a ) ED absorption due to inversion asymmetry parameters C' and G, matched to 65=65 a.u.; peak absorption versus magnetic field for n-InSb. Absorption is for B 11[001] and is approximately proportional to F2 2. 2.21 59 60 2coc+Cos(a+) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 0=65 a.u.; peak absorption versus magnetic field for n-InSb. Absorption is for Boll [111] and is approximately proportional to IF0 2. 2.22 os() ED absorption due to inversion asymmetry parameters C' and G, matched to 8 =65 a.u.; peak absorption versus magnetic field for n-InSb. Absorption is for B II [110] and is approximately proportional to IF12. 2.23 s( _) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 0=65 a.u.; peak absorption versus magnetic field for n-InSb. Absorption is for B ll [111] and is approximately proportional to IF0 2 61 62 63 2.24 s(a+) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 0=65 a.u.; peak absorption versus magnetic field for n-InSb. Absorption is for B II [001] and is approximately proportional to IF* 2. 64 2.25 30c(r) ED absorption due to warping parameter I = 0.55; peak absorption versus magnetic field for n-InSb. Absorption is for B 11[111] and is approximately proportional to W 2. 65 2.26 3cc(_) ED absorption due to warping parameter I = 0.55; peak absorption versus magnetic field for n-InSb. Absorption is for B 11[001] and is approximately proportional to W 12. 2.27 3cc(a+) ED absorption due to warping parameter i = 0.55; peak absorption versus magnetic field for n-InSb. Absorption is for B II [110] and is approximately proportional to W2 2. 66 3.1 Experimental setup for inter-Landau level absorption spectroscopy. 93 3.2 Light 3.3 3.4 10.6 pm for n-InSb. B II [111], q II [T10] and T = 25 K. Fan diagram of intra-conduction-band transition energies for n-InSb. Light transmission (detector output) versus magnetic field at 10.6 pm for n-InSb. B II [110], q II [T10] and T = 77 K. 3.5 3.6 3.7 3.8 3.9 transmission (detector output) versus magnetic field at Magnetoabsorption versus B at 10.6 pm for n-InSb with B01 [111], q II [110] and T = 25 K. (a) it polarization; (b) a 1 polarization. Magnetoabsorption versus B at 10.6 gm for n-InSb with B II [110], q II [T10] and T - 77 K. (a) 7t polarization; (b) L polarization. Magnetoabsorption versus B at 10.6 p.m for n-InSb with B 011[T10], q II [111] and T = 25 K. (a) it polarization; (b) a 1 polarization. Magnetoabsorption versus B at 10.6 jim for n-InSb with B II [001], q II [T10] and T = 25 K. (a) 7t polarization; (b) _L polarization. A Real and imaginary parts of F 3 + F versus 0 about nlII [T10]. A A 'A Zero angle corresponds to = z, II [110]. Dashed line is and imaginary Zero angle corresponds to is F + 0.85F . 1 104 105 108 109 111 parts of F + F A3 3 99 100 124 imaginary part of F3 + 0.85F 1. 3.10 Real 67 versus 0, for il11[111]. A Dashed line II [110] , II [I12]. 1 125 A 3.11 Real and imaginary parts of F versus 0 about rl II [T10]. A A A angle corresponds to = z, II [110]. A 3.12 Real and imaginary parts of F versus 0 about l 11[111]. A A angle corresponds to II [110] , II [112]. 1 Zero 126 Zero 127 A 3.13 Absorption versus 0 about T1 II [T10] for 20c( 1,_) transition. Zero C A A A angle corresponds to = z, II [110]. A 3.14 Absorption versus 0 about ri II [111] for 2 0c(o L) transition. Zero C A A angle corresponds to II [110] , II [112]. A 3.15 Absorption versus E about 1 II [T10] for 2o +so (rt) tramsition. A A C A 4.2 4.3 4.4 129 S Zero angle correspond s to 5 = z, 11[110]. A 3.16 Absorption versus ( about ] II [111] for 2c+s(x) A , A Zero angle correspond s to II [110] , ( 11[112]. 4.1 128 130 tra nsition. 131 Raman weight factor versus B for o , 2o c , and 2 c+ s transitions at kz=0 in n-InSb, for incident photon energy E 1 =117 meV. 159 Raman weight factor versus B for c , 2 c , and 2c +o s transitions at kz=0 in n-InSb, for incident photon energy E 1 =232 meV. 160 20 Raman weight factor versus k for o and transitions z C C B =35 kG in n-InSb, for incident photon energy E 1 =117 meV. Relative Stokes output power versus applied magnetic at 161 field for InSb spin-flip Raman laser. Threshold pump intensity versus applied magnetic field for InSb spin-flip Raman laser. Low magnetic-field cutoff for stimulated SFR scattering versus pump photon energy for n-InSb. Also shown is the field-dependent energy gap calculated from the PB model. Relative Stokes output power versus applied magnetic field in InSb spin-flip Raman laser. 170 Magnetoabsorption coefficient [uc(B o) - o(0)] versus B for n-InSb. 176 4.9 Stokes frequency shift versus applied magnetic field B II [110]. 4.10 Relative Stokes output power versus B 0 11[110] for 4.867 gm pumping. 178 4.5 4.6 4.7 4.8 172 173 175 179 LIST OF TABLES 2.1 2.2 Effective velocity operators for axial model ED transitions. Transitions due to H(a ). 74 76 2.3 Transitions due to H(yo). Magnitudes of warping functions W (a,p,y) along directions of high 77 symmetry. 77 2.4 2.5 Operators transitions. causing first-order inversion-asymmetry-induced 79 of inversion-asymmetry functions along F (a,,) 2.6 Magnitudes 2.7 directions of high symmetry. Effective velocity operators for axial model MD/EQ transitions. Matrix elements and peak absorptions for Voigt transitions. 2.8 3.1 4.1 ED Matrix elements of the velocity operator transitions in the decoupled model. for MD/EQ Electronic transitions in Landau level Raman scattering 80 86 87 and ED 118 146 1. INTRODUCTION magneto-optical This thesis explores single-crystal This material n-type InSb. is which semiconductor the among electrons of conduction effects in is a narrow-gap III-V compound most extensively studied narrow-gap It is the classic example of a narrow gap semiconductor with semiconductors. direct energy gap at k = 0. The energy gap is between an s-like conduction This greatly simplifies band (cb) and a spin-split p-like valence band (vb). of effective the application mass theory to the dynamics of electrons and The narrowness of the gap causes a holes, and to magneto-optical processes. small effective mass and large g-factor, resulting in large cyclotron and spin resonance frequencies in comparison with wider-gap materials. has been extremely Magneto-optics determining characteristic allow studies absorption Interband semiconductors. of parameters for useful determination of the energy gap, and intraband absorption measurements allow determination of magnetic field B levels associated field. the effective masses and g-factors. Application of a causes the conduction and valence bands to split into Landau with quantized orbital and spin motion in the magnetic The density of states diverges at the energy minima associated with these levels. intraband This absorption. causes easily observable peaks in both interband and Pioneering work on semiconductor magneto-optics was done by groups led by B. Lax at MIT's Lincoln Lab and C. Kittel at U.C. Berkeley. Many useful reviews of magneto-optics have been given. [Lax 60, 67, McCombe 75, Zawadzki 79, Pidgeon 80, Weiler 81, Seiler 92]. Kim 89a, Rashba 91 and Work on free-carrier magneto-Raman scattering by Wolff, Yafet, Wright et al., and Makarov identified three [Wolff 66, inter-Landau-level occur in n-type InSb at k B. Yafet 66, Kelley 66, Wright 68, Raman = 0, where k scattering processes Makarov 68] which could is the momentum of the electron along These were the double cyclotron, spin-flip double cyclotron and spin-flip processes at frequencies 2o c , 20c+ co, and An = 2 processes, without and with spin flip. orbital quantum frequencies. number, and cc and os The first two of these are s . The symbol n is the Landau or are the cyclotron and spin-flip The last scattering process is pure spin flip, with An = 0, and shows a much narrower line width than the first two which are broadened because the spin precession is less affected by collisions. The spin-flip Raman (SFR) process was predicted to have the largest cross section, and SFR scattering was soon experiments. The observed in stimulated both spontaneous process was and recognized stimulated for applications in the form of a magnetically tunable IR laser. scattering having device The device is known as the SFR laser. A large portion of the experimental and theoretical work in this thesis is devoted to obtaining a more precise magneto-optics. description of free-carrier intraband The theoretical work attempts to unify and give some new perspective to previous work. [Rashba 61a, 61b, Pidgeon 68, 69, Ohmura 68, Weiler 76, 78, Zawadzki 76, Trebin 79, Gopalan 85, Wlasak 86, La Rocca 88a,b]. The experimental work resolves a significant problem concerning the 20 2oc+Oc absorptions. The formalism of Lipari c and and Baldereschi [Baldereschi 73, 74] has been applied to characterization of the angular dependence of the magnetoabsorption which was first determined for general Bo by Rashba, Sheka, and Zaslavskaya [Rashba 61a, Sheka 69]. The Pidgeon and Brown (PB) model has been used to find the magnetic field dependence of the inversion asymmetry and warping induced absorptions as well as isotropic absorptions which are caused by wavevector-dependent mechanisms. magnetic dipole (MD) and electric quadrupole (EQ) The decoupled theory for the conduction band has been used to obtain the limiting behavior of the absorptions at low fields, and a better understanding of the physical nature of the absorptions. Chapter 2, inter-Landau-level which follows magneto-optical perspective of the PB model perspective. It is introduction, transitions presents from the the theory coupled and also from the decoupled of band conduction band The latter is the more useful one for understanding the physics. analogous to the wavefunction is treated operator. this Pauli model for Dirac electrons in which the as a two-component spinor and R is a 2x2 matrix Here we show that the EQ matrix elements for the 2ec(a) absorption and the EQ/MD matrix element for the 2c+ os(rt) absorption are of sufficient magnitude to interfere with the ED contribution due to inversion asymmetry and produce and observable effect upon reversal of B or q. These effects are analogous to the one observed in the spin resonance by Dobrowolska et al. (1983). This theoretical analysis suggests that the B-reversal and q-reversal effects should be observable in the 2oc(ol) and as in the Os(Ir) absorption. 2 oc+os(7) absorptions, as well This is shown to be related to the way in which the 20 c , 2oc+o s and Os scattering processes occur together at kB = 0. Chapter 3 gives a description of the experiment which was conducted recently at the MIT Francis Bitter Magnet Laboratory to observe the B-reversal effect in the 20 c and 2 0c+s absorptions. compared with the theory given in Chapter 2. The results are described and Chapter 4 presents the results of the motivated the investigation of the magnetic Chapters cross SFR laser experiment which field reversal effect described in 2 and 3, and includes some new theoretical calculations of Raman sections in both the PB and decoupled models. It demonstrates the importance of intraband absorption in the output of the SFR laser and shows the dependence of this effect on the crystal orientation. My work on SFR scattering was carried out at the Francis Bitter National Magnet Laboratory. Previous work was conducted by Aggarwal, Weiler and Lax [Aggarwal 71a&b, Weiler 74]. The 10.6 gm pumped SFR laser had been studied at fields up to 10.4 T using a high-power pulsed TEA CO 2 laser as a pump. The Magnet Lab had the capability of 18 T in a 2-inch bore Bitter solenoid, and there was great interest in studying the SFR output at fields above 10 T. The main interest was in determining whether electron-LO phonon coupling would: (i) increase the threshold for stimulated increase the Stokes SFR scattered scattering output by at increasing saturation the by linewidth; (ii) increasing the relaxation of the upper level; or (iii) change the spin resonance frequency by polaron coupling at fields near LO-phonon energies are equal. 12.5 T where the spin splitting and the Other phenomena of interest were one- and two-photon absorption processes which were known or expected to affect the output, and the effect of large B at near-bandgap energies. crystal orientation became on the resonant enhancement SFR scattering The linear magnetoabsorption and its dependence on the main interest in my work when the electron-spin-LO-phonon coupling was not observed [Favrot 75, 76a]. The last chapter presents the conclusions and recommendations for future work. 2. THEORY OF INTER-LANDAU LEVEL TRANSITIONS 2.1 Overview The starting absorption in point InSb [Pidgeon 66,69]. is which the I use 8x8 for the theory Pidgeon and Brown of magneto-optical (PB) Hamiltonian This Hamiltonian is a generalization of Kane's Hamiltonian [Kane 57,66] to the case of finite magnetic fields, and contains terms up to order k2 in the k-p effective mass theory. energy bands, wavefunctions, It permits the calculation of and optical transition matrix elements involving the lowest conduction band and three highest valence bands. used to calculate interband absorption. [Weiler 78] to explain It was originally This model was extended by Weiler experimental results for intraband magneto-optical absorption [Weiler 74, Favrot 76] arising from inversion-asymmetry and warping effects. The present theory uses this model to calculate the absolute Also, in order to obtain simple results in the limit of small absorption. applied magnetic fields and small electron momenta, the reduction of the PB model to decoupled models for the conduction and valence bands is considered, following Rashba and Sheka [Rashba 61b], and Braun and Rtissler [Braun 85]. The PB model is significantly more accurate than the decoupled model for large magnetic fields B0 and wavevectors k . However, the decoupled model is simpler, and easier to interpret physically. Figure 2.1 shows calculated energy bands and Landau levels for the conduction band (cb) and valence bands (hh, lh and sb) which are obtained by diagonalization of the 8x8 Kane and PB Hamiltonians. to denote the heavy hole, light hole and spin Here I use hh, lh and sb split-off bands, respectively. Kane model PB model 0.5 a, z wU -0.5 -0.2 -0.2 -0.1 k/k[X] Fig. 2.1 Kane model energy Figure 1 of [Weiler 78]. bands and PB levels, after The Kane model calculation is for an average direction of k (or neglects warping). 10 T. model Landau The PB model is for B 11 [111] at The PB level separations from the band edges have been scaled up by a factor of 5, for better visibility. Band parameters of [Goodwin 83]. The Kane model bands are shown for wave vectors out to 20% of the distance to The PB the X point of the Brillouin Zone, in a spatially averageddirection. model Landau k = 0 at levels are for a field of 10 T the in [111] crystallographic direction, with the level spacings exaggerated by a factor of 5 for better visibility. The present chapter deals only with intra-cb Landau For the conduction band the a-set and b-set levels may be level transitions. regarded simply as spin up and spin down, and the optical transitions between Landau transitions which valence the at the aC(O) level thesis originate The demonstrate band levels are The two new and spin-flip. levels may be both spin conserving described effect field-reversal in this and end at the aC(2) and bc(2) levels. important the for calculation of scattering amplitudes, and will be described in Chapter 4. A general formulation of the PB model based on irreducible spherical tensors has Lipari 70, been developed who Baldereschi 73,74] Hamiltonian [Luttinger 56]. the large spherical coordinate frame so the applied lines Lipari of this technique Baldereschi, and to the Luttinger This provides the best way to take advantage of component that along the of Hef and to express Heff in quantization direction coincides with the direction of the magnetic field B r . a rotated of the basis states The usefulness of this for the B = 0 case has been discussed by Johnson [Johnson 84]. For finite B0 this makes it easy to obtain eigenstates for the spherical (or axial) part of the Hamiltonian. explanation of the The spherical terms in tensor the anisotropic coordinate frame. [Rashba 61a, La Rocca 88a]. formulation part provides of Hef in an a simple arbitrary The quantization [Luttinger 55] direction of the Luttinger-Kohn can be chosen arbitrarily only in cases where transform like irreducible representations crystal point group. functions these functions (irreps) of the full R(3), or like irreps of R(3) multiplied by some and (LK) basis rotation group 1-dimensional irrep of the This occurs in the cases of the cubic point groups Td, 0 Oh , which possess a particularly high level of symmetry. When this condition applies, Hff usually contains a large spherical component so that the anisotropy may be regarded as a In perturbation. the case of the conduction band in InSb the anisotropy occurs in fourth order in momentum in the decoupled Hamiltonian, so perturbation theory works particularly well. In this development elementary particle-like the perspective of the theory PB lattice disappears is useful to notice and holes near k = 0. nature of electrons discrete it and is replaced by the In this an effective Hamiltonian, the EMA Hamiltonian, which reflects the point-group symmetry but not the discrete translational formulation symmetry of the lattice. was devised by of Hff which I use the invariant [Luttinger 56] for the case of germanium, expanded by [Bir 74], applied to the PB model by [Trebin 79], and further developed by [R6ssler 84] and [Braun 85]. electric dipole optical [Dresselhaus 65], perturbations, [Suzuki 74], I follow [Zawadzki 76], In treating the effect of [Rashba 61a], [Grisar 78], and [Stickler 62], [Trebin 79] in replacing k in Hef(k) by k + (e/c)A l and expanding to first order in the potential A1 , as is done in the Dirac and Pauli perturbing electromagnetic theories. This is equivalent to setting the perturbing Hamiltonian equal to (e/c)A . V H S , or to (e/c)A ,v , with k eff v =V H k eff (i/h) r] = (ih)[H , r] .(2.1.1) eff The importance of this formulation for the PB model, as well as the fact that interband and intraband transition matrix elements are identical in form when obtained this way in the PB model, was first pointed out by [Zawadzki 76]. A of calculation the the in magnetoabsorption anisotropy-induced conduction band includes a generalization of the calculations of [Rashba 61] transitions [Sheka 69]. and [Gopalan 85] to the case of the warping-induced The high-field treatment using the 8x8 PB model for both the warping- and the transitions inversion-asymmetry-induced improvement a represents and simplification of the theory derived by [Weiler 78 & 82], [Zawadzki 76] and The selection rules which arise when B 11[001], [111] and [110] [Wlasak 86]. are explained by the symmetry arguments used by [Suzuki 74] and [Trebin 79] for the valence band magneto-optical contained are rules selection clearly quite These transitions in Ge and InSb. in of mathematics the the irreducible spherical tensor formulation of Hef . In this treatment of the 8x8 PB model Hamiltonian I extend the invariant symmetry, which were to all obtained by [Weiler 78]. formalism tensor spherical irreducible applied to all twenty of the terms in Hef t of [Trebin 79] formulation of these terms, allowed by (See Appendix C.) The has been (Oh) and wavefunctions it is of Lipari and Baldereschi including the warping inversion-asymmetry (Td) terms. In order to calculate necessary to diagonalize numerical energy the axial levels and part of the PB described in Chapter 4 and Appendix A. Hamiltonian, which is 2.2 Formulation of the Effective Mass Theory for Magnetoabsorption In this section the PB Hamiltonian is formulated using the irreducible tensor methods of Lipari and Baldereschi. [Lipari 70, Baldereschi 73&74] addition to obtaining an accurate calculation of the In absorption, the results give a clear understanding of the selection rules and orientation dependence of the intraconduction band magneto-optical transitions in InSb. The crystal orientation dependence is contained in nine angular functions that are shown in polar plots. coefficients The present formulation will be used to obtain absorption which will later be compared with previous [Favrot 76] and current experimental results on InSb. Inversion-asymmetryzincblende-type and semiconductors warping-induced have been magneto-optical the subject transitions of experimental theoretical studies over the past 40 years. [Seiler 92, Rashba 91] relative La Rocca 88a&b] to the crystallographic x, y and z directions. and A general treatment of the problem requires use of a coordinate frame 4r1 rotated in which is [Rashba 61, The zeta direction is chosen to coincide with the direction of the applied magnetic field B . The LK basis states [Trebin 79] may be quantized along zeta because each degenerate set of LK basis states transforms with respect to the point group Td like basis states of the full rotation group R(3), and not just the group Td. [Trebin 79] operators of the PB model to form sets which spherical tensors with to reflections. vector respect The kinetic momentum operator k potential, irreducible [Lipari 70] can be used in polynomials This causes the matrix transform arbitrary R(3) like irreducible rotations and p + (e/c)A, where A is the of different spherical tensor operators of arbitrary rank. orders to form The PB Hamiltonian Heft contains products of involving parts matrix operators and operators formed from the components of k and B [Trebin 79]. The effective Hamiltonian may be divided into parts which have spherical octahedral R(3), Oh and antisymmetric The latter terms are antisymmetric terms contain irreducible combinations tensors of of with respect to inversion. irreducible zero, rank tetrahedral Td symmetry like tensor k 2, B-J [Trebin 79]. The spherical operators or K(2)J which (2 ) form [Lipari 70, The octahedral (warping) terms in the PB model may be Baldereschi 73,74]. made irreducible of rank 4, as shown for the valence band block of Hef by The antisymmetric (inversion-asymmetry) terms in the Lipari and Baldereschi. PB model are irreducible of rank 3. When the direction of B 0 the terms in Heff which were is chosen, spherical become axial, with symmetry group C h. A This part of Hef commutes A with the operator N1F + F , where N is the Landau level number operator for a spinless electron, 1F is the unit 8x8 matrix, and F whose elements are the m is the diagonal matrix values of the LK basis states. [Trebin 79] The eigenfunctions of the axial part of Hef have a simple form and conserve the A total angular momentum along Conservation Yafet, of this A (spin plus orbital) associated with N1F + F . in the axial quantity approximation was discussed by [Yafet 73] by Trebin et al. [Trebin 79] and recently by Rashba and Sheka. [Rashba 91] [Luttinger 56, (The valence band case had been considered by Luttinger Suzuki 74].) eigenvalue of (N - 21F I use X (and sometimes 1) to denote the + F , so that X = 0 for the lowest energy level in the cb, and I call this the 'axial quantum number'. x4 + cubic harmonic like the irreducible terms in H ef transform The fourth-rank octahedral - (3/5)r4 , and have the irreducible tensor form 4+ [Baldereschi 73] T(4) C 2 T+4)] 4)+T(4) 4 5 -4 (2.2.1) 0 The third-rank antisymmetric terms transform like the function xyz and have the form T23)- TA( 3) 7--23) (2.2.2) tetrahedral antisymmetric The considered by irreducible of components. Baldereschi and Lipari i = 3, rank invariants can and be in were not Baldereschi 73] are which Hef, [Lipari 70, expressed in irreducible tensor Using Weiler's designation of the band parameters [Weiler 78], and with t = v3 T of Trebin et al. [Trebin 79] some of these are + c.p.] H(G) = - iG[tx {k,kz = -Y H(N) = 2 --6 G[t(')® K (2)]A(3) (2.2.3) N [(k - k)o t + c.p.] 2 X y N [K(2) t 2 H(C) = (C/~[k({Jx, X Jy2 = - (2C/V3)[K'(® j(3) zz )(2)](3) A (2.2.4) z + c.p.] (3) A (2.2.5) H(G'), H(C') and H(N3) are similar to H(G). Rotation of the antisymmetric terms may be carried out with the Cartesian form of the invariants by the Euler angle transformation method of Rashba, La Rocca's [Rashba 61] Gopalan, [Gopalan 85], and La Rocca [La Rocca 88a&b]. description is the easiest to follow, but neglects to make the connection of the antisymmetric coefficients with (Ic;gv) symmetric (KXlR) coefficients introduced by Rashba and Sheka, [Rashba 61] but expressible in a simpler form. These coefficients are expressed in terms angles, [La Rocca 88a] F through F3. of four functions of the Euler Polar plots of the magnitudes of these functions are given in Figs. 2.2 - 2.5 at the end of this section. Rotation of the octahedral invariants is accomplished in a similar fashion, as was done by Sheka and Zaslavskaya [Sheka 69] and recently by Obuchowicz and Wlasak. [Obuchowicz 91] The symmetrical coefficients (kgXv) which are obtained for this case may be expressed in terms of five functions of the Euler angles which are denoted W0 through W4 . Polar plots of the magnitudes of these The functions are given in Figs. 2.6 - 2.10 at the end of this section. rotation of Hef may be simply expressed when the irreducible spherical tensor form is used. The spherically symmetric terms have the same form in all rotated frames. For the Oh case note that the f = 4 warping terms represented (4 ) contain only the m = 0 and ±4 spherical tensor components in the xyz by TC frame. The t = 3 antisymmetric Td terms represented by T(3) contain only the m = ±2 components. If Heff is expressed in a rotated coordinate frame, all 9 of the t = 4 components will occur, in general, components will occur. The complete Hamiltonian is given in Appendix C. rotation and all 7 of the of all terms The general expressions are in e= 3 the PB T(C4) m TA( 3) = D( 4C)((4,y) T 4)', m m (2.2.6) D(m 3A)(X, 3,y Tm( 3) m (2.2.7) where D(4c) y) m 2 [D 4,m ,)* ( 4 ) (a, + D(4) ( -4,m ,y)+ V D( 4 )(a,,)*] 5 O,m (2.2.8) , and D ( 3 A)(ca, p' ,) m and Tm( 4) frame, - 1[D(3 ) (,,y)* 2 2,m + D(3 ) (a,,y)*] , and Tm( 3 ) ' represent the spherical tensor components in the rotated i.e. with components. k+ defined Here 4TI as k + ik1 , and similarly the R(3). representation for other vector are the coordinates in the rotated frame, specified with respect to the xyz frame by the Euler angles acpy. are (2.2.9) -2,m matrices [Tinkham 64] for The matrices D(,)(a,P,y) m'm the eth representation of The operator T(e) raises the axial quantum number ? by m when B is m A along . The functions Dm( 3A)(a,p,y) are proportional to the angular functions F(xP,y) defined by La Rocca et al., and originally derived by Rashba and Sheka [Rashba 61] for y = 0. The functions D(m4C)(3,P,y) are the analogous angular functions for the warping terms in Hef , and are proportional to the , for m # 0, and to (W - 3/5) for m = 0. functions W The y-dependence in both cases is simply exp(imy). The zeros of the angular functions which occur for specific specified by and z4 - (3/5)r4 y4+ 4+ ox J3, with rotations about the [001] are easily understood. Oh symmetry is The symmetric A directions, cubic with respect directions, C3 rotations about the [111] and C2 rotations about the [110] directions. to C4 directions, Coordinate rotations by an angle y about zeta cause the mt h component of the cubic harmonic in the r1j be multiplied by exp(imy). harmonic frame to For this term to be invariant with respect to C4 rotations, m can only be 0 or ±4. Thus all of the angular functions Wm A associated with warping with m # 0 or ±4 must vanish when is along [001] or Similarly, the functions must vanish when m # 0 or +3 a similar direction. when zeta is along a [111] direction, and they must vanish when m # 0, +2 or A ±4 when is along a [110] direction. Similarly, the cubic harmonic xyz is antisymmetric with respect to C4 rotations about [001], symmetric with respect to C3 rotations about [111], and antisymmetric about [110]. when A with respect to C2 rotations This implies that the angular functions Fm must vanish if m # ±2 A is along a [100] direction, if m # 0 or ±3 when fl1 or ±3 when direction, and if m A is along a [111] is along a [110] direction. The vanishing of the angular functions along the high-symmetry directions is exactly what is required to produce the selection rules obtained for magneto-optical transitions by Trebin et al. [Trebin 79] when B is along those directions. (a) (b) 90. 90" 90" 120' 135' 0.8 45' 0.8 ~0.8 .4 0.8 180. 0.1' 180 0.8 0 .... 225' 60' 0.8 ..... 18 210 33 C 315' 240' Fig. 2.2 300' 270' 270' 270' (001) (110) (111) Inversion-asymmetry muthal angle ax and polar angle function B F (a,3,y). on 4.50 grid (stereo pair). angle in planes of high symmetry. F = 0 8 (a) Magnitude i sin(2a)sin 2 3 cosp vs. (b) 18Fo azivs. (a) (b) 90" 90" 90" 60' 120' 135* 0.8 0.8 45' 180' 0.8 0' 180' 33 210' 225' 315' 300 240 (001) Fig. 2.3 270 2-70 270" (111) (110) Inversion-asymmetry muthal angle cc and polar angle function P Fl(a,0,y). (a) Magnitude on 4.50 grid (stereo pair). angle in planes of high symmetry. F - ' e [cos(2a)sin(2) 1 16 + i sin(2ca)sinp(3cos 2P - 1)] vs. (b) 116F1 azivs. (a) (b) 90" 90" 90" 120' 135' 8 45' 8 [11 0.4 8 180' 0.4 O' 60* . 0.8 150 . 0.8 180' 4 0.8 O' 180' 210 225' \..30 . .33 315' 240* Fig. 2.4 300 270' 270* 270' (001) (110) (111) Inversion-asymmetry muthal angle ca and polar angle function 3 F 2(x,,y). (a) Magnitude on 4.50 grid (stereo pair). (b) angle in planes of high symmetry. F = ~ e2i[2cos(2x)cos(23) + i sin(2o)cosp(3cos 2 - 1)] vs. azi- 8Fz vs. (a) (b) 90so 90 90 120' 135 .. 180 60* 0.8 0.8 45' 0.8 0' O'180' 180' 33 210' 225i 315 240' (111) (110) (001) Fig. 2.5 300 270 27 270' Inversion-asymmetry function F (a,3,y). (a) Magnitude muthal angle a and polar angle 0 on 4.50 grid (stereo pair). angle in planes of high symmetry. F 3 =3 e3iY[cos(2)sin(2) 16 + i sin(2a)sinp(1 + cos 2 3)] vs. azi- (b) 14F 3 1 vs. (a) (b) 90' 90' 90' 120' 135* 60 45" 0.8 0.40.4 __.4 0.4 180 0* .. .. I 5....... 315' 225' 8 0.4 " '"" . "'" '"1...3.... 150 11 .... 0.4 210 ... 240' Fig. 2.6 40.8 30' " ...... 330 - 300 270' 270' 270' (001) (110) (111) Warping function W (c,,y). (a) Magnitude vs. azimuthal angle a and polar angle P on 4.50 grid (stereo pair). (b) IW vs. angle in planes of high symmetry. Wo = (COS 4 0 + sin 4 C)sin4p + coS 4 = (cos4a + 3)sin 4 p 4 + cos 4 (a) (b) 90" 90" 90 60' 120' 0.8 08 45' 0.8 135" [111] 0. - 180' 30' 0 4 0.8 O' . - 150* .4 .4 0.8 0.8 0 1801 0' 180 330' 210* 315' 225. 300' 240. Fig. 2.7 270* 270* 270 (001) (110) (111) Warping function W (cc,,y). polar angle [3 (a) Magnitude vs. azimuthal angle cc and on 4.50 grid (stereo pair). (b) 18W 1 vs. angle in planes of high symmetry. W = eY[(cos4a sin2p + 7sin2p - 4)sinp cosp + i sin4a sin 3] (a) (b) Fig. 2.8 270' 270' (001) (11o0) Warping function W2(a,,y). polar angle 3 on 4.50 grid (stereo pa (111) (a) Magnitude vs. azimuthal angle a and (b) 18W) vs. angle in planes of high symmetry. w2 = 16 e,2 iy(cos 4 (cos2 + 1) + 7cos 2 p _- )sin2 + i (2sin4a sin2 cos] (a) (b) 9C 0.8 [111] 0.4 0.8 270' (001) Fig. 2.9 (110) Warping function W (a,3,y). polar angle 3 (111) (a) Magnitude vs. azimuthal angle ca and on 4.50 grid (stereo pair). (b) 18W 3 1 vs. angle in planes high symmetry. 33 32 e3iy [(cos4o(4 - sin2p) - 7sin 2 [)sinp cos3 + i (sin4a sinp(3cos 2 3 + 1))] (a) (b) 90' 0.4 0.8 n* 180' ,w 330* - 225" 315' (3001 270* 270) (110) (001) Fig. 2.10 Warping function W4(c,3,y). polar angle 13on 270 (111) (a) Magnitude vs. azimuthal angle cc and 4.50 grid (stereo pair). (b) 18W 4 I vs. angle in planes of high symmetry. w44 = j e4iy (cos4a(sin4 64 + 8cos 2 ) + 7sin 4j3) + i (4sin4a cos3(cos 2 + 1))] 1] 2.3 Calculation of Magneto-optical Absorption Coefficients In this section I compute using the effective transitions the mass absorption theory presented coefficients of 2.2. in section basic formulation follows that of Bassani et al. [Bassani 88] several The The key feature is the importance of some electric quadrupole (EQ) and magnetic dipole (MD) These processes for the conduction processes that were overlooked previously. are band of sufficient asymmetry-induced q-reversal magnitude to with interfere the inversion- electric dipole (ED) absorption and produce B-reversal and effects like the one observed in spin resonance at lower fields. The two new transitions which show the interference effect are the 21c(). transition, which has an EQ component that is larger than the ED one, and the 0o (r) transition which has a mixed EQ-MD component that is smaller than 20+ the ED component. Here, 2o c refers to the second harmonic of CR, and 2c+ os is a combined resonance transition which changes both Landau orbital and spin state. The ol polarization is for the perpendicular Voigt configuration, while it is the parallel Voigt configuration. The relation between the absorption coefficient and the transition matrix element is electrons and obtained light. by considering Following the optical interaction Bassani et al. [Bassani 88] between the I express the interaction Hamiltonian as (2.3.1) H' = (eA /2c)(Ve - int + h.c.) , where A 10 is the 'magnitude' of the vector potential which is real and positive, and velocity. V is an operator (frequently nonhermitian) with dimensions of The vector potential of the radiation field is A (r,t) = '[Al ei(q-r - ot) + c.c.] , (2.3.2) A A with complex amplitude A1 - A We , and complex unit polarization vector e AA 2 Note that e-e* = 1 , and A -A* = A 2 10 10 to the greatest magnitude of Al(r,t). 10 , and that A 10 is not generally equal The complex amplitudes of the electric and magnetic fields are E 10 = iA iA C iA = 10 =i A e, C B 10 A 10 iqxAo =iAqxe . 10 10 (2.3.3) The electronic transition rate R due to the radiation is given by the "Golden Rule" (eA/2c)2 1Vfo R = 2 2 (hc - E ) . (2.3.4) The absorption coefficient, in the extreme quantum limit, is found from oc = n ehR/I , (2.3.5) where ne is the carrier density, and II is the radiation intensity given by 1 - where c2 2 cn A 0 (cgs units), 8where is the refractive index. If we assume a Lorentzian lineshape nI is the refractive index. If we assume a Lorentzian lineshape (2.3.6) 1 y g() + (2.3.7) 2 where y is the half-width at half-maximum and the peak height is given by g(0) = /liy, we find po mlVfol 2 g(0 - ofo), = t() h (2.3.8) n Oc 47tn e2 e is the squared plasma frequency for free electrons. where C 2 pO Then m finally, the peak absorption is given by 1 o a(max)= -p mlVfo hec n Oy The next formalism processes. step in 2 . computing (2.3.9) the absorption needed to calculate the matrix elements is to develop the basic for ED, EQ, and MD For this I start from the most common form of the interaction Hamiltonian (2.3.10) H' = 2 e(A (r,t)-v + v-Al(r,t)) where v = V H k eff V = where . v,eiqr} The operator V is then given by , { , } denotes the anticommutator. (2.3.11) The usual approach expands eiq 'r to first order in q-r and separates the ED, MD, and EQ parts as follows. A A V = e-v + e v,q.r + . . . (2.3.12) (eq) e- v + -(exq)-(vxr - rxv) + (rv2) + -[(vr)2) where (rv)( 2) is the 2nd rank tensor product formed from the vectors r and v according to the prescription (rv)(2) (r1)®(v))(2) [Edmonds 73] and it is A e.q = 0 , which is valid if the magnetic birefringence is small. assumed that The first three terms correspond to the ED, MD, and EQ processes, A respectively. One sees that e -v corresponds to the ED part, since this can be obtained simply produces both by neglecting isotropic the spatial and anisotropic magneto-optical transitions. variation of A (r,t). (with respect to crystal This part orientation) A The term proportional to exq is the MD term, and the one proportional to (eq) (2 ) is the EQ term. For the case of unbound carriers in Landau levels localized only in the x direction, it q-dependent is easier part only to work directly after computing with Eq. the matrix (2.3.11) elements. and find When the q is perpendicular to B the first-order effect of eiq-r is found to be equivalent to that of (qxk) zeq-r (See Appendix F). Two additional forms for the interaction Hamiltonian may occur. The first is H' = eE.R , (2.3.13) where R is an operator with dimensions of length. spin-orbit interaction, where R = K kxa, and K S of h2/m2 2 S An example is the ordinary is a constant with dimensions In this case . A V = ie-R . (2.3.14) EQ and MD effects are obtained by replacing this by the expression V = i -e. R,eiqr . (2.3.15) Finally, the simplest MD interaction has the form H' = g*. BBI.J = -*BI-J . (2.3.16) Using this we obtain V= ig*(qxe)J where J is replaced by = -ig*e -(qxJ), 2 for the spin-!2 case. (2.3.17) 2.3.1 Magnetoabsorption in the Pidgeon and Brown Model The method of calculating demonstrated through examples. magnetoabsorption in the PB model will be I will first consider the inversion-asymmetry induced cyclotron harmonic transition 2 c( c), transition 2oc + cos(r), computing other and then the combined resonance both at k = 0 . Prescriptions will also be given for transitions. The resulting curves of absorption versus magnetic field are presented at the end of the section. For the 20(0 ) transition the initial state is the aC(O) conduction band state, with axial quantum number e= with 2 . components The transition t = n + m has J At = +2, of the inversion-asymmetry -- = 0. 2 and The final state is aC(2) results from the m = 3 Hamiltonian in the rotated coordinate A frame with B function F . along B along the axis. These terms are proportional to the angular Notice that the incident by one unit of h Y photon lowers the angular momentum in the axial approximation, so the inversion-asymmetry part of Hef must supply the plus three units required to bring At to +2. The perturbed component of the velocity v 1- = 2V k+H1 (2.3.18) is an operator with m=2 if Vk+ operates on the m=3 part of the perturbing Hamiltonian H , since Vk+ removes a factor of k+. We will assume for simplicity that the transition results entirely from the part of the inversion-asymmetry Hamiltonian associated with the parameter G. The parameters C, C', N2 and N 3 may be treated similarly. From Appendix C we see that the m = 3 part of H(G) in the 4rTI frame is , -iGf3t+k HI(G) I = ~f 3 +~~ where t+ is the basis (2.3.19) matrix associated with the '+' component interband velocity (or momentum), in the cv block of Hf. of the To convert this into an 8x8 matrix, one must replace it+ by 0 it+ 0 (it ) t 0 0 0 0 0 0 = i -(t 0 t+ 0 0 0 0 0 (2.3.20) where the dagger denotes hermitian conjugate. For v 1- we have v =- 4iGf3 t+k+ . (2.3.21) expressions apply for H(G') in the cs block, with G' --- Identical t+--- t . We will use the single-group approximation which sets G and G' = G. We next evaluate the transition matrix element Vfo = (1//2)[(v)fo + i[v _,S ]fo] , which results from the three processes: (1) a 0 1- ao (e=O) v (2) a (E=O) - a af (e=2) H ar (t=- 1) - a (f=2) (2.3.22) H (e=0) Here, v0 v 1 a (3) a , o- af. (e=3) is the (e=2) velocity operator obtained from the axial (unperturbed) portion of Hef, which contains parts that are both constant and linear in k. Processes (1), (2) and (3) are evaluated as = <aflvl_ao> (v_)f (1) r (3) 0-fr iro r 0 C (H )fr,(vo_)r'o/(Ef- Er) , where the r sum is over the a-set states with the a-set states e= with 3. Note that e =- 1 and the r' sum is over v0 , v1 _ and HI are all spin-conserving operators at k = 0 . For evaluating these three terms a program which specializes in matrix manipulations, such as Matlab, extremely useful. (Clo C2+1 where I use 't' from The MathWorks Inc., Natick, MA, is The unperturbed wave functions of definite t have the form C3 0- 1 C65 , c5,+ to denote 'transpose', 1 C4+ 2 cs C7+l) t (2.3.23) so that the result is a column vector. The labeling of the c i coefficients is that of Pidgeon and Brown, which gives odd numbers to the a-set states, but the ordering is by decreasing m within the conduction bands. (c I C2 ), valence (c 3 c6 c 5 c4 ), and split-off valence (c8 c7 ) The matrix representation of the above state is just the column vector of the coefficients without the spatial functions, i.e. (C C2 C3 C6 C4 C5 c8 (2.3.24) c 7 )t The k+ operators, which are simply related to the Landau level raising and lowering operators, may be converted to matrix operators which depend on the -value of the column vector which they act upon. (The k operator is simply a constant associated with the column vector state, which is taken here to be zero.) The k+ operator is replaced by the matrix k+ = VT V-TT1 A+2 V+3 diag[ VNT Vf+Z e+T VT2 ], (2.3.25) where s=eB /hc=ec-2, where the magnetic length ec is the smallest quantized cyclotron radius, and 'diag' refers to the diagonal matrix with the enclosed values ordered from top left to bottom right. Similarly we have k = V~ diag[ V T VViT iT The ordering of operators is important. on a column vector of specific /Ai T e]-2 . (2.3.26) If the operator k+t+ or k+J+ operates e, one must increase e by 1 in the specification of k+ , since the matrix operators t+ and J+ increase e by one. It is easy .to see that the matrix for the product k+k is proportional to the number operator k k_ = 2s diag[ e+l e-l e1 e+2 e e+1]. (2.3.27) Similarly, we have k = 2s diag[ v(e+1)(e+2) /e(7+1) ... ¢(e+2)(e+3) i , (2.3.28) and k = 2s diag[ e(T-TT) (e+-l V(-1)(-2) ... . . ] , (2.3.29) The evaluation of terms (2) and (3) may be simplified by writing each as a product of matrices. For (2) we have S(v)(H1)ro/(E - E) where af and a - Rt H a at v= R (E-E ) (2.3.30) are real column vectors, and all of the matrices are real, except for the factor if3 in H which is factored out. 3 whose columns , are the eigenvectors of H for f = 3, diagonal matrix whose elements are (E i - E )-1, eigenvectors in R. R is the real matrix 11 and (E-E )-1 is a ordered the same way as the I have used dots to denote matrix multiplication. Care must be taken in defining the matrices vo_ and H to account for the -value of the vector which they act upon. In the present example, H 1 acts on vectors with f = 0, and v0_ acts on vectors with e = 3. Term (3) may be expressed as X (H)fr,(vo )ro/(Ef-Er,) = a HI R' (Ef-E') Rt v where R' is made from the eigenvectors with e =- 1. ao , (2.3.31) The 2oc+ os(nt) inversion asymmetry-induced ED transition has At = 1 with initial state aC(O) and final state bc(2). The At = 1 part of H(G) is H(G) = where k k2 iGf[ -t was dropped. + 2t k+k] - The last term is zero when H operates on states with k = 0 , but is needed to compute v v (2.3.32) , which is found to be = - iGfI(2t k+) . (2.3.33) The transition matrix element is o (2.3.34) 1=(vS)f + i[V0 'SlIf 0 which results from the three processes: V 0 (1) (2) f f=l (6=1) (o ( =0) ao v b . b H r r (t=O) (e=o) (= 1) H (3) The v a a (e=o) ( =1) o matrix bb - r" calculation different intermediate states. b f • (e=1) proceeds as before, with different matrices and Next we consider the ED cyclotron resonance absorption ac(al) in the Voigt geometry, and the EQ CR-harmonic absorption 2mc(al). The EDCR absorption is easily found from (v+)fo = af v0+ a , with a = aC(O) replacing v0+ af = aC(1). and by (2.3.35) The EQ 2oc(a) absorption is found by (-iqk+/2s)vo+, where we have chosen A q = qrl. This requires the evaluation of (vo+k+)f = a with a = aC(O) v+ k+ ao af = aC(2). and (2.3.36) The low-field dependence of the ED and EQ matrix elements is B 0/2 and B10, respectively. The Voigt MD spin resonance transition cos(t) and the mixed MD and EQ cyclotron harmonic combined resonance transition 2oc+ os(t) are both found in the PB model by a simple modification of the calculation of the ED combined resonance transition O+ Oas(7). This last transition requires evaluation of the matrix element (v)fo = b with vo0 ao ao = 0aC(0) and by replacing v0 ; by (2.3.37) , b = bC(1). f {vo, - sqk4) The MD and EQ matrix elements are obtained and keeping only the k_ component of k for the MDSR evaluation, and the k+ component for the 2o0 + o the cs(x) MDSR transition one must then evaluate evaluation. For -(iq/4s) {Iv ,k} , where the symmetrization is required because v0 is linear in k+. contains a small part which The transition matrix element also has a small contribution from the magnetic dipole terms in Hef , which contain the parameters N , K, K' and K". For the 20+ s(t) transition one must evaluate - (iq/4 s) {v ,k }fo B1 and It is significant that the B -dependence of the matrix elements is Bo, 0 0 0 B20 for the os, c + 0s and 20C+ co transitions, transition has a lower-order dependence on B because less cancellation occurs among the respectively. + than the c terms which The os (s ED transition contribute to the matrix element. The result of calculations of the peak absorption for various transitions is given in the figures. In all of the calculations I assumed a free electron concentration of 2 x 1016 cm - 3, and a linewidth of 15 cm - , which is the observed half-width at half-maximum (HWHM) linewidth of the 2wc transitions at 12 T. I also assumed quantum limit conditions and neglected the Reststrahl absorption which occurs near photon energies of 25 meV. The band parameters used were those of Littler et al. [Littler 83]. Figures 2.11 and 2.12 show the ED cyclotron and ED combined resonance absorptions versus B for the o1 -Voigt and r-Voigt geometries. Figs. 2.13-2.15 show the MD and EQ absorptions, which result from the finite of the incident wavevector These light. are harmonic resonance and the cyclotron harmonic 7r-Voigt, a_-Voigt and 7t-Voigt the combined resonance, The respectively. geometries, cyclotron spin-resonance, in the actual spin resonance linewidth is much less than 18 cm - 1, but this value was used so that the integrated strengths absorption for the 2 c+ of the co lines can be The compared. integrated transition starts off lower than that of the spin resonance but becomes greater than the latter at fields above 7.5 T. Figures 2.16-2.18 show the absorption for the cyclotron 20c harmonic resonance for three polarizations, assuming that only the inversion asymmetry mechanism contributes. The curves are matched at low fields to a value 50=65 a.u. for the cb inversion asymmetry parameter. This value corrects the value of 56 a.u., found by [Chen 85b], to account for energy-band nonparabolicity. Figures 2.19-2.21 show the absorption for the 2 c+ co combined resonance for three polarizations, assuming that only the inversion asymmetry mechanism contributes. Figures 2.22-2.24 show the absorption for the os spin resonance for three polarizations, assuming that only the inversion asymmetry mechanism contributes. show the absorption for the 30 c transition for three polarizations, assuming that only the warping due to the parameters t and pt' Figures 2.25-2.27 contributes. The single-group approximation p. = pt' is assumed. 7000 6000 5000 4000 3000 2000 1000 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.11 oc(al) ED cyclotron resonance, peak absorption versus magnetic field for n-InSb, with ne= 2 x1016 cm - 3 and y(HWHM)=15 cm - 1, and B II [111], [110] and [001], from top to bottom. 10- 0L 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.12 wc+os(n) ED combined resonance, peak absorption versus magnetic field for n-InSb, with ne=2x1016 cm - 3 and y(HWHM)=15 cm - 1, and B II [111], [110] and [001], from top to bottom. 0.03 0.025 - 0.02- . 0.015 - 0.01 0.005 - 0 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.13 o)s(7t) MD (with some EQ) spin resonance, peak absorption versus magnetic field for n-InSb, ne =2 x016 cm - 3 , with B 11[111], from top to bottom. [110] and [001], The linewidth was assumed to be 15 cm - 1. The actual linewidth ys is much narrower, so the peak absorption should be multiplied by 15 cm-ly . 0.7 0.6 0.5 0.4 0 0.3 - 0.2 - 0.1 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.14 2%c(_l) EQ double cyclotron resonance, peak absorption versus magnetic field for n-InSb, with n =2x106 cm 3 and y(HWHM)=15 cm'. dashed line at left is the decoupled approximation. right is the spherical PB approximation. The dashed curve on the The solid curves are PB model for B II [001], [110] and [111], ordered top to bottom. [Littler 83] are used. The The band parameters of 0.03 0.025 0.02 0.015 0.01 - 0.005 - 0 0 20 40 60 80 100 120 160 140 180 200 resonance, peak Magnetic Field (kG) Fig. 2.15 absorption 2o c+-ws(r) versus EQ/MD magnetic double field for cyclotron n-InSb, combined with ne= 2 x1016 cm 3 and y(HWHM)=15 cm -1. The solid curves are PB model for B II [111], [110] and [001], ordered top to bottom. The dashed curve at the left is from the decoupled model, neglecting g" and y0 . are used. The band parameters of [Littler 83] 0.9 0.8 0.7 a 0.6 - o 0.5 C 0.4 0.30.2 0.1 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.16 2o)c(7) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 =65 a.u.; peak absorption versus magnetic field, for n-InSb with ne=2x10" cm - 3 , B II [001] and y(HWHM)=15 cm inversion asymmetry resides in the indicated parameter. the decoupled approximation. G, respectively. IF2 12_ 1. Each curve assumes the The dashed line is The upper and lower solid curves are for C' and The angular dependence is approximately proportional to 0.7 0.6 0.5 0.4 a 0.3 0.2 0.1 , 20 0 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.17 2coc(a) ED absorption due to inversion asymmetry parameters C' and G, matched to 50=65 a.u.; peak absorption due to v versus magnetic field, for n-InSb with n = 2 x1016 cm - 3 , B II [111] and y(HWHM)=15 cm -l . e 0 Each curve assumes all of the inversion asymmetry to reside in the indicated parameter. The dashed line is the decoupled approximation. curves are for C' and G, respectively. The upper and lower solid The angular dependence approximately proportional to IF3 12 if one neglects the contribution of v+. is 0.06 0.05 0.04 S0.03 0.02 0.01 0 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.18 2)c(Y) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 =65 a.u.; peak absorption due to v+ versus magnetic field, for n-InSb with ne= 2 x10O 16 cm,-3 B Ii [110] and y(HWHM)=15cm.- E Each curve assumes all of the inversion asymmetry to reside in the indicated parameter. The dashed line is the decoupled approximation. curves are for C' and G, approximately proportional to F respectively. 2 The upper and lower solid The angular dependence if one neglects the contribution of v is 1.2 1- " 0.6- C -" 0.4- _ 0.2 0 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) 2 Fig. 2.19 and G, c+o s(7c) ED absorption due to inversion asymmetry parameters C' matched to 8 =65 a.u.; peak absorption versus magnetic n-InSb with ne= 2Xl016 cm -3 , B 11[110] and y(HWHM)=15 cm . field, for Each curve assumes all of the inversion asymmetry to reside in the indicated parameter. The dashed line is the decoupled approximation. curves are for G and C', approximately proportional to IF respectively. 2 The upper and lower solid The angular dependence is 0.9 0.8 0.7 0.6 0.5 M 0.4 , 0.3 - 0.2 0.1 - 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.20 2mc+ms(al) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 =65 a.u.; peak absorption due to v versus magnetic field, for n-InSb with ne=2x106 cm 3, B II [001] and y(HWHM)=15 cm - 1. Each curve assumes all of the inversion asymmetry to reside in the indicated parameter. The dashed line is the decoupled approximation. curves are for G and C', respectively. The upper and lower solid The angular dependence approximately proportional to IF2 12 if one neglects the contribution of v+. is 0.8 0.7 0.6 E 0.5 - .9 0.4 < 0.30.2- C . - 0.1 00 40 20 80 60 100 120 140 160 180 200 Magnetic Field (kG) 2c+s(al Fig. 2.21 ) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 =65 a.u.; peak absorption due to v+ versus magnetic field, for n-InSb with ne= 2 xlO16 cm - 3, B 11[111] and y(HWHM)=15 cm-1. Each curve assumes all of the inversion asymmetry to reside in the indicated parameter. The dashed line is the decoupled approximation. curves are for G and C', approximately proportional to IF respectively. 2 The upper and lower solid The angular dependence if one neglects the contribution of v_. is 1.4 1.21 0 & 0.8 o0 " 0.6 0.4 0.2 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.22 %s(o) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 =65 a.u.; peak absorption versus magnetic field, for n-InSb with 16 -3 ne= 2 x10 6 cm, B -1 11[110] and y(HWHM)=15 cm . Each curve assumes all of the inversion asymmetry to reside in the indicated parameter. is the decoupled approximation. and C', respectively. IF 12 The dashed line The upper and lower solid curves are for G The angular dependence is approximately proportional to 0.06 0.05 - 0.04 o 0.03 o0 0.02 0.01 0 0 20 40 60 80 100 120 140 160 180 200 .Magnetic Field (kG) os(al_ ) ED absorption due to inversion asymmetry parameters C' and Fig. 2.23 G, matched to 50=65 a.u.; peak absorption due to v_ versus magnetic field, for n-InSb with ne= 2 x1016 cm,- 3 B0 II [111] and y(HWHM)=15 cm - 1. Each curve assumes all of the inversion asymmetry to reside in the indicated parameter. The dashed line is the decoupled approximation. curves are for G and C', approximately proportional to F0 respectively. 2 if The upper and lower solid The angular dependence one neglects the contribution of v+. is 0.2 0.18 0.16 0.14 E a 0.12 o. 0.1 - S0.08 0.06 0.04 0.02 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.24 os(l) ED absorption due to inversion asymmetry parameters C' and G, matched to 8 =65 a.u.; peak absorption due to v+ versus magnetic field, for n-InSb with ne=2xl016 cm - 3 , B II [001] and y(HWHM)=15 cm . Each curve assumes all of the inversion asymmetry to reside in the indicated parameter. The dashed line is the decoupled approximation. The upper and lower solid curves absorption are for C' and G, respectively. The proportional to IF*2 12 if one neglects the contribution of v D is approximately 0.9 0.8 0.7 0.6 0.5 0.4 0.3 0.2 0.1 00 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.25 absorption 3WCc(t) ED absorption due to warping parameter gt = 0.55; peak versus magnetic field, for n-InSb with n =2x106 cm - 3 and y(HWHM)=15 cm - '. B II [111] The dashed curve is the decoupled approximation. angular dependence is approximately proportional to IW3 2 The 0.6 0.5 0.4 . 0.3 0.2 0.1 0 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.26 absorption B0 11[001] 3Oc(ol) ED absorption due to warping parameter g = 0.55; peak due to v and approximation. versus magnetic field, for n-InSb with ne=2 x1016 cm - 3 y(HWHM)=15 cm 1. The dashed curve is the decoupled The angular dependence is approximately proportional to IW if one neglects the contribution of v+. 2 0.1 0.09 0.08 0.07 - 0.06 - .5 0.05 - o - 0.04- 0.03 0.02 0.01 - 0 0 20 40 60 80 100 120 140 160 180 200 Magnetic Field (kG) Fig. 2.27 3 c(() ED absorption due to warping parameter p = 0.55; peak absorption due to v+ versus magnetic field, for n-InSb with ne= 2 X1016 cm -3 B II [110] and approximation. y(HWHM)=15 cm-1. The dashed curve is the decoupled The angular dependence is approximately proportional to if one neglects the contribution of v . W 22 Decoupled Model: Semiquantitative Treatment of Magnetoabsorption 2.3.2 The decoupled model for the conduction band (cb) provides greater insight into of the the physics model. in n-InSb than transitions the PB In this section we consider magnetoabsorption in the decoupled model We consider all terms to order k4 as was done by Ogg in which Hef is 2x2. and magneto-optical McCombe, Barticevic 87]. complete. and more We follow However, recently I the by latter include Barticevic treatment the [Ogg 66, because effective is quite significant it is spin-orbit leads the most interaction, to measurable proportional to E.kxo, which absorption. This term was introduced by Yafet [Yafet 63] and was used by [Sheka 65], [McCombe 69], and [Kim 89a]. and McCombe 69, See also the review by Rashba and The decoupled Sheka [Rashba 91] and a recent application by [Jusserand 94]. Hamiltonian to fourth order is [Barticevic 87] Hff = k/2m eff2 * {k x k + g*gB-a + eKSEkxo + 2(4( z 0 x x y - k2} B o({k 2 z + c.p.) + yoB(axBxkx + yz). It would be useful to redefine parameters so that H(g") = 2g"t(GB)(2) K (2) H(ox) = - k c.p.) B 2 + g'gB.TBk2 + 2g"g (-k)(B-k) 2OB + C0k4 + + + 4) (2.3.38) K(2 1](4) H(y o) = YOR[(aB)2'( In H(c%) k4 k+ k 2 ,k2 } + c.p.= - I used k4 + k4 + k4 x y z Appendix C). (2.3.39) C ) + k4 , and then made irreducible by subtracting the part which has rank zero. (See The general form of the Hamiltonian in a rotated coordinate frame is given in Appendix C. For the purpose of computing magneto-optical transitions we take the unperturbed Hamiltonian to be Ho = k2/2m * + g* B0 . (2.3.40) The remainder of Hef is treated as a perturbation, and is denoted H. We use the Landau gauge A° = B 0 1 , (2.3.41) A so A B = B0 is along the axes oriented relative (See Appendix C.) axis in a general coordinate frame with the 4ri to the xyz axes via the Euler The unperturbed eigenfunctions A functions of N, k7, different gauge k and a . and different angle transformation. are taken to be eigen- Here we follow Barticevic et al., but use a set of eigenfunctions. The explicit eigenfunctions are n,krk,a(r) = e ik l eik n(4 - kllIs) X , where the 0n is a simple harmonic oscillator function, (2.3.42) On(x) = (n!)-1/2(bt)n 40(x) . Here b! = (p /h + isx)/V2s 0 (x) XG is 0 =(s/h) 4 e -(1) (2.3.43) (dimensionless, with s = eB /hc) and 2 (2.3.44) if a is up (a-set) and if cy is down (b-set). is real if n is even, and imaginary if n is odd. The phase of On(x) The operators k+ = k + ik are related to the Landau level raising and lowering operators at and a via k+ = v2sa , k_ = V2-a. (2.3.45) When the fourth and higher-order corrections to H 0 are considered, one finds A that N and (% are no longer conserved separately, but that the combination N + -a is conserved. In particular, the fourth-order term H(g") causes mixing of spin-up and spin-down states at finite k First consider the electric dipole (ED) transitions. If we consider just the unperturbed Hamiltonian, we see that the only ED transition for a free cb electron is cyclotron resonance (CR), which is caused by the operator v+ = k+/m* , at the frequency (2.3.46) o c = eB lm*c = h2slm*. For the aC(O) to aC(1 ) transition, using the notation of [Pidgeon 66] and [Weiler 78], the matrix element is (v )fo = 2s-/m* . (2.3.47) Terms in the perturbing Hamiltonian H 1 produce new ED transitions by lowering the symmetry of H ef relative to that of H . isotropic perturbations. cyclotron resonance, The but no k4 , involving and The terms new transitions. produce two however, 2g"l B(*-k)(B-k), terms First consider the (B.o)k 2 produce eKsE-kxa and first term is new transitions. The analogous to the ordinary spin-orbit Hamiltonian in the Pauli Hamiltonian for a free electron, which is derived from decoupling proportional to g" does the Dirac not Hamiltonian occur in the Pauli [Foldy 50]. The term Hamiltonian. It produces mixing of a-set and b-set (spin-up and spin-down) wave functions when k # 0. The new ED transitions which are produced are the combined resonance coc + os(t) which occurs for A polarization (denoted 7r) in the Voigt geometry, and the ED-induced spin resonance transition ws(a_,k which occurs for a_ polarization in the Faraday geometry, for finite k in the _1 polarization in the Voigt geometry. The combined ) , and resonance transition (sometimes denoted KR) involves a change of both orbital and spin states, in such a way that the sum n + m At = 0 transition, where t = n + m - I remains constant. i.e. This is a is the integer-valued quantum number which is conserved in the axial approximation, and which is zero for the lowest conduction subband aC(0). The matrix element which appears in the expression for the absorption coefficient may be written A V = e-v where Veff is (2.3.48) an effective velocity operator which is the operator in the case where the optical perturbation ordinary velocity is proportional to A v. 1 For the spin-orbit-like term H(K) we may write H(K) = eE-R , s (2.3.49) where R - K S kxo. (See [Rashba 91].) v eff = i3KSkx (2.3.50) We then have . (2.3.51) The ED transitions, and the operators which produce them, are veff = v eff Occ + c s (t): (ED spin resonance) K ka Ks k+ a 2 S+- (Cyclotron resonance) (Combined resonance) . where we have included only the parts of the operators which give energy- absorbing transitions. is g-factor transitions eff v" -2, I free in the Pauli correction, approximation and the the spin-reversing with os(o+,kL) a . electrons the radiative neglecting are = -oKsk For vf - oKf k , and c - os(7r ) with cannot originate from the ground + The latter transition cannot originate from the ground state. For the term H(g") = 2g"g B(a-k)(B-k) it is useful to consider only the part which involves the second rank tensor components Km 2). To obtain this part we use (c-k)(B-k) = (oB) (2 . K(2) + noting that the part -B)k 2 3 !(oxB).(kxk) (2.3.52) is zero since kxk is proportional to iB. The reason for doing this is that the axial approximation requires this part to be combined with the m = 0 part of the cubic term H(yo), as is done in Appendix C. The ED transitions and velocity operators then are (a_,k) • v~ =- (g" I(W + I y(W S=o(g- -))k (ED spin res.) a (Cyclotron res.) -))kaa ) Oc( OS(C) ac + where W as( t) :" V = o o(Wo ))k_ , (Combined res.) is the angular function for m = 0 terms in the warping (octahedral) part of Hef, W = (B o The ox + B4 oy matrix element + B4 )/B4 or for the (2.3.53) o os(c_,k ) transition must be multiplied by a correction factor g1 =1 0 s/(( S This is S + (0c) C required to (2.3.54) account for the A contribution [e-v o, iS]fo which results Sifo from wave function mixing, as shown in Appendix F. Table 2.1 summarizes the results for ED transitions which occur in the axial approximation. Table 2.1 Effective velocity operators for axial model ED Transitions. Transition At s-,k ) (Oc+) Velocity operator -1 v_ = +1 v+ = k+/m* c k = C 2 k(Y[s + os(Y+,k ) The anisotropy +1 v of the + - (co (g Sv o(g- W o - the incident light ) = Order k5 and ok3 (oc + (os((t) transition might account observed anisotropy in the output of the 10.6 [pm-pumped SFR laser. is strongest when B - ))] for the The output is directed along a [111] crystallographic direction with polarized parallel to B. The oc + os(7) absorption contributes to the SFR scattering cross section, as pointed out by Aggarwal [Aggarwal 71] and this is the orientation for which the o c + os(rt) absorption is strongest. Next consider the ED transitions induced terms H(o0 ) and H(y) first because they warping We consider the warping-induced transitions in Hef. contribute by the fourth-order to the axial varying degrees of anisotropy in them. model transitions and produce For a general direction of B the warping terms produce many other transitions which violate the axial model selection rules. Zawadzki 76, in all As Trebin 79], polarizations, considers was all orders considers out previously all inter-Landau general for a of perturbation restricted to zero, or if B or if one pointed [Rashba 61a, level transitions direction of B 0 at theory. Selection Weiler 78, become finite k rules exist possible, , if if k one is is chosen to be along a high symmetry direction, only transitions which occur in first-order perturbation in first-order perturbation theory in the anisotropic terms. In order to compute the strengths transition theory we need the Hamiltonian and velocity matrix elements in the rotated A reference frame 4rli with B along H(y0 ) are given in Appendix C. . The general expressions for H(cx0) and The velocity operators are easily computed from these, and the results are given in Tables 2.2 - 2.4. are indicated which account for wavefunction mixing [Gopalan 85]. transitions on k the contribution to the Correction factors transitions from The magnetic field and k dependence of the may be easily understood. fourth-order terms in Heff is third-order in k. The velocity associated with the Thus An = 1 or 3 transitions may be independent of k , while An = 0 or 2 transitions must contain k once or three times. proportional The first set of transition matrix to B3/2 since each factor of k+ or k An = even matrix elements will be proportional to B k elements be will contributes B 2. The to lowest order in k . Table 2.2 Transition Transition operators and angular dependences due to X(ao). Operator factor At - S1 C (k -5k2 -s)k + 0 vl+ v1 W' -3W 2 2c 2 - ak 2k -6W 30 3 - aok 3 -2W Correction factor: 0 1 1 -6W 12W 24W 4W 8W 1 c v_ 2 0 c The correction factor for the cc transition due to vl+ must be replaced by 1, both here and in Tables 2.3 and 2.5. Table 2.3 Transition operators and angular dependences due to f(y o ). Transition At 0 - 1 S 0 C - S1 v+ v1 vI cy sk 4W 2W - W %sk+ - W 2W 2 4W 3 y sk+ + - W' 2W 4W 2 1 2 S1 C S+ C Operator 210 0S 0 0 y Ysk -+ -W 20 Correction factor: 2 -2 0- -1 0 2 c 0 1 W'0 - W1 1 C+ C Magnitudes of warping functions Wm(aj,y) along m directions of high symmetry. W0 1 1.000 W| 0 W3 0 W4 8I - 0.125 [111] 3 = 0.3333 [110] 1 = 0.5 2 0 12 0 0 -/ 0.1179 0 c(0+ C Table 2.4 [001] 2 3 32 = 0.09375 Finally, consider the inversion-asymmetry Hamiltonian H(50 ), which is third order in k. This is the Hamiltonian which Rashba and Sheka introduced [Rashba 61a] and used to predict ED-induced resonances. In the absence of an applied magnetic third-order splitting of the conduction spin resonance and combined field it produces the band which was first predicted and analyzed by Dresselhaus [Dresselhaus 55]. This is the Hamiltonian which is important in the interference effect in spin resonance in which the absorption changes upon reversal of either B or q, where q is the optical wavevector [Dobrowolska 83, Chen 85]. The absorptions, including absorptions [Rashba 61a], were treated by Gopalan et al. not considered in the spin conserving [Gopalan 85]. The general expression for H(80) in a rotated coordinate frame was given by [La Rocca 88]. operators 2.5 - 2.6. The result is reproduced in Appendix C, and the velocity to the different which contribute The correction which must be factors, in Tables are given transitions applied to the matrix elements of v+ and v_ , give the correction due to mixing of the unperturbed wave functions first-order by the perturbation perturbation. theory have Only been transitions which considered. result from Higher-order transitions are expected to be much weaker, but some transitions are predicted in the PB model which have a higher-order dependence on B than the ones in the tables. These might be observable at large magnetic fields. In the decoupled model, all of the transition matrix elements are of order k 2 , which means order B or Bkk. The low-field absorption then is proportional to B for the transitions occurring at k finite kr. = 0, and to k 2 for those which require Note that now it is the An = odd transitions which depend on k and the An = even transitions which occur at k = 0. The magnetic field dependence of the absorptions, obtained with the PB model, are found in the preceding section. Table 2.5 Operators induced ED transitions. Transition o At causing Operator - 1 80(k2 - 3k) S 0 - first-order v inversion-asymmetry- V1 4F_2 -2 V1 6F -4F - 8F 4F -1 0 c - a 2 8 +k + 12F C 1 8 0ak +k 0 8F1 16F c + 0 0 8 k k 12F 8F - 20F 2F F 2 - 2F 4F k2 - 2F - 5F 20c - Os 3 80 k 2 20 2 8 C 2c+ C S 1 Correction factor: 0 60 + 0 -+ 2 0 0- SC - 6F 3 -6F 2 1o C Table 2.6 Magnitudes of inversion-asymmetry functions Fm((a,P,y) along directions of high symmetry. [001] F0 1 [111] 0 12 = - S0 [110] 0.1443 0 0 1 = 0.0625 0 0 16 1 IF2 0.125 2 IF 3 0 12 83 = 0.2041 3 16 - 0.1875 Now we consider magneto-optical transitions which are induced by the [Bassani 88, La Rocca 88, Kim 89a, finite wavevector q of the incident light. Kim 89b and references consider We therein.] approximations, which are linear in q. and absorption. At high the MD and EQ The allowed transitions are the same ones which occur as 2-photon transitions. scattering only These include the cases of both magnetic fields the transitions are generally mixed MD and EQ in character, except for At = 2 transitions which must be pure EQ. For example, the spin resonance transition is pure MD only in the lowest-order approximation in B 0, reflecting the time-reversal symmetry which exists in the limit B 0 = 0. The allowed approximation are 3m MD and s, 2 + ms at finite k . [Yafet 66, 71], absorption transitions 20 + 0 at k [Wright 68] [Zawadzki 76], These in -0, the spherical and ( - 3 (or + 0, ,OC are and [Makarov 68]. [Trebin 79], all the possible For 2-photon [Weiler 82], [Wlasak 86], energy-absorbing axial-model transitions with At < 2, for positive g-factor materials. All but the transition in are able to axial) (For the analogous Raman scattering transitions see [Kelley 66], see [Seiler 92].) c, EQ occur in the quantum limit, which c- only s the ground-state aC(O) Landau subband is occupied. The MD contribution to the optical absorption results most clearly from terms in Hff which contributions contain B explicitly. Other MD as well are obtained by expanding eiq-r in the optical as EQ perturbation to first order in q before, or sometimes more conveniently after, computing the desired matrix element. An = +1 transitions functions. (i/s)(qxk) The part of q which is perpendicular to B0 causes between the spatial (i.e. spinless) Landau level wave The effect of exp(iql.r) is found to be equivalent to that of (See Appendix F, or take matrix elements , to first order in ql. of the identity [r,H] = ih2k/m.) The effect of exp(iq () is to change k of the state which the exponential operates on, producing a mixture of a-set and b-set states with the same n + ms . choosing k = q/2. the initial state to have k The effect at k =-q/2 and = 0 is obtained by the final state to have (See [Kim 89a], after Eq.(49).) First, we will compute the matrix element for spin resonance which is MD to lowest order. From Section 2.2 we have H'g* B ' (2.3.55) with effective velocity operator i A V =- g*e-qxo . (2.3.56) Keeping only the part which produces a to b transitions we have V = -Ig*(e q - e+q)G_ . (2.3.57) This produces spin resonance for the it-Voigt and o_-Faraday geometries. A that e+ = V2 when A A (Note A e = e_ = (4 - ir)/V2.) The appearance of q+ in the first term implies a phase which varies with the direction of q 1 . The matrix A elements I take q = qrl for the Voigt geometry, are given in Table 2.5. following [Bassani 88] and [La Rocca 88]. The matrix element for spin resonance with 7t polarization, then, is (2.3.58) V = (i/4)qg* , fo for the transition from aC(O) to bc(O). particularly important in the calculation The phase of the matrix element is of the interference the absorption changes upon reversal of B effect in which or q, for certain geometries and crystal orientations. Next we consider the 2(o transition. This transition can only occur in the ol-Voigt geometry since 2 units of angular momentum are transferred when the photon is absorbed. The transition velocity operator, then, is V = !.{k/m*,(i/s)(qxk) A A } . (2.3.59) A Taking e = ( and q = qr this becomes V iq/sm*)k . (2.3.60) Keeping only the part which produces the 2c c transition, we have V = (- iq/4sm*)k+ . For the aC(O) to aC(2), 2 oc(a) V (2.3.61) transition we then have the matrix element = - iq/V2m* . (2.3.62) This result has the same dependence on q, and lack of explicit dependence on B o, as the matrix element for spin resonance. The matrix elements have an implicit linear dependence on B ° since q = nol/c must be evaluated at the transition frequency, which depends linearly on B in both cases. It is interesting to note that the two matrix elements are very different in terms of their physics. The one for spin resonance comes from a permanent magnetic dipole moment which exists when B ° = 0, while the one for 20 c comes from an induced electric quadrupole moment proportional to e2 which exists only in the transition state, and which diverges like 1/B 0 as00B - 0. The matrix element V for the 20o transition is a factor qt smaller B c fo than the one for cyclotron resonance with the same initial state. This relationship was noted by Johnson and Dickey [Johnson 70] who considered the possibility that a wavevector-dependent process could cause the 2o c absorption The value of (qe ) 2 which which they observed in n-InSb at 1.2 T and 2.0 T. they calculated is small by a factor of about 2500, which is (2nn 1)2 times a The corrected value of (qB)2 is 10-4 at 2 T round-off factor of about four. instead of 4 x 10- 8 , but this is still too small to account for the strength of the 2o The c transition which they observed. wavevector-induced matrix element for the 20o c + o s transition involves higher-order band parameters than the previous two matrix elements which resulted optical from interaction. the unperturbed For the effective n-Voigt Hamiltonian geometry the Ho , calculation with the requires modification of the calculation of the matrix element for the ED combined resonance transition, A oc + 0) (n). The velocity operator for that transition, A due to H(K ), with e = C, was V = ioKs(kxo) a ). (2.3.63) A For incident wavevector q = qqr this becomes V = io)Ks(kxo)4( - i/s)qk4 . If we keep only the component which contributes to the 2o (2.3.64) c + 0os transition we get V = q 2oKk (2.3.65) . The matrix element between aC(O) and bc(2) is (2.3.66) Vfo = v2iqoK , which is proportional to B. This is higher order by a factor of B than the matrix elements for spin resonance and 20o. A In the Faraday geometry, with the optical wavevector q parallel to is impossible for H(Ks) to cause the 2 that the contribution of K mechanisms. c + ws(a+) transition. , it This implies to the transition is a 1-to-1 mix of EQ and MD This is understood as follows. If the transition were pure EQ in nature, the matrix element would involve the combination eq_ + eq , which is the m = - 1 component of (eq)(2). Similarly, if the transition were pure MD in nature, the matrix element would involve the combination eq - e_q , which is A i(exq) . A 1-to-1 mixture of these two combinations is required to make the e_q part to drop out, producing the result of the direct calculation. Contributions to the 2c c + co s matrix elements from the parameters g" and a few 0 are computed in a similar fashion, except that there are The first is that there is an additional MD part which comes complications. from the parts of H(g") and H(y) which depend explicitly on B1 . This must be For the added to the parts which result from the explicit dependence on A . A parameter g" the two parts cancel for n-Voigt. For q parallel to the B part of H(g") gives a finite contribution to the (a-Faraday transition. There is an additional contribution proportional to g" which results from mixing of a-set and b-set wave functions due to H(g"), proportional to k . This part is computed with the A l part of H(g"), including the eiq discussed above. spatial variation, as Notice that the contribution of H(g") to 2m + m is also a 1-to-1 mixture of MD and EQ mechanisms, but that now the two parts subtract instead of add, so the matrix element is finite for a+-Faraday and zero for x-Voigt. The matrix elements, given in Table 2.7. including the contributions from H(yo), are It is of interest that the contribution of Ks, g" and yo to the spin resonance matrix elements may be obtained in a similar fashion, and that the result also contains a mixture of MD and EQ components. The dependence of the Voigt-geometry matrix elements on B0 , based on a PB model calculation, was given in the preceding section. Table 2.7 Effective velocity operators for axial model MD-EQ transitions. A Transition A At Type q, e V 0s(Rt) -1 MD 1, 5 (i/8)qa_g* os(a_) -1 MD , - (- 2oc(a_) +2 EQ I, ( - i/4)qk+/(sm*) 2o c + )s(n) +1 EQ+MD 1, 20 c + +1 EQ+MD r, + s(o+) Correction factors pg c+ 2 = (20 _k 2/8)qa_g* _ (1/v )qa [K 0co+ 0 (W 0 -3) _[g g" + )/(o + o ) and gt3 =-(30c - 8 3T0 (W -5)] o )/(o) + cO) are A required to account for the contribution [e-v0 , iS]fo which results from wave function mixing. Here W - (B4 + B 4 + x y )/B4. z (2.3.67) The transition matrix elements originating from the ground-state subband aC(O) limit conditions) quantum (assuming k , k+ -- simply makes the replacements geometry with spherical model for the principal A q = qy 2sv'2 , Y_ and one for 2 - The resulting matrix elements and spin-flip transitions, and zero otherwise. peak absorptions since compute, are quite easy to the Voigt transitions in are given in Table 2.8. Matrix elements and peak absorptions for Voigt transitions at k =0. Table 2.8 a(peak) V Type At Transition 2 po v2-/2m* ED +1 +(l) 2 j C + o0 (t) S 0 ED -1 MD - s2o0K S pO (4p K 2)(2g B )2 B 0 1 S 7 2 2cny n o Ss(t) 1 qg* 2 o 3 B m m4 2cy 2oC(1l) EQ +2 - V2iq/2m* 2cy no 20 + s(X) +1 EQ+MD V2iqwK '1p p = m/m* + g*/2 and p 2 2mm* + g*/2 mc m* (2 2 2cy 24 B = free electron cyclotron energy. o 0 2 3 4g B 2 n 8g B (4p K2 20 B B) B 0 mc 3 3. MAGNETOABSORPTION AND FIELD-REVERSAL EFFECT IN n-InSb In this chapter I present the results of my recent magnetoabsorption experiments in n-InSb at wavelengths near 10 pm and magnetic fields up to 15 T. The most striking feature of these new measurements geometry is the observation of a significant in the Voigt field-reversal effect in the absorptions at 2o c and 2(oc+Ocs , in good agreement with the theory presented in the previous chapter. factors of 2.5 The observed effect involves a significant change, by to 3, of the magnetoabsorption coefficient for these transitions upon reversal of the direction of the applied magnetic field. polarizations for which the effect is observed are the a_ 20c transition and the TCpolarization for the result is (EQ and/or surprising because MD) inversion-asymmetry the which causes 2 0c+Os wavevector-dependent the effect by transition. absorption interference The present mechanism with the induced ED absorption was overlooked or thought to be of the interference the q-dependent The polarization for the insignificant in all of the previous work on magnetoabsorption. occurrence two The actual effect is reasonable from the perspective absorptions have selection rules which are that similar to those for 2-photon processes (absorption and scattering) in the isotropic model. In this latter case the An = 2 processes are known to accompany the An = 0 processes. Here n is the Landau level quantum number in the conduction band. The observation of the field-reversal effect in the 2oc(a) transition is the first time that the effect has been seen in a spin-conserving transition. spin-conserving effect transition between levels (PB was predicted by Bassani et al. [Bassani 88] The for a the a+(0) and a+(2) heavy and light hole valence band notation) with the same polarization, but the An = 2 conduction band transition was said to be too weak to be of significance. This chapter is organized as follows. After a brief review of the relevant background for the experiment, I will describe the conditions of the experiment. I will then present the experimental results and discuss how these results compare with predictions of the theory presented in the previous chapter. 3.1 Background on Magnetoabsorption and B-Reversal Experiments Magnetoabsorption in n-InSb has been the subject of numerous research papers and review articles over the past 40 years. The present work was begun as an extension of work done at the MIT Francis Bitter National Magnet Lab by Aggarwal et al. [Aggarwal 71a] on the SFR laser, and Weiler et al. [Weiler 74] on magnetoabsorption magnetoabsorption, and experimental studies. served the as SFR motivation These included [Huant 85]. Pidgeon 80, affects laser. Reviews which interference resonance is effect in early articles called in n-InSb the by the subsequent [Weiler 78], include Seiler 92]. Weiler 81, for work on theoretical [Goodwin 83], [McCombe 75, Zawadzki 79, reviews of Dobrowolska et case, al. intraband The magnetic field reversal electric-dipole-magnetic-dipole spin-resonance and [Grisar 78], Earlier magneto-optics were given by Lax [Lax 60, 61]. effect, My presented in Chapter 4, demonstrated the anisotropy of the absorptions, and which was discovered [Dobrowolska 83]. (EDMD) in spin It was extensively developed in a series of papers by the Purdue group during the period between [Kim 89a]. 1983 and 1988, culminating in the review by Kim et al. The effect is also covered in the recent review of magneto-optics by Rashba and Sheka [Rashba 91]. Notable historic work, in the review discussed articles, includes the observation of CR in InSb by Dresselhaus et al. [Dresselhaus 55a]; observation of CR harmonic absorption in p-type a semiclassical explanation; McCombe Ge by Lax et al. [Lax 60], with observation of combined resonance in n-InSb by [McCombe 69]; observation of CR harmonic absorption by Johnson [Johnson 70]. The LO phonon assisted absorptions were observed by Enck et al. and described theoretically by Bass and Levinson [Enck 69, Bass 65]. As mentioned above, the field reversal effect was overlooked or rejected in several [Grisar 78], [Johnson 70]. effect. studies. These [Chen 85b], The include [Gopalan 85], first four [Weiler 74], [Favrot 75, 76], [Lee 76], [Bassani 88], and the earlier work of studies did not look for a field-reversal The articles by Johnson, Gopalan and Bassani imply or state that the B-reversal effect does not occur to an observable degree for the 20 c 20 +o C S conduction band transitions. and 3.2 Experimental Conditions This apparatus, section and provides procedures a description used to of the InSb study the samples, magnetoabsorption experimental for intra- conduction band transitions. SAMPLES: Magnetoabsorption measurements were made on two InSb samples in different orientations at temperatures T near 25 K and 77 K. The InSb samples were n-type, tellurium doped, with carrier concentration ne about 2 x 1016 cm - 3 and length about 2 cm. The samples were obtained from Cominco American, Inc., Spokane, WA, and their specifications are the following. InSb #16 -- Lot W3173-B, Te doped, n-type Dimensions 9.7 x 8.1 x 21.3 mm 3 - along [111], [112], [T10] n = 1.5 - 2.4 x 1016 cm -3 p -3 = 2.6 - 3.4 x 10 2 cm (77 K) (77 K) g = 1.0 - 1.2 x 105 cm2/VN s (77 K) InSb #17 -- Lot W3262-C, Te doped, n-type Dimensions 9.5 x 7.9 x 22.6 mm 3 - along [110], [112], [111] n = 1.7 - 2.2 x 1016 cm -3 (77 K) p = 2.6 - 3.1 x 10- 3 Q cm g = 1.1 - 1.2 x 105 cm2VN s (77 K) (77 K) The end faces (smallest dimensions) are ground and polished, but not etched. EXPERIMENTAL SETUP: Optical measurements were made in the Voigt geometry with the magnetic field B wavevector directed q. vertically and the light propagating They were made in the middle infrared horizontally with spectral range at wavelengths between 9.6 and 11.6 microns. The experimental setup consisted of the following apparatus shown in Fig. 3.1. Liquid He Cold-finger Dewar Bitter Magnet Liq. He cooled Germanium Bolometer IRCoil Heater Chopper Fig. 3.1 Polarizer Filter Experimental IF setup spectra in the Voigt geometry. in the text. for obtaining magneto-optical absorption The individual components are described MAGNET: The magnet was a Bitter solenoid capable of fields of 0 to ±15 T in a 4-inch diameter bore. The InSb samples were mechanically fastened to a copper sample holder which was screwed against the copper end plug of the liquid helium cold-finger of a stainless steel research dewar made by Janis Research Co. The optical windows were 2 mm thick zinc selenide, at room temperature. IR SOURCE: The IR source was a Model PE-1 coilform heater from Buck Scientific, rated at 12 to 14 amps. It was operated at 14.0 amps, at a power of 44 watts. The effective black body temperature is estimated to be approximately 1000 0 C. (This was not measured, nor was the information available from the supplier. Globars of SiC supplied by Perkin Elmer are rated at temperatures of about 1100 0 C.) The active area is 0.128 inch diameter by 1 inch long, and consists of 4 strands of nichrome wire wound tightly on a porcelain cylinder. source is imaged reflective optics. on the entrance slit of the monochromator The with f/3.5 A long-wave-pass filter is placed immediately in front of the slit to eliminate diffraction orders higher than the first. MONOCHROMATOR: A Spex model 1680B, 0.22 meter double grating monochromator was used. The gratings were 75 lines/mm, blazed for about 9.8 microns. A long wave pass filter at the entrance slit was dielectric coated Ge, with 5% cut-on at 7.6 microns, transmitting 80% (average) from 7.72 microns to 15 microns. Coating Lab, Inc., Santa Rosa, CA, No. L07600-9B) is given by :D" " (Optical The spectral resolution R R(gm) = 0.5(slit width/220 mm)(13.33 gm) cosO 6 cm' for 2.5 mm slit, at 10 gm OPTICS: Reflecting optics were used to image the exit slit of the monochromator onto the sample and then onto the detector. surface aluminized glass or pyrex. The mirrors were standard front- The focusing mirror was of 8-inch diameter and 1 m radius, in a 1:1 imaging configuration. The collecting mirror was of 6-inch diameter and 0.8 m radius and approximately 1:1 imaging. DEWAR: The stainless steel optical cold finger dewar was made by Janis, Inc.. The main body of the dewar was 8 inches in diameter, with a 1 1/8-inch diameter liquid helium cold finger. The 2-inch o.d. outer tail has two 2-mm thick by 3/4-inch diameter ZnSe side-facing windows for IR transmission. SAMPLE HOLDER: The InSb sample holder was machined from 1.1 inch diameter copper. The sample is held against the copper with Dow High Vacuum Grease and clamped with beryllium copper differential finger contraction stock. Stresses of copper and induced in the InSb were sufficient sample by the to fracture the bottom of the sample after several thermal cycles. The result was that the bottom broke free of the remaining sample to a depth of about 1 mm. The induced stress in the sample was nonuniform, since it was applied at only one face, and the experimental results are in good agreement with the strain-free theory. Additional work should be done to determine whether there are any stress related effects. DETECTOR: A Ge bolometer detector from Infrared Laboratories, Inc., Tucson, AZ was used to detect the IR light. It consisted of a Model HD-3 liquid helium dewar with model LN-6 amplifier and Ge bolometer unit #325. thick by vertical.) 1 inch diameter KRS-5 There is an internal The Detector has a 2 mm window facing the horizontal. filter wheel having six 1/2-inch (Plane is diameter slots occupied primarily by far infrared filters which were not used in the present experiment. One slot was vacant, and this one was aligned between the window and the light cone which led to the bolometer element. The optimum signal was obtained when this vacant aperture was misaligned by about two thirds of its diameter from the axis of the light cone. SIGNAL AND NOISE: The light was chopped at 150 Hz and the output from the detector preamp was measured by a Princeton Applied Research (PAR) 5101 lock-in amplifier. With the PAR set on 250 mV scale the output was 1 V dc for 250 mV input at the reference frequency. With 2.5 mm slit width, the maximum dc output signal for light transmitted through the sample at B = 0 was: 0.54, 0.31 and 0.15 V for 9.6, 10.6 and 11.6 pm light in al polarization, and 0.38, 0.15 and 0.05 V for 9.6, 10.6 and 11.6 gm light in n polarization. The noise level in all cases was 0.002 V. PROCEDURE: 1. Set the heater current to 14.0 amps. 2. Turn on Spex 1680B controller and 150 Hz chopper (30 Hz motor, with 5-slot wheel). 3.Calibrate Spex 1680B (75 lines/mm) and set to 600 for 9.6 microns, 662.5 for 10.6 microns, or 725 for 11.6 microns. 4. Set wire grid polarizer (gold on AgBr) for 7t or a 1 polarization. 5. Set Spex slits to 2.5 mm. 6. Turn Ge bolometer bias and preamp on and uncover KRS-5 window. 7. Set lock-in amplifier (PAR #5101) to 250 mV scale, with prefilter at 0.3 s and postfilter at 0.1 s. 8. Set Keithley 182 digital multimeter to 3 V scale with internal filter off. 9. Adjust optics and dewar position for optimum signal. 10. Adjust filter wheel on bolometer, and reoptimize optics. 11. Sweep B from 0 to ±15 T and back. (5-min or 2-min sweep rate from minimum to max, or max to min.) 3.3 Results of the Magnetoabsorption Experiment The most significant feature of the experimental results presented in this section is the observation of a strong magnetic field reversal effect in the 2(oc+o the Yl s absorption for the n polarization, and in the 2o polarization, in the Voigt geometry. investigated, and the 3.2, shows theory predicts c absorption for (The Faraday geometry was not no effect for this geometry. See configuration which [Gopalan 85].) Figure displayed the largest B0 11[111]. the transmission field-reversal data effect. for the The data is for InSb #16 The wavelength is fixed at 10.6 gm in the the magnetic field varies from -15 T to +15 T. with Yl polarization, and The curve consists of two traces for each sign of B0, corresponding to the field being swept in the two possible directions. labeled with the The transmission minima in the figure are identified and aid of the fan diagram transition energies versus B . [Goodwin 83].) of Fig. 3.3 which displays the (Small anisotropy of the energies is neglected In Fig. 3.2 we note that the infrared transmission is maximum when the magnetic field is zero, and decreases, the field is increased in either direction. with strong oscillations, Both positive and negative as field directions are shown in order to emphasize the change in the 2m c absorption, labelled '2', inter-Landau when the field direction is reversed. level transitions as follows: The labels identify the The number 1 to 4 identifies the change in the Landau level quantum number in the transition. The letter s indicates that spin-flip from spin up to spin down has occurred. The letter L indicates that an LO phonon has been emitted in the absorption process. of the observed transitions are considered to All 0.3 3 3L 0 .2 . . .. .. .. ..... 3.... 25 0..12 2 0- -0.1 -15 -10 -5 0 5 10 Magnetic Field (T) Fig. 3.2 a Transmission (detector output) vs. magnetic field at 10.6 pLm, polarization, for InSb #16 with ne=2x10'6 cm 3 , B,11 [111], q II [T10] and T = 25 K. 15 250 . 3L .. 3s 3 2sL 200 2L 2s 150 11 1sL 9. 6 mO 10, 6 urn - - - -, - 0 " Is 20 0 - -- - -- 40 60 80 100 140 120 160 180 200s Magnetic Field (kG) Fig. 3.3 Fan diagram following [Weiler 74] of intra-conduction and [Goodwin 83]. band transition energies, The dashed curves give the energies of the LO-phonon assisted transitions, in which an LO phonon is emitted. The curves were computed with the PB model parameters of Goodwin et al., using their value of h0Lo = 24.4 meV. in the center Circles give are photon the approximate energies used in the Horizontal lines present experiment. magnetic field positions of the absorption peaks for 10.6 tm. 100 occur in the extreme quantum limit and to originate from the lowest Landau sublevel, denoted aC(O), in the conduction band. Therefore '2' denotes the double cyclotron resonance transition between the aC(O) and aC(2) conduction band levels. is Note from the fan diagram that the energy of the 2%c somewhat transition smaller between than ac(O) twice and the ac(1), energy so the of the designation energy as 2o c is more symbolic than numerically precise. cyclotron of transition resonance the transition The most important aspect of the transmission shown in Fig. 3.2 is the significant change in the depth of the 20C minimum when the direction of B 0 is reversed. present case we see that the 2 c For the transmission nearly saturates to zero for the negative direction of field, but remains well above zero, at about 14%, for positive B The 'zero' . line which is displaced about 0.005 units below the field axis is the detector signal obtained by sweeping the field with the IR source blocked. In order to convert transmission to absorption I used the formula Ac(B0) = a(Bo) - a(O) = - Iln[I(B )/I(O)]/L . Here I(B ) and I(0) are the detector signals (3.3.1) at finite field and at zero field, after subtracting the detector signal with the beam blocked, and L is the length of the sample. This formula assumes that the zero field absorption is high enough that multiple passes inside the sample can be neglected. corrected formula, taking multiple passes into account, but neglecting The any change in the absorption which occurs when the direction of the wavevector q of the radiation is reversed, requires use of the formula for the transmission (1 - R)e-aL (3.3.2) T = 1- R 2e -2cL 101 Here (n - 1)2 R = - 0.36 (3.3.3) (n + 1)2 is the single surface reflection, a is the absorption coefficient, and L is In the present case R2e - 2 aL is less than 0.01 in the the sample length. 9.6 pm to 11.6 pm range at B ° = 0 if one uses the value 1.0 cm - 1 for the absorption at 11.26 ptm [Patel 71, Weiler 74], with L = 2.1 cm. One must use the X- 2 dependence of the free carrier absorption to correct for the different wavelengths. We next use Eq. (2.3.1) to compute the absorption for the 20 c peaks. Using I(B )/I(0) = 0.14 for positive B and 0.015 for negative B absorptions Aat of 0.92 cm - and 1.97 cm - . we get A reasonable estimate of the error bars for the stronger absorption is obtained by assuming that the zero offset (the 'dark' signal) could be wrong by 50%. This would make I(B )/I(0) equal to 0.0075 or 0.0225 instead of 0.015, since the transmitted signal averages to These values would correspond to absorptions about 0.00 at the peak position. of 2.30 cm -1 and 1.78 cm - , instead absorption near the 2o by taking c the slower magnetic field absorption Lorentzian lineshape. Better results for the peak could be obtained by using a shorter sample, or blocked and then unblocked. chosen, of 1.97 cm - 1. peaks scans near the peak with the light beam Note that if the transmission zero is improperly will deviate significantly from the expected If too low a zero is used, the absorption peaks will appear to be flattened on top, and if too high a zero is used, the peaks will be excessively pointed on top. Care was taken in the experiments to mask the samples so that no light 102 However, there was evidence of some light could leak around the samples. leakage in an early which was the first sample data set for sample #17, The evidence for this came from the aL absorption at 11.6 gm at high studied. fields near +15 T where the absorption saturates due to the strong absorption at the Here the transmitted signal from (See Fig. 3.3). transition. C+LO signal with the beam the detector at saturation was higher than the 'dark' Correction was made blocked by about 10% of the transmitted signal at B ° = 0. by shifting the 'dark' The data was used to obtain line up by this amount. better understanding of the absorptions, but is not presented in the figures. in the early experiments of the data were made Slight field displacements where the time constant of the electronics was excessively long. Fig 3.4 shows typical transmission data for the i polarization. For this polarization the detected signal at zero field is weaker than it was for Gl' due to the lower reflectivity of the gratings, but the magnetoabsorption is The strongest absorption peaks in this polarization cause the also weaker. transmission to drop to only about 20% of the zero-field value, so the error Note that only the due to uncertainty in the zero line is lower than before. 20 c +oos absorption, labeled '2s', shows a significant when B0 is reversed. Fig. shows 3.5 the magnetoabsorption vs. B for sample B II [111] and q II [T10], for polarizations n and oL, at T = 25 K. significant 2o c feature in this figure in the absorption is _l polarization measured from with #16 The most is the strong change in the absorption when the magnetic field is reversed. the base of the peak it is at If the found that the absorption due to the 2o c transition changes by a factor of about three upon reversal of the field. This compares 103 with a factor of 2 for the spin resonance absorption measured by Dobrowolska et al. and Chen et al. in samples with lower carrier concentration at 118 jIm [Dobrowolska 83, Chen 85b]. None of the other peaks for this polarization change by significant amounts when the field is reversed. are those at 2o c+o s The peaks of greatest interest besides the 20 c peak and 3 c, which are normally due to inversion asymmetry and 0.15 0.1 0.05 0 -0.05 ' -15 -10 -5 0 5 10 Magnetic Field (T) Fig. 3.4 Transmission (detector output) vs. magnetic field at 10.6 lam, t polarization, for InSb #16 with ne =2 x06 cm-3 and T = 77 K. 104 B 11 [110], q II [T10] 0.6 0.5 E 0 0.4 C 0.3 a I 0.2 0.1 0 -0.1 -15 E C.) 1.5 01 I 1 -10 -5 0 5 10 -10 -5 0 5 10 e 0.5 0 -15 Magnetic Field (T) Fig. 3.5 Magnetoabsorption vs. magnetic field at 10.6 Lm for InSb #16 with n e=2x1016 cm - 3 , B oII [111], (b) q II [110] and T = 25 K. L- polarization. 105 (a) ix polarization; warping [Weiler 78]. geometry with and warping, polarization as was and are is in violation of the selection pointed out by Zawadzki peaks LO-phonon-assisted orientation, The existence of the 30 c peak (or shoulder) in this at nC +LO of are no particular [Zawadzki 90, isotropic interest rules with in the associated 92]. respect present The to crystal work, except that they provide a good reference against which to measure the peaks of interest. C+0 Lo, occurs near 18 T for 10.6 gm radiation and is The n=l peak, largely responsible for the increasing absorption observed at large B . The peaks for n=2 to about 5 or 6 are seen as a series with decreasing intensity at fields below 9 T. The linewidth of the absorptions in meV may be found by multiplying the linewidth in magnetic field by the slope of the curve of The absorption for the it polarization displays transition energy in Fig. 3.3. only three peaks out to ±15 T. These are identified, with the aid of the fan C +0 +LO, diagram of Fig. 3.3, as the and 3C transitions. 20 + C +0 S+0LO peak is seen to be quite a bit wider than the other two. The Part of the extra width is real, and part is due to the lower slope of the transition energy curve vs. magnetic field. Of these peaks, only the weak 20c+0 s peak, which violates the selection rules of Table 3.1, shows any significant change upon reversal of B . The smaller of these two peaks is seen to have a pronounced shoulder on the low-field side. in agreement with the selection rules. The 3%oc peak is quite prominent, The it spectrum is simpler than the 0l because the absorbed photon contributes no angular momentum, corresponding to v -induced transitions, while in the latter case the photon contributes both +1 and -1 units of angular momentum, Z_ corresponding to the operators v+ +- and v. Figure 3.6 qshows and II [10],the formagnetoabsorption polarizations SII [110] B0 11[110] and q II [110], for polarizations 106 vs. B nt and for #16 0and , at sample T 77 K. TL, at T= 77 K. with (The (The higher temperature was used because a cold leak in the dewar prevented the use of liquid helium.) This geometry is the optimum one for the field-reversal effect in the 2co +os absorption for n polarization. The effect in the 2s peak is seen to be quite pronounced, with a change in absorption by a factor of is reversed, where the absorption is measured relative to about 2.6 when B the average height of the bases of the peaks. quite a bit larger than the C+ +oLO peak on the positive field side, and side. quite a bit smaller on the negative B strong peaks at 2o) and 3o c . Notice that the 2cc+cs peak is Notice the rather surprisingly All of the absorption peaks are broader at the higher temperature, but the breadth of the 3c c peak in particular causes one to speculate 2o + o that other some absorption be might which occurs at nearly the same field. + is in polarization violation The peak at 20 rules for of the selection inversion s polarization, For the effect is still strong the for 2 For the present case the absorption changes by a factor of 2 instead of 3. 2 (o cos c+ c [111]. absorption, but not as strong as in the previous figure for B along see that the 7 peak when the temperature is lowered, as field-reversal the for asymmetry will be seen in another figure for the case where q is along [111]. S01 as The peak shifts to and warping, and might be somehow related to impurities. lower fields closer to the 2C0c+o such contributing, We absorption has completely disappeared and that the 3oc absorption is now quite resolvable above the broader 2oC+cLO peak. Figure B II [T10] geometry 3.7 shows and the the magnetoabsorption q II [111], interference 20c( 20 +O (r) and B 0 II [110], q 11[T10] ) geometry. but One 107 is at sample with In this for both the in the observed weaker than significant #17 T = 25 K. is effect (field-reversal) for B polarizations, for both transitions, vs. difference it was in the present case is the reversal of the positions of the stronger of the two peaks at 2wcc(o ) relative to those at 20c+(s(c). This effect will be shown to be in 0.6 0.5 0.4 -E- 0.3 CO, &0 0 0.2 0.1 0 -0.1 - -10 -5 0 5 10 -10 -5 0 5 10 (b) E 1.5 0 1 I- es 0.5 0 L -15 Magnetic Field (T) Fig. 3.6 Magnetoabsorption vs. magnetic field at 10.6 gm for InSb #16 with n =2x1016 cm- 3 , B 11 [110], e o (b) .1 polarization. q II [110] and T = 77 K. 108 (a) it polarization; 15 (a) 0.6 0.5 E 0.4 ov 0.3 I el 0.2 0.1 0 -0.1 -10 -5 0 5 10 -10 -5 0 5 10 (b) 2 E 1.5 C 1 I e~ 0.5 0 -15 Magnetic Field (T) Fig. 3.7 Magnetoabsorption vs. magnetic field at 10.6 lam for InSb #17 with n =2 x1016 cm - 3, B II [T10], (b) q II [111] and T = 25 K. _L 1 polarization. 109 (a) it polarization; agreement with the predictions of the theory. Notice in the 7n polarization that the forbidden 2o c peak appears to have split into two peaks. is not understood, liquid nitrogen The reason but the higher-field peak is found to become strong at temperature, temperatures near 25 K. while the lower-field peak becomes strong at The simultaneous appearance of the two peaks leads to speculation that T was slightly higher than 25 K, possibly due to sparseness of the silicone grease used for thermal contact. The amount of grease was minimized in an attempt to reduce the mechanical stress induced in the sample upon cooling. Figure 3.8 shows the magnetoabsorption B II [001] and q II [T10], orientation the interference for both effect vs. polarizations, is not B at expected polarization because the 2+os( (n) and 2oc(0) for sample #16 T = 25 K. to occur In for are both zero when the appearance is along [001]. of a strong 20c(O ) direction of B. change transition for the B 11[001] case was We see that both the 2 0c(YI) and The 2c +0 s(t) absorption is quite small, but shows a clear The approximately 1.0 cm - ' when B it and F3 are finite and show small changes on reversal of the on reversal of B. For the either The violation of the selection rules by first pointed out by Weiler [Weiler 76, 78]. 20c+os(t)absorptions this absorptions are both forbidden via the inversion asymmetry mechanism, since the angular functions F A with 2 0c(aL) absorption is rather is negative and 1.1 cm -' when B large, being is positive. polarization the 20 c absorption is allowed via inversion asymmetry and has a strength of about 0.3 cm - 1. The 20 +cos and 30 transitions are both forbidden, but are seen to have finite magnitudes of about 0.03 to 0.05 cm- . For the _L polarization the 20c+ s and 30c absorptions are both allowed and observed. 110 0.6 E 0.5 0 0.4 & O 0.3 O 0.2 0.1 0 -0.1 -10 -5 0 5 10 -10 -5 0 5 10 (b) 2 E 1.5 CO 0 rnIs 1 0.5 0 -15 Magnetic Field (T) Fig. 3.8 Magnetoabsorption vs. magnetic field at 10.6 gm for InSb #16 with ne =2 x 10 16 cm- 3 , B o II [001], q II [T10] and T= 25 K. (b) al polarization. 111 (a) t polarization; 3.4 Discussion of Magnetoabsorption Results I now present a quantitative description of the magnetic field reversal effect in the magnetoabsorptions at 2o c and 2cc+ s . The effect is caused by interference between the q-dependent (MD and EQ) and inversion-asymmetryinduced (ED) components of the absorption. I use the decoupled model because of its simplicity, but make modifications based on the PB model to obtain results which are more accurate. After the discussion of the transitions which show the field-reversal effect, I make a comparison with theory of the other inversion-asymmetry and warping-induced transitions. We begin with the function F (oapy). the spin 2 Oc+s(7) transition which depends on the angular The description resonance transition, and of this transition is similar to that of is simpler than transition which depends on both FI and F3 . 2 o c+o s(t) transition is mixed EQ and MD. that of the 20c(1_) The q-dependent part of the If this mechanism is considered by itself, the absorption computed from the PB model is 0.015 cm - 1 at a field of 10.2 T and a transition energy of 117 meV (10.6 pm wavelength) for carrier concentration 2 x 1016 cm - 3 and FWHM linewidth 30 cm - 1. (See Fig. 2.15.) The inversion-asymmetry induced electric dipole (ED) part of the transition, taken alone, causes an absorption of 0.32 cm - 1 for B 2.19). directed along [110] (Fig. Notice from the figure that this absorption is nearly independent of whether the parameter C' or G causes the transition. The matrix element for this part of the transition is proportional to F 1, which is maximum along the [110] directions, and zero along the [001] and [111] directions. The interference effect is maximized when q is along [110], since this makes both the q-dependent and inversion-asymmetry-dependent matrix element purely imaginary, parts of as in the case of electron 112 the transition spin resonance [Chen 85b]. SFI , we If we choose B ° along [110] with q II [T10], so as to maximize would expect coefficients absorption the for two the opposite directions of B to be 0 jiVO-0T5 + i03-212 = 0.47 cm-' or 0.20 cm- 1, with an average value of 0.335 cm - . This agrees well, to within about 20%, with the absorptions measured in the experiment, background due to other absorption processes. after subtracting the Next consider the experimental geometry which places B 0 along [T10] and q along [111]. In this geometry the q-dependent part of the transition matrix element is the same as before, since it is only weakly dependent on sample orientation, and since B direction which is equivalent to [110]. is along a The ED part of the matrix element, proportional to F 1, has the same magnitude as before, but now has both real and imaginary parts. This causes the interference to be somewhat weaker. Evaluation of F for this geometry gives FI= (1/16)-J- compared with i (1/16)( - i) , for the previous geometry. The absorption coefficients for the two opposite directions of B 0 are now given by IiV.OTT5 + V032 (0.577 ± 0.816i)1 2 = 0.45 cm 1 or 0.22 cm -1. (Notice that only the imaginary part of F changes sign when B is reversed.) The interference effect is only slightly weaker for the 2 c+cs(t) transition in this geometry, as was the case for the as(7) transition [Chen 85b]. Now we consider the interference effect for the 20c(O) transition. The analysis is similar to that given by [Bassani 88] for the heavy to light hole 113 valence band transition a+(0)-- a+(2). level even though the wave ladder.) The q-dependent meaning that moment. (Note that a+(0) is a heavy mass function is the bottom rung in the light-hole 2 part of the the transition state contains c(l) transition is EQ in nature, an oscillating electric quadrupole If this mechanism is considered alone, the absorption computed from the PB model is 0.62 cm - at a field of 11.6 T and a transition energy of 117 meV, for carrier concentration 2 x 1016 cm - 3 and FWHM linewidth 30 cm (See Fig. 2.14). . The inversion-asymmetry-induced electric dipole (ED) part of the transition, considered alone, causes an absorption of about 0.10 cm - 1 when B is along [111] (Fig. 2.17). Thus the EQ-induced absorption for calculated to be stronger than the inversion-asymmetry-induced This result contradicts statements by Johnson and Dickey 2 (c 1l) is ED absorption. [Johnson 70] and Bassani et al. [Bassani 88] claiming that the EQ component of the absorption is negligible. It differs from the 20c+o (n) and o (n) spin resonance cases where the q-induced absorption is smaller than the ED absorption. element for the ED part of the 2 oc((L) The matrix transition is proportional to F 3 + FI (decoupled approximation), which is maximum near the [111] direction, and zero along the [001] direction. The interference effect is maximized when q is along makes [T10], since asymmetry-dependent this both the q-dependent and inversion- parts of the transition matrix element purely imaginary, as in the 2o +o (n) and os( ) cases. Figure 3.9, at the end of this section, A shows the imaginary part of F 3 + F1 versus angle 8, measured from the z axis, for the case q II [T10]. the value If we choose B along [111] the function F 3 + F has i/24 = 0.2041i, and the expected directions of B are 0 ilx/076 ± iVO- = 1.22 cm- or 0.22 cm , 114 absorptions for opposing with an average value of 0.72 cm - '. experimental values. contribution The These are significantly smaller than the discrepancy is expected of ionized donors [Zawadzki 80]. to result from the The matrix element for this mechanism is expected to have a random phase, so the absorption due to this mechanism should simply add to the absorption inversion-asymmetry mechanisms. of the combined EQ and We can estimate the contribution of the ions from the data for case with B II [001] and q II [110], for which both F and F 3 are zero, implying no contribution from inversion asymmetry and no field reversal effect. The peak 20oc(aj) absorption for this case is 1.0 cm suggests an absorption of 0.38 cm - ' due to ionized impurities. 1 which The absorption for the opposite directions of B0, for the [111] case, would then be IiVO'O2 + i(TM-12 + 0.38 in much better 0.53 cm - '. agreement with the experimental values of 1.7 cm' and Increasing the inversion asymmetry contribution from 0.10 cm - 1 to 0.13 cm - 1 improves the theoretical result purely phenomenological require absorptions fit, neglecting to 1.70 cm 1 and 0.56 cm - 1. the contribution of the ions, of 1.03 cm - 1 due to EQ alone, and 0.083 cm' inversion asymmetry alone. what follows = 1.60 cm - 1 or 0.60 cm - 1, A would due to These values differ substantially from theory. In we will use the value 0.13 cm - 1 for the ED absorption for B 11[111], which is 30% higher than the value obtained with the PB model with the parameters of [Goodwin 83] with inversion asymmetry parameter 8 = 65 a.u. We next consider the experimental geometry with B along [T10]. along [110] and q The EQ part of the transition matrix element is unchanged, being purely imaginary, and causing an absorption of 0.62 cm - '. The ED part of the matrix element is proportional to F 3 + F1 , which now has the value il8. 115 This is smaller by a factor 0.6124 = VT38 ED absorption then changes than the B 11[111] case. 0.13 cm -' from to 0.049 cm - 1. The effective The actual absorptions predicted by theory, for opposing directions of B 0, are 2 SiVC062 ± iV1T4 with an average + 0.38 = 1.40 cm - ' or 0.70 cm - 1, of 1.05 -1 . cm - The experimental values for the 2o(o transition in this geometry are 1.3 cm -1 and 0.59 cm - ' at 77 K. 1) The values at 25 K are expected to be about 25% larger, or about 1.63 and 0.74 cm - 1. The change in peak absorption with temperature was obtained from measurements made at 77 K and 25 K with B II [111] and q II [T10]. 0 We now consider the experimental geometry with B along [T10] and q along [111]. The EQ part of the transition matrix element remains imaginary, and unchanged. The ED part of the matrix element, proportional to F 3 + F1, now is and differs from its previous value both in magnitude and phase. complex Evaluation of F 1 and F 3 for gives F = (1/16)- i - , F3 = (1/16)( 5F - i compared with -(i/16) and 3i/16 for the previous case. F3 + F = (1/8) 2' , The sum is - i (magnitude v2/8), compared with i/8. The absorption coefficients for the two opposite directions of B are now given by ivD--62 + VOT49(1.155 ± 0.816i) 12 + 0.38 = (V07-2 . + T.3) + 0.44 = 1.38 cm - I or 0.81 cm - with an average of 1.09 cm - . , The interference effect is slightly weaker for the 2o0(01) transition in this geometry. 116 Somewhat better agreement between experiment and theory is obtained if we observe that the FI (o+) contribution to the a1 absorption is smaller, relative to the F 3 (_) contribution, than it is in the decoupled model by a factor of about 0.85 . This is shown by the PB model results of Figs. 2.17 We therefore use F + 0.85F 1 in place of F 3 + F in the oa and 2.18. element. matrix If we choose B along [110], with q along [T10], the sum F3 + 0.85F has the value 0.1344i, which is smaller than the value 0.2041i which it has when B is along [111]. This reduces the absorption due only to inversion asymmetry to 0.4334 times 0.13 cm -' which equals 0.0563 cm - . We would then expect the absorption coefficients for the two opposite directions of B to be Ii/-.-6 ± i/0.056-31 2 + 0.38 = 1.43 cm-1 or 0.68 cm - 1, If B is along [T10] and q along [111], the ED part of the matrix element is proportional to F 3 + 0.85F = (1/16)( 4.15 - 1.85i{- compared with (2.15/16)i for the previous case. The absorption coefficients for the two opposite directions of B 0 are now given by Si-.-. + /T.056 (1.1144 ± 0.7026i)12 + 0.38 = (V0-.62±V 027)2 + 0.45 = 1.36 cm-1 or 0.84 cm - , with an average of 1.10 cm . The interference effect is slightly weaker for the 2o(a_) transition in this geometry. 117 The results are summarized below. General case: ac = Ii62± V2(T3(F 3+.85F) q[T10], B[111]: a = q[T10], B[001]: a = 0.62 + 0.38 = 1.00 cm-1 q[T10], B[110]: a = iv- 2+ 0.38 ± i-312 + 0.38 = 1.70 or 0.56 cm - 1 _i2i56I + 0.38 = 10.7874i ± 0.2373il 2 + 0.38 = 1.43 or 0.68 cm - ' q[111], B[T10]: a = 10.7874i + (0.2645 + 0.1668i)j 2 + 0.38 = 10.7874i ± 0.1668il 2 + 0.45 = 1.36 or 0.84 cm - 1 The complete angular variation of the field-reversal rotated in planes perpendicular to q is computed below. matrix elements which contribute to each absorption. effect as B0 is Table 3.1 gives the The wavevector q is A parallel to il. Table 3.1 Matrix elements of the effective velocity operator for q-dependent magnetic dipole/electric quadrupole, and electric dipole transitions in the Voigt geometry, based on the decoupled model. Transition: V (MD/EQ): fo V (ED): fo 20 Cs() -l g*q 12F* 8 s 10 (o ) - 4V(F +F )8 s 13 (t) -v2 icO KsIq S V2m * 1 2 c+( 0 -20V2 F 8 s 10 The ED contribution of the ionized impurities is not included in the table and is taken to add incoherently to the 2 oc((l) absorption. the other two transitions. 118 It is neglected for The MD/EQ matrix elements in the table all have phase - i. The ED matrix elements for the -F 1, and 20o s, and 2cc+ since respectively, [Cardona 86c]. a = (v- q s and 86 both are and real positive is then found from The absorption for os() y1 Re(16F,)) 2 0 + Vii 110 Im(16F 11))2 + (V Im(F *) = - Im(F1). where I used transitions have phases of F 1*, -(F 3 +F1 ) s The absorption for 2Oc+os(nt) has the same The two absorptions therefore expression, but with different aq and a o. show constructive or destructive interference on the same side of B0=0. The absorption for 2c(a ) is found from a = (v +V 111 Im(F)) 2 + (vrc' Re(F)) 2 + a. 111 ions IF, is 3 times larger Note that IF3 F - V24(F3+F ), with XL0.85 at 12 T. where than q 16F 1 has where the latter is maximum. for B 11[110] unit magnitude along [110], and F3 has magnitude 0.204 along [111]. Figures 3.9 through 3.12, at the end of this section, show the variation of F33 +FI 1 B0 is and F 1 when rotated in the (T10) perpendicular to q, with q taken along [T10] and [111]. 3.15 expressions given above. a 111 =0.13 cm - ' For 2 Oc(a~) a ions=0.38 cm - l . and calculation of Figs. 2.17 and 2.18. but it causes B II [110], 2oc+ws() a slight q II [110] I relative X=0.85, used of used a =0.62 cm', based to field-reversal the the B II [T10], I used a =0.015 cm l and a 10 =0.32 cm'. q from the on the PB The change from the case X=1 is small, enhancement case at B 0= 12 T I planes Figs. 3.13 through and 2c+%s(nr) computed at 20c(a) show the absorptions and (111) 110 119 effect q 11[111]. for the For Figure 3.13 shows the field reversal effect for the 2c(a) with q II [110]. line is for B =B A Zero angle corresponds to A absorption A =[001] and 4=[110]. and the dotted line is for B= -B A 0 . The solid One can also consider the dotted line as the continuation of the solid line for 0 between 1800 and 3600. The figure shows that the field reversal effect is finite for all angles except 0 and 1800, where B II [001] and [00T] and the field reversal effect vanishes. For the assumed orientation we see that the absorption is larger when B is up (along [001]) than when B is down, which is opposite to the case observed in my Sample #16 in Figs. 3.5 and 3.6. Rotation of my sample by 1800 about q would achieve the orientation of Fig. 3.13. Fig. 3.13 that the maximum field-reversal direction towards the [001] direction. Notice in effect is displaced from the [111] The magnitude of the displacement will depend on k in the function F, and careful experimental determination of the displacement might be used to measure k. For low fields with =1I the maximum should occur for sin0=2/3 or 0=41.80. Fig. 3.14 shows the field reversal effect for the 20c(a 1 ) absorption with A q II [111]. A Zero angle corresponds to C=[110] and =[Ii2]. A again is for B =B0 that the field The solid line A and the dotted line if for B= -B reversal effect is maximum when B ~. The figure shows is direction, and disappears when it is along any [112] direction. maxima occur every 600. than it was in weaker [110] The zeros and is down, which is opposite to the case observed in my Sample #17 in Fig. 3.7. substantially any For 0=0 we see that the absorption is smaller when B° is up (along [T10]) than when B is along for B 11[110] the previous case Notice that the field-reversal effect in with experiment. 120 the present case q II [T10], with q II [111] which agrees with the Figure 3.15 shows the field reversal effect for the 2oc+os(t) absorption for the same geometry as Fig. 3.13. Chen et al. for the The figure is quite similar to Fig. 6 of spin resonance [Chen 85b], except that the effect is stronger in the present case. It shows smaller absorption when B [110] [110], which is opposite to the case of the than when it is along is along experiment shown in Fig. 3.6, as expected from the 20c(_L) result. Figure 3.16 shows the field reversal effect for the for the geometry of Fig. 3.14. et al. [Chen 85b], case. 2 oc+os((r) absorption The figure is quite similar to Fig. 7 of Chen except that again the effect It shows smaller absorption when B is stronger in the present is along [110] than when it is along [1TO], which is opposite to the case of the experiment shown in Fig. 3.7, as expected from the 2%c( L) result. Next we will compare the observed absorption strengths at 20 3c c with those predicted by the anisotropy theory alone. et al. [Weiler 78] [Favrot 75, 76], but Weiler for the the comparison experimental used 20c+os and This was done by obtained data an incorrect c, formulation in 1975 of the radiation interaction and neglected the q-dependent EQ and MD mechanisms which cause the field-reversal effect in the 2Oc(o) and 2 cc+s(rt) absorptions. The transitions which are expected to result primarily from anisotropy at k = 0 are 2oc(t) and 2cc+os(_L) from inversion asymmetry, and 3oc(nt) from The other warping. expected to have three transitions, additional with contributions the which opposite result polarizations, from the are ionized donors, and also from the electric quadrupole (EQ) and magnetic dipole (MD) mechanisms. 121 For the observed Lorentzian linewidth 2y = 30 cm - ' (FWHM) the PB model predicts an absorption of 0.18 10.6 jtm for B II [001]. to 0.28 cm - for the 2 0c(t) transition at Here the first number is the value which results from the parameter G in the single-group approximation (G' = G) if no other parameters contribute to the absorption, and the second number is the value which results from the parameter C' if all other parameters are neglected. Both G and C' are matched to a value of the decoupled third-order inversion asymmetry parameter 68 of 65 a.u. (I neglect C relative to C'.) The observed absorption about -1 cm 1. 2oc+os(LY) transition for this the PB 0.18 cm -1 for transition model is predicts B II [111]. The 0.3 0.26 cm -' observed 0.2 cm - '. The absorptions at 2oc+os(Tl) For absorption for absorptions are B II [001] and 0.3 cm-1 and are simplified by the fact that the angular functions F 0 and F 2 associated with the 7 transition matrix element are nonoverlapping when B [111]. the and a+ parts of the is parallel to [001] and This implies that the absorptions for these two directions of B are independent of the direction of E in the plane normal to B 0 . The 3%c(7c) transition is caused by warping and is (approximately) proportional to the squared magnitude of the angular function W3. model predicts an absorption 10.6 Lm for B0 11[111]. Next consider the of 0.28 cm - ' for a linewidth The observed absorption is 0.4 cm 3mc(ol) transition, for which The PB of 30 cm - ' at absorption is . the proportional to IW2 -2W 4 12, in the decoupled approximation, if we neglect the contribution from the ions, and possibly from bound impurity atoms. absorption should be finite for the cases of B but zero for B0 11[111]. This parallel to [001] and [110], We see in the data that the absorption is in fact finite but weak for this latter case, indicating that a mechanism other than 122 warping is present [see Zawadzki 90, 92]. W2 = 0 and W -2W 2 IW2 -2W1 = 0.3125. SW- = 0.2577. 2W4 slightly relative to 12W 4 -0.85W2 = 0.25. 4 For For For the B II [001] case we have B 0 11[110] B II [T10] with with q II [T10] q 11[111] we we have have In the PB model the magnitude of the W2 part is reduced that of W so that at 7.5 T the relevant quantity is and the values become 0.250, 0.294 and 0.244, respectively. The absorption for the B II [001] case obtained with the PB model (Fig. 2.26) is 0.17 cm -1 , so the other two absorptions would be 0.235 cm after multiplying absorption absorption by (.294/.25) 2 (.244/.25) 2. and 7.5 T for B 11[001] subtracting the background absorption. absorption 2 mC+oLO peaks overlap with the broader near is about absorption at 3o 0.30 cm - '. is about 0.25 cm -1 . c is For For The and 0.16 cm - 1 observed absorption. 10.6 Lm The peak 0.35 cm- 1 approximately B II [110], q 11[111], the peak B II [110], q II [110], the correction is applied to account absorption increases to 0.31 cm - . should be larger smaller. than that peak This last value is for T = 77 K as opposed to 25 K, so the peak is lower due to the increased linewidth. 25% after for the change in linewidth If a the The PB model predicts that this absorption for B II [001], but it appears, Finally, the peak absorption for B° 11[111], instead to be q II [110] is found to be about 0.1 to 0.15 cm - ', in violation of the warping model selection rules which indicate that this should be zero. Additional data taken at 9.6 gm at 77 K show that the 3Oc(a_) absorption is larger when q II [110] than when q II [11], for B II [110], as predicted. Absorption at 9.6 gm and 25 K shows 3c(al) peak absorption of 0.4 cm - , nicely separated from the 20c+ L absorption. was measured to be about 0.35 cm-1 123 The absorption at 11.6 jim SII11 001 111 112 114 221 110 221 111 112 114 0.25 0.2 0.15 0.1 0.05 0 -0.05 30 60 90 120 150 Angle e (Degrees) A Fig. 3.9 A A F vs. 0 about q = [110]. = [110]; the rotation is right-handed about rl. Zero angle corresponds to A = z, are F3 + F 3 + 0.85F. 1 F = ll(sin36 + 5sin6). 3 64 124 F = /(3sin3O 1 64 Dashed lines - sinG). 180 AII 112 1 1I112 01il 121 110 -60 -30 0 211 101 0.2 0.15 0.1 0.05 0 -0.05 -0.1 -0.15 - -90 30 60 Angle 0 (Degrees) Fig. 3.10 F + F A A vs. 0 about ii= [111]. Zero angle corresponds A = [110] , 4 = [112]; the rotation is right-handed about r. is F 3 + 0.85F.1 3 16 3 3 125 1 16 3 Dashed line 90 AII 001 11001 114 114 112 112 221 111 110 221 111 112 114 0.04 0.02 0 -0.02 -0.04 -0.06 -0.08 30 60 90 120 150 180 Angle 8 (Degrees) Fig. 3.11 A = [110]; F 1 vs. 0 about A Ti = [T10]. Zero angle corresponds to the rotation is right-handed about 126 fj. A A = z F 1 = 64-(3sin30 - sine). AII 112 01i 121 i10 211 i01 0.06 0.04 Im(F) 0.02 0.02 (111) Plane -0.02 -0.04 Re(F) -0.06 -90 -60 0 -30 30 90 60 Angle 8 (Degrees) A F Fig. 3.12 vs. 0 r = [111]. about Zero A A A [110] , angle = [112]; the rotation is right-handed about TI. F F1 = - 16 3 127 i cos3 F . corresponds to II 001 112 114 111 221 110 221 111 112 114 2 1.5 E 0o C 0 L. <0 0.5 0 0 30 60 90 Angle Fig. 3.13 2 120 150 180 e (Degrees) absorption for B° in (110) plane, with q II Ti = [T10]. _oc(1l) A A A Zero angle corresponds to 0 = z, = [110]. A Solid line is for B II z; A dashed line is for B II- z. Circles are experimental data normalized to linewidth at 25 K. 128 A 11112 01i 121 iO -60 -30 0 101 211 1.5 E 1 O O 04- 0 Cn 0.5 -90 -90 60 30 90 Angle 0 (Degrees) A Fig. 3.14 Zero 2c(_1l) absorption for B0 in (111) plane, with q II T11= [111]. angle corresponds to A = [110], B II [110]; dashed line is for B II [110]. 129 A ( = [112]. Solid line is for II 001 114 112 111 221 110 221 111 112 114 0.5 0.4 E 0.3 0 0 Cn 0.2 0.1 0 30 60 90 120 150 180 Angle 8 (Degrees) Fig. 3.15 20c+os(x) Aq q II1T1 = [T10]. absorption for Zero angle corresponds to A A is for B 0 II z; dashed line is for B II-z. 0 130 B0 in = z , (110) = [110]. plane, with Solid line S II 112 01i 121 110 -60 -30 0 101 211 0.5 0.4 E 0.3 0 O 0 ff0 0.2 i 0.1 0-90 90 60 30 Angle 0 (Degrees) Fig. 3.16 A q II Ti = [111]. 2o +c+s(t) absorption for B0 in AZero angle corresponds to (111) Zero angle corresponds to ( = [110] , line is for B II [110]; dashed line is for Bo II [110]. 131 A plane, = [112]. with Solid 4. SPIN-FLIP RAMAN LASER Introduction 4.1 Spin-flip Raman (SFR) scattering in n-InSb is a process in which infrared light scatters inelastically from conduction electrons near k = 0 in InSb in the presence of an applied dc magnetic field, causing the spins of individual electrons to flip. In transition from a lower energy spin-up state to a higher energy spin-down the Stokes scattering process state, gaining the spin-flip energy ho s = RB is the Bohr magneton, and B an electron makes a IBB 0 .g* Here g* is the g-factor, . is the applied magnetic field. The scattered photon loses the amount of energy that the electron gains, so )SR = p--s SR p s where OSR is the scattered Raman Stokes frequency and (p is the pump (or incident) frequency. If the pump is sufficiently intense the scattering process can become stimulated, provided that the end faces of the crystal are polished to form an optical cavity and the temperature is below about 40 K. This can produce significant power conversion from the pump frequency to the Stokes frequency with free carrier concentrations ne in the range 1x1014 cm - 3 to about 5x10 cm - 3 . The device which is based on this process is known as the spin-flip Raman laser, or SFR laser. Features which make spin-flip Raman scattering in n-InSb of interest are the large g-factor and the very large scattering cross resonant when the incident photon energy approaches section which is the band gap energy The effective Hamiltonian for conduction electrons in InSb is E = 0.23 eV. g spherical to lowest (second) order in momentum, and contains terms which are similar to those in the free-electron 133 Hamiltonian, but with modified coefficients. The spherical symmetry of the lowest-order terms is a result of the cubic symmetry (Td point group) of InSb. The effective mass m* is about 0.0136m, where m is the free electron mass, and the g-factor at B° = 0 is about which is 25.5 times larger in magnitude than the free electron -51, g-factor and of opposite sign. term is - (1/4)ag*/laE (Yafet model), which has a value 108 times larger than The coefficient the free electron value of - 1/(4mc2). of the spin-orbit interaction Here, the electron energy E may be measured relative to the bottom of the conduction band or the top of the valence band. the large energies It is the large effective spin-orbit interaction which produces SFR cross section which band-valence are band The resonance. a for conduction significant approach resulting fraction must cross electrons. be of used section is E , to At incident photon a coupled properly significantly account larger conduction for the than the Thomson cross section for elastic scattering from free electrons, exceeding it by factors of the order of (m/m*) 2 , or (g*)2 , times [EgaOp/(E-2 h 2- )]2 The 2000 over the Thomson cross first factor section. gives an enhancement of about The second factor, which is resonant at E , is about 4/9 for 10.6 jLm CO 2 laser radiation with photon energy equal to half the band gap, but becomes very large for wavelengths near 5.3 gm. In the above approximation the cross section is independent of B 0, and is finite at B ° = 0. For magnetic fields of 1 T or more the nonparabolicity of the bands and the variation of the energy gap with B cause the low-field formula to become inaccurate, so that more detailed calculations based on the coupled-band model are required. Enhanced electronic Raman scattering from conduction electrons in InSb in a magnetic field was predicted by [Wolff 66]. band models by [Yafet 66] and [Kelley 66] 134 Calculations based on coupled indicated that spin-flip Raman scattering with no change of the orbital quantum number (An=0) should be the most important of the various inter-Landau level and spin-flip scattering processes. Spontaneous SFR scattering of 10.6 gm radiation from electrons in n-InSb was reported by [Slusher 67], and stimulated SFR scattering was first reported by [Patel 70]. SFR scattering from bound electrons and holes in CdS, which is a wide-gap hexagonal material, was observed by [Thomas 68]. theory in this case is different from that for InSb due to the The lower point-group symmetry and the need to consider both bound and excitonic states of electrons and holes. cw operation of an InSb SFR laser was first obtained by [Mooradian 70], using a CO pump laser operating at 5.32 jim, and high-power operation of an SFR laser using a TEA-CO 2 pump laser at 10.6 gm was obtained Since 1970 SFR scattering has been observed and studied in by [Aggarwal 71]. many semiconductors, including narrow-gap and wide-gap, cubic and hexagonal, nonmagnetic exist, and magnetic including ones materials. by Excellent [Dennis 72], reviews of SFR [Scott 75, 76, 80], [Wolff 76 & 77], [Smith 77], [Geschwind 84] and [Hdfele 91]. scattering [Colles 75], SFR scattering in dilute magnetic semiconductors (DMS) is reviewed by [Ramdas 88], and is also covered in [Hifele 91] and in a recent review of laser spectroscopy in high magnetic fields by [Heiman 92]. The purpose of the experimental work was to study effects influencing the operation of the InSb SFR laser at magnetic fields up to 18 T. This was the highest field which was readily attainable in a 2-inch bore Bitter magnet at the time the work was conducted. there was interest in Particular interest centered processes Previous studies had ended below 11 T, and which could occur at on the magnetic field region near higher 12.5 T where h0o s becomes equal to the zone-center LO-phonon energy hOLO= 24.6 meV. 135 fields. This implies the possibility of increased spin relaxation due to emission phonons, and polaron pinning effects similar to those observed cyclotron resonance energy hwc becomes equal to hCoLO. studies a frequency-doubled of LO when the For these high-field TEA-CO 2 laser producing radiation in the 4.8 to 5.4 gm region was chosen as the pump. This choice took advantage of the resonant enhancement in the scattering cross section which occurs when hCo is P near to Eg , and also avoided the free-carrier absorption which becomes large at fields above 10 T for 10 im pumping. I made a detailed study of the operation of the 10 jm-pumped SFR laser at fields up to 13 T, in addition to the high-field operation of the 5 jm-pumped SFR laser. Emphasis magnetoabsorption harmonics, orientation along at was placed on cyclotron-resonance with the similar the (CR) effect of harmonics LO-phonon-assisted linear and free-carrier spin-flip transitions. CR The dependence in the applied field (anisotropy) and pump-wavelength dependence of these transitions was studied in detail. 136 4.2 Theory of Inter-Landau Level Light Scattering In this I section discuss theory the of level inter-Landau light scattering from free carriers in InSb for comparison with my experiments on stimulated spin-flip (SFR) Raman scattering. 2o s, transition at 2 0 c+s and finite k . discuss and origin the and present numerical results for approximations for the cross section do/dI, the I Raman scattering transitions at k = 0, and the o c The 20c and 2 c+'Os transitions, although not observed in the stimulated SFR experiments, are important because of their connection with the magnetic field-reversal effect in magnetoabsorption The numerical calculations for these two cases is discussed in Chapter 3. correct results given which by Wright et al. [Wright 68]. Small effects which result from anisotropy will be reviewed and discussed. Two treatments of the cross section do/dQ are considered: the decoupled model, and the axial 8x8 Pidgeon and Brown model. expressions which are valid at low fields. the selection The first employs analytic It provides a good description of rules in the axial approximation, and the lifting of the sel- ection rules, due to warping and inversion asymmetry, for arbitrary values of The second treatment obtains numerical results for the momentum k along B . scattering in the axial electrons, from conduction approximation, which are accurate for arbitrary values of magnetic field B and incident frequency o 1. For the purpose of scattering, the free carriers in InSb are regarded as free strong elementary spin-orbit particles with interaction. effective small The spin-orbit mass, large interactions g-factor, result from and the multiband nature of the infinite Luttinger-Kohn or 8x8 Pidgeon and Brown 137 Hamiltonian, just as the atomic spin-orbit two-band nature of the Dirac Hamiltonian. understood interaction which Luttinger-Kohn are (LK) approximation obtained from transformation (EMA) results the the discrete coupled [Luttinger 55]. from the lowest-order utilizes decoupled Hamiltonians to order k2 . approximations, kinetic energy nature of the lattice representation of the free the and valence band Hamiltonian The via effective the mass LK transformation, and In this, and higher finite-order associated with the point group symmetry remains. the from These interactions are most easily in the framework of the decoupled conduction Hamiltonians in results carriers, disappears, but anisotropy The anisotropy is present in contrast with the atomic where the anisotropy is present in the potential energy of the lattice, V(r). Some general properties of inter-LL Raman scattering are listed below. The strongest scattering is electric dipole (ED) in nature, and the associated electronic transitions conserve parity at k = 0. Magneto-optical effects resulting from cubic anisotropy tend to be small, with a few exceptions where heavy holes act as initial or final states. The strongest transitions occur in the axial approximation, in which the quantum number n+m is conserved, where n is the Landau level number and m is the "effective" angular momentum of the LK basis state along B0 . The actual point group symmetry is the intersection of the tetrahedral point-group Td with the axial symmetry group Cooh, which contains only the identity element for a general direction of B0 [Rashba 61a, Trebin 79]. In spite of this, the axial approximation good for the conduction and light-hole bands in InSb near k = 0. dipole nature of the inter-LL scattering causes the intensity is very The electric pattern of the scattered radiation to be the same as that produced by an oscillating electric 138 dipole [Yafet 66, Romestain 74]. This applies to both the magnetic scattering caused by the spin of the scatterer, and the charge scattering caused by the charge. light The dependence of the scattering on the polarization of the incident has occurs electric via virtual dipole character interband also. electric This dipole is because transitions in the the scattering coupled-band approximation. 4.2.1 Scattering Cross Section The scattering cross section is given by d/dl 2, = (e2/mc 2 )2(o 2 /1)IAfo (4.1) where e2/mc 2 is the classical electron radius, 2.82x10 the incident and scattered frequencies, and A perturbation theory via the Golden-Rule. the effects associated with the InSb band involving the refractive indices, 3 cm, o and w2 are is an amplitude computed from This latter quantity structure. contains An additional (n2/n 1 2, must be included if nl n 2 . all factor If the cross-section is computed as a ratio of energy fluxes rather than photon fluxes, one must replace (n2/n 1 )2(o2/) In the infinite by (n2/n)(2/31) 2. coupled-band Luttinger-Kohn representation at k=O [Luttinger 55] and the 8x8 PB model, the scattering amplitude A A forOt- in the ED approximation is given by the expression A f I ro E A A I fr hO - E fr (4.2) +[(e V)(e V )H 139 A A Here e and e 2 are the complex unit polarization vectors of the incident and scattered level radiation; o, f wave functions; A where first-order initial, final and intermediate in the infinite LK It is A (e*.e )fo in the free electron the intermediate It the vV kHeff is the velocity operator it only contributes A-v. r label The last term results from terms of order k2 in Hff. representation. replaced by and states has to elastic scattering. The first term, involving Ir>, results from second-order perturbation resonances optical case and the infinite LK case, transitions. when the incident In the large-field, radiation theory in excites allowed low-temperature (extreme quantum limit) approximation, the sum over intermediate states is carried out as in the intermediate one-electron and final problem, states valence band intermediate virtual with Ir> and initial state If> unoccupied lo> occupied and [Wherrett 69]. For states, the many-electron viewpoint requires that a transition from r to the final state f in the conduction band (cb) precede the relaxation of the cb state o to the hole r created in the vb by the first transition. 4.2.2 (See [Dennis 72].) Scattering in the Decoupled Representation This approximation functions, and an uses decoupled effective conduction scattering amplitude between these wave functions. and valence operator band wave which acts on or The amplitude operator A seat is obtained as a power series in the kinetic momentum operator k, and is useful when B and kz are sufficiently small. both the cases description lifting This approach has the advantages that it works for of finite k of the selection of the selection and finite rules rules, to anisotropy, and provides for the axial approximation, lowest 140 order in k, for the a simple and of the anisotropic The disadvantages are that the approximation is valid only for very low case. fields if the incident photon energy is close to the band-gap energy Eg, and that the coefficients of the k-dependent terms can be quite complicated. In the low-B limit the scattering amplitude A the matrix element of a matrix operator A decoupled wave functions. may be approximated by between two- or four-component Thus [see Wolff 75] A = <f olAs tlo >, 0 scat 0 fo where Ifo> and o0> are the component wave functions If> and the simplest representation of the (4.3) decoupled Io>. representations of the infinite- The decoupled wave functions provide actual multiband wave functions. The latter can be derived from the decoupled wave functions by inverting the LK transformation. The operator A scat is obtained as a power series in k. lowest order is ko which gives elastic and spin-flip scattering. The The result in this order is quite simple, but the result to order k 2 contains many terms, and is rather difficult to obtain even in the Yafet approximation. In this order the scattering can cause a change in the orbital state as well as the spin of the scatterer. Both orders show resonances corresponding to the interband energies Eg and E +A. at frequencies One of the terms in order k 2, associated with Faraday rotation, shows an additional resonance when o= 0. I have used operator techniques to valence, and split-off to valence band cases. Ac , A and A . obtain A scat for the conduction, These operators will be denoted The derivation to order ko (or unity) is quite simple. result for A c is 141 The 2 2P2 A= (1+2F) + - 1 - 3m 9 (0) + - I E (4.4) G* E" g 2P - ih(a) 2 1 the derivation c0) E 3m where 1 .- is Xe 2-) 2 - 2' 2 2( ) on the invariant , 1 2 g based expansion of the PB Hamiltonian, and makes use of some matrix algebra given in Appendix A. Notice that the summation over intermediate states has been replaced by a sum over bands [see Braun 85]. Here 1+2F is the contribution from the free electron mass and from higher p-like conduction bands, P is the valence to conduction band momentum matrix element, E is the valence to conduction band energy gap. A e A and scattered e2 are the radiation, complex co is the unit polarization frequency vectors of the of the incident incident and radiation (actually (01), E' E +A , g (4.5) and E'2 E2 E_2 E g - p(o h22 My definition of the resonant function ,2 E'2 p,2(0o) 2 h2 2 (4.6) is larger than that of Makarov [Makarov 68] by a factor (E'IE )2. My choice causes both (p2 and (pl to equal 1 when 0)=O. 142 The following are important points for the isotropic model: * The first term in A c (Eq. 4.4) causes elastic scattering. causes spin-flip approximation scattering and Faraday is independent of B . rotation. The The second term Notice that spin-flip Ac in this scattering is elastic if B = 0, and inelastic (Raman) if Bo# 0. * The first term in A c may be regarded as scattering from the charge of the electron (charge scattering), and the second term as scattering from the spin (magnetic scattering). scattering amplitude In is this small-B0 antisymmetric with A approximation, respect A to A scattered polarization light of must have the a component light. incident that Notice, magnetic interchange of the A polarization vectors e1 and e 2, i.e. proportional to e xe*. the the This means that is perpendicular that the to the scattering is independent of the optical wavevectors, and is therefore electric dipole (ED) in nature, for both the charge scattering and the magnetic scattering [Yafet 66; see also Romestain 74]. * Notice this also the conservation of parity for the state of the A one-photon approximation. scatterer in ED transition changes the parity, so a two-photon ED transition conserves parity. * My expression for Ac omits resonance effects associated with higher conduction bands, since these resonances are at energies large compared with It also omits contributions of higher bands to the magnetic scattering, E . g since the 1/E2 dependence of the coefficients make these terms small for InSb. * My expression for the resonant coefficient of the magnetic term, obtained from the 8x8 PB model, is an improvement on the one obtained by Wolff. 143 The latter was obtained from a 2-band model, with inclusion of the "free-spin" part of the 2-band Hamiltonian [Brown 72, Wolff 75]. The more accurate result, consistent with the PB model, is obtained by replacing (1/2)(1/m s - 1/m)(Pl/E ) = - (P2/3)(I /Eg)(1/Eg - lIE') 1 in Wolff's expression for the "Raman Hamiltonian" (where m/m s - g*/2) by 2/E'2 - (P2/3)(9 /E2 In the low frequency limit the first quantity approaches (1/E )(g*/2 - 1), while the second approaches K = (1/E + 1/E')(g*12 - 2N - 1). For InSb the S g 1 three-band expression is larger than Wolff's expression by 23% at 0=-0, and by 29% when ho=E . Furthermore, the three-band expression makes it clear that g the scattering is associated with the effective spin-orbit term in the decoupled cb Hamiltonian, proportional to eK s , instead of the effective Zeeman term, proportional to gtBg*. above quantities, The SFR cross section involves the squares of the so the three-band formula gives cross sections which are larger by 50% to 67% as the incident frequency ao varies from 0 to E /h. I g In the limit o 0, the coefficients in A c simplify so that - M AA A C = -(e -e* 1 + 2iht M 1 2) G A A 4). KS(e 1xe*.-) , 2 (4.7) where m 2P2 1 2 - 1+2F + + m* 3m E g (4.8) E' is the reciprocal conduction band effective mass at k=0, and K S Pl 3m 3m 1 1 E E2 E (4.9) g 144 is the coefficient of the effective spin-orbit interaction for the decoupled conduction band [Yafet 63, Rashba 91, Jusserand 95]. To order k2 for conduction electrons, transitions become allowed in which the Landau level index changes. If we consider only order k 2 we find occurs to order ko.) A C (Only spin-flip Raman scattering, with An=0, = (a)(e "e*)k + i(b)(e xe*)'Bo + (c)(e 1 A A 1 2 k2 i(e)(e xe*) .k2 - * 2 0 12 )(2 )-( A + (d)(e AA 1 2 (Bo 0 ( 2) (f(elxe*) -{k, k a} + (g)(e e*)().( (4.10) The coefficients (a) through (g) have been derived from the Yafet model and are given in Appendix H. contain the parameters, and expressions result, and APi..j , and effectively, are therefore The expressions resonance from quite 4th are functions order functions 9 ( w) and perturbation complicated [Yafet 63]. of the band 9(2(o). theory The The in k.Pi Raman transitions obtained in this order by expressing A c in spherical components are summarized in Table 4.1. 145 Table 4.1 Electronic transitions in Landau level Raman scattering from conduction electrons for finite B in the axial approximation, in order k 2 and Here n is the integer Landau level quantum number and s=+11/2 is the higher. The coefficients are from Eq. (4.10). spin quantum number. Transition Operator A 0 sS Coefficient A k2 - i(elxe*) 1 2+ A 0c - a s C 30 Here, (z,+), (-,z) (z,+), (-,z) (g) (z,+), (-,z) Order k4 & higher --- 1 1 (+,-) (c) 1 0 (z,-), (+,z) A A c -1 (f) - ii(e 1xe*) k k yZ 2-+Z 2 0 A A 2t Polarization (e) e*) ( 2)k k S As - ii(e 1xe*) k k_ 2+-+ (e e(2)(Y' _B S(e C An (f) A kk - i(exe*) 1 2Z Z+ (f) Order k4 & higher --- 2 (e e*)(2)k 2 -2 + 1 C (z,-), (+,z) -1 1 (+,+), (-,-) (z,z) (c) 2 0 (+,-) + 03s - i(exe*) k2 (f) 2 - 1 (z,-), (+,z) + o Order k4 & higher --- 3 -1 (+,-) S 2- 1 +- o s is the "spin-flip frequency" Nonparabolicity and oc is the "cyclotron frequency." effects cause both to depend on the Landau level index n. Note that At=An+As varies from - 1 to 2, for these energy-absorbing electronic processes, where t-n+ms 2 is the quantum number which is rigorously conserved in the axial approximation. (z,z) polarization, important in conservation approximation, requires Note that the c+os transition also occurs in the order k4 , but this is not law for the axial shown model, that At for the electronic in the transition the total change in the photon angular momentum alongt:) B 0 . Z:) t") 146 in the table. electric exactly An dipole opposes Only the terms proportional to (c) and (f) produce inter-LL transitions with An O. (c) is associated with nonparabolicity spin-orbit interaction (or A) is zero. and is finite when the It causes the 2 c Raman transition at k = 0, and the coc Raman transition at k 0. (f) is finite only if A is z c z finite. It causes the 2o + s Raman transition at k = 0, and the oc+s Raman transition at k # 0. It also contributes to the oa Raman transition at k # 0. z c z The term proportional to (g) gives a contribution to SFR scattering which is A symmetric in amplitudes A e to and e2. differ for A A This B0>0, causes since the the (z,+) and scattering at (-,z) scattering B0=0 is purely antisymmetric in e1 and e . 2 As an example of computation of the polarization selection rules, note that A A i(elxe*) S2+ =(e e * 2 1Z 2- e*) 1+ 2Z associated with the ws Raman (SFR) transition, is maximized in magnitude when AA the incident and scattered have photons polarizations A abbreviated (z,+) and (-,z). (z,e ) A or A (e_,z), A (Note that e2 = V2 when e2 = e.) Quantitative Estimate of Anisotropic Scattering When one goes beyond the isotropic approximation one finds three new effects: dependent The (1) on isotropic crystal model orientation. transitions listed (2) k -induced The in Table 4.1 transitions become of the isotropic approximation become allowed at k =0 due to inversion asymmetry. (3) The axial model selection rules are lifted. These effects are small for the case of inter-LL scattering by conduction electrons. 147 The orientation the isotropic model dependence of scattering cross sections which is found by considering the axial terms (Oh symmetry) in the effective Hamiltonian. angular function W defined in Appendix C. occur in part of the warping These terms involve the The magnitude of the anisotropy of SFR scattering in the low-field limit is of the order of (y70 s/oK), which is 8% at B = 5 T and zero at B = 0. 0 0 Inversion asymmetry causes finite-k transitions of the isotropic model to become allowed at k =0. For the An=1 scattering transition the magnitude z of this effect at k =0 relative to k -is of the order (8/v3)2 , which is 1% at B = 5 T. The axial and nonaxial parts associated with inversion asymmetry are of similar magnitudes. The scattering nonaxial part transitions, of inversion and asymmetry new polarizations and for the warping causes old transitions. new This may be dealt with by an adaptation of the approach used by Rashba and Sheka, Gopalan et al., and La Rocca et al. for the case [Rashba 61, Gopalan 85, La Rocca 88a,b]. of inter-LL absorption Details are given in Appendix H. The new warping-induced scattering transitions have An=even at k =0, and are weaker than the axially-allowed An=2 (aE0)2=0.004 or ( 0/E )2=0.04. The transition new by inversion factors of order asymmetry-induced transitions have odd An at k =0, and are weaker than the axial transitions by a factor of order 0.01 at B =5 T. Quantitative Estimate of Isotropic Scattering Quantitative estimates of the cross 148 section for the various inter-LL Raman are transitions representation. easily obtained in the completely decoupled The SFR scattering process is the only Raman process which occurs to zero order in k, and is finite for Bo-- 0. For this case there are two enhancements over the Thompson cross section for light scattering from a free electron. (or average) effective The first enhancement is the factor hoK which is the incident s photon spin-orbit energy times interaction in the band parameter effective the mass associated with approximation. the For hO) = E /2 (10.6 pm wavelength) this factor has a dimensionless value of 7.8, g which is squared in computing the cross section. The second factor comes from the presence of the resonant denominators and may be expressed as Ks(o)/Ks(0), s s where K(w) is an o-dependent expression which evaluates to K for co=0. The value of this second factor for h0 = E /2 is 4.15. The overall enhancement of g the cross section relative to the Thompson cross section then is about 1000. This factor becomes much larger when he approaches the resonance at E , as will be seen in the next section. For the An=2 scattering transition the k2 dependence near k=0 causes the coefficient to be more complicated than the one for SFR. (away from resonance) the relevant factor is E k 2 or When o is small Eos , where e0 is the coefficient of the k4 term in the decoupled cb Hamiltonian, and s=-eB 0 /hc is the reciprocal of the Landau radius squared. The obtained from the Yafet model, is = (1/8)d(m/ m *)2/ dE = ( 1/4)(m/m*) 2(1/E ). If we evaluate s at B0=10 T and convert it to an energy using h2s/m = 2. B o we obtain a dimensionless factor 149 expression for Eo, 0 s - (1/4)(m/m*) 2 (2p BBIE ) 6.0 , where we used m/m* = 70, 2g B° = 1.15 meV, and E = 235 meV. This factor becomes 36 when squared for the scattering cross section. The coefficient for the An=1 the one for An=2 if we set k =1/e =1/v, z at k 0 is close to z is the Landau radius. This scattering transition c where t neglects the contribution of the coefficient c (f) relative to (c) in Eq. 4.10. Note that <k> is of the order of l/~ in the experiment of Slusher et al. z [Slusher 67]. 4.2.3 Scattering in the Pidgeon and Brown Model This approach uses the 8x8 axial coupled-band model of Pidgeon and Brown [Pidgeon 66, 68, Weiler 78]]. This model is accurate for light scattering by conduction electrons in InSb for arbitrary values of the magnetic field B0 and arbitrary frequencies o) of the incident light. It takes account of the axial component of the warping anisotropy and can be modified to include the axial component of the inversion asymmetry anisotropy. anisotropy requires diagonalization of much larger Treatment of the nonaxial matrices, as has been discussed by Evtuhov for the case of the 4-fold degenerate valence band in germanium, and by Trebin and by Pfeffer for the more complicated cases of InSb and GaAs [Evtuhov 62, Bell 66, Trebin 79, Pfeffer 90.] Wave functions in the PB model have the multicomponent form fi(r)}, where the index i is the label associated with the eight Luttinger-Kohn (LK) basis functions for the s and p-like conduction and valence bands of InSb at k=0. The Hamiltonian is an 8x8 operator matrix, where 'operator' implies that 150 the matrix elements contain the kinetic momentum operator k-p+ecA, in addition to perturbing of the Construction invariants" potentials which and fields Hamiltonian may [Luttinger 56, Bir 74, Trebin 79] tensor techniques by use is facilitated of r be functions along of the with and t. "method of irreducible spherical [Baldereschi 73, 74] and numeric computation software, such as Matlab [Mathworks 89], capable of matrix operations. (See [Favrot 94] for a brief description of the application of irreducible spherical tensor methods to the PB model.) Matrix algebra can be used along with the method of invariants simplify the to greatly particularly to third computations of k-p perturbation order in k and the applied and fourth theory, fields. See Appendix A. is In the invariant formulation, Heff is broken into blocks, and each block expanded via products of basis matrices times operators containing components of k or B. We then have [Trebin 79, R6ssler 84] Hcc cc HcCV HsCS Heff (4.11) Hvc Hvv Hvs where hermiticity implies that H VC =H , CV H SC H =H t =H t SV = Cs' VS The invariant formulation of the blocks is given in Appendix A. In the axial approximation, the Landau level wave functions have the form W = exp(ik y)exp(ikzz)[ct c2tq +1 C3 (Pt 1 (4. 12) C6 (p 151 C5 (P+ 1 C4 (P+2 IC8 ( C7 (P+1 It where the transpose symbol 't' is used to indicate that the wave function is actually a column vector, and the vertical bars are used to visually separate the components associated with basis functions for the F band (cb), F (=3 ) valence band (vb) and F (=1) 8 2 7 2 (j=i) conduction split-off band. The labels of the coefficients refer to the PB basis functions ui(r), and the ordering is by decreasing mj within each band. From the form of the wave function one finds that n+m is conserved, where n is the index of the Landau level wave function, and mj is the component of "effective" angular momentum of the LK (or PB) basis function "effective" in quotes angular momentum, in the direction because of the magnetic the basis states are not but transform like the corresponding field B0 . true I use eigenstates atomic states of with respect to the restricted set of rotations contained in the Td point group. I will refer to the quantity = n+mJ (4.13) 2 as the axial quantum number, which is conserved rigorously in the axial model. It is related to Luttinger's constant of motion Q for the case of germanium, and to Rashba's "angular quasimomentum," n+m . Suzuki 74, Bir 74, A operator (N Trebin 79, Rashba 91.] [See Luttinger 56, Yafet 73, It is the eigenvalue of the A -)1 + F [Trebin 79], where N is the Landau level number operator 1 is the unit 8x8 matrix, and F is the 8x8 F z generalization of the angular momentum matrices s and J WhnZ Z for free spinless electrons, F When Heff operates in an 8-dimensional subspace of fixed e it is replaced by a purely numerical matrix [Yafet 66, Pidgeon 66, Weiler 78, Jimenez 94]. (The basis n+m - = e, functions for this subspace are the functions <pn(r)ui, with where u. is best regarded as a 8-component column vector with a 152 single unit element in the location corresponding to the basis function ui(r), and zeros elsewhere.) The representation of the wave function in this subspace is the column vector of the coefficients [cc 1cc c 1 C22 1 C3 C6 C 5 The representation c]t. C4 1IcC8 C7 (4.14) of Hff is obtained by moving all k i operators to the right, and replacing them by their -dependent numerical representations k = V2 diag[~T1k = v2- diag[b/ T-+ V/a VT VT v V +2 v/m VT'2 VTT rt+3 1 vti 2] it eTl-] (4.15) (independent of ) k = k 1 A 2sN = k+ k- = 2s diag[ +le-+11e e+l t+2 e t+1] etc., where s eB /hc is the magnetic wavevector squared (k2 ), and the reciprocal squared (t-2), and 'diag[-]' diagonal elements. operations require Note denotes that k the diagonal matrix with the enclosed and k attention to the changing raise t by value of e. with the spherical tensor form Xm raise (or lower) e by m. Diagonalizing energies Ei and the matrix eight sets magnetic length representation of coefficients +1, so Matrix sequential operators (See Appendix C.) for Hff generally yields eight eigenvectors). Exceptions (or occur for the three lowest values of t given below. I use the notation of [Luttinger 56], [Pidgeon 66] and [Weiler 78]: e=-2: b+(0) e=-1: (4.16) bc(O), b+(1), a+(O), aS(O) 153 f=0: bC(1), aC(O), b-(2), b+(2), a+(1), aS(1), bs(O) = 1: bC(2), aC(1), b-(3), a-(2), b+(3), a+(2), aS(2), bS(1) etc. The conduction and split-off bands (cb and sb) are both spin-- like, but their LK basis states have opposite parities. For the cb, the a-set designation implies a large ms=+! component near kZ=0; for the sb the a-set designation i l2 implies a large ms=- component near k =0. largest component of the wave function. band edge. The band-edge The index n is the index of the It is 0 for the level nearest to the levels at finite field are aC(O) and aS(0); the bc(0) and bs(O) levels both lie within the respective bands. The Luttinger notation for the light hole and heavy holes is more complicated. The a-set Landau levels in the decoupled (j= ) representation have two finite components For the a-set levels the index is that of the m=-- at k =0 instead of one. z J 2 component function, and for the b-set the index is that of the m function. The light hole effective mass and g-factor. a+(1) nearest (lh) Landau levels have a fairly component well-defined The initial lh levels are a+(1) and b+(1), with to the band edge. The '+' superscript denotes 'light hole' except for the levels a (0) and b+(0) which are heavy hole levels, along with the a-(n) and b-(n) levels which are defined for n>2. The heavy hole Landau levels have effective mass and g-factor which are well-defined only at large n, due to interactions known as the Luttinger effect. contained in the 4x4 decoupled representation. diagonalization of the depends on the effective Hamiltonian in the The heavy hole Landau levels nearest to the band edge are a+(0), b+(0), a-(2) and b-(2). energy These interactions are values of the orientation of the magnetic field B0 . 0 154 The ordering of these four levels in Luttinger parameters, and on the The calculation of matrix elements of the velocity operator between LL which wave functions requires the 8x8 matrix representations of v+, v_ and v, depend on the f value of the wave function (or subspace) which is acted upon. The 8x8 components of the velocity operator are found from v = 2aH/ak , v v = 2aHlak , (These are the spherical components of v in the 471( , with v+-v +ivl.) directed along (4.17) = aH/ak . coordinate frame with B In the matrix representations of these A operators, one again moves factors of k , k and N to the right before making the matrix substitutions given in Eqs.(4.15). Note that v raises the axial quantum number e by one unit, v_ lowers e by one unit, and v unchanged. leaves Z Thus the eigenvector of coefficients on the left-hand side of v has an t value which is larger by one than the eigenvector to the right of v. To compute Afo for SFR scattering we must consider the processes in Eq.(4.2) which have aC(O) and bc(O) as initial and final states, and therefore At=- 1. These are v (a) aC(0) v (t=0 intermed.) - (t=O) bc(0) - (R=O) (=- 1) v v (b) aC(0) (t=-1 intermed.) (e=0) bc(0) (e=-1) (t=-1) and V VH k+ (c) kz eff aC(O) > bc(O) (t=o) (=- 1) 155 . The last process proceeds without an intermediate state in the PB model. means that the actual intermediate bands treated explicitly "spin-conserving", produces only i.e. in the state is outside the PB a-to-a or a-to-b and model. b-to-b b-to-a Note that transitions, transitions at 8-dimensional at v set of produces k =0; k =0. This and The that number only v of intermediate states is therefore fewer at k =0. A For Eq.(4.2) second (z,+) scattering, contains only sum contains with the only A A e =z E=0 and A intermediate the t=-1 A e =(x+iy)/v', states intermediate the (process states first sum in (a)) and the (process(b)). The resonances for (z,+) scattering are caused by the following absorptions: v v -2 aC(0) bC(1), V a+(0)~- bc(0) , and a(0) ~ The second resonance occurs at energy ho =E +Ih(O +OWs) I the low-field limit. g2 C bc(O) . in the Yafet model, in S This resonance cannot be reached, however, due to the resonant interband absorption v aC(0), b (2)- which occurs at energy ho I=Eg2+Ih(O-Os). C A For Eq.(4.2) second (-,z) scattering, contains only sum contains with the only S A A e =(x-iy)/2 t=-1 intermediate i=0 the A and states intermediate A e2 =z, the first sum in (process (b)) and the states (process(a)). resonances for (-,z) scattering are caused by the following absorptions: V b (2) -- v bc() , b+(2) - v bc(O) , 156 and bs(O) - bc(O) The The first resonance occurs at energy ho I=Eg2+h( C +0 ) in the Yafet model, in S the low-field limit. It is blocked by the resonant interband absorption V aC(O), a-(2) at energy h) =E +!h() -0). g2 I S C The resonances associated with the split-off band are blocked by strong interband absorption that occurs when h0lI >Eg2+h(w C-0).S The conduction band resonance at energy h0 =h(Oc+ms) for (z,+) causes the cross section section for for (-,z). this polarization (EII B0) to be larger than the cross Observation of this resonance, however, is prevented by light, and increasing of the scattered CR absorption the strong free-carrier combined resonance absorption at h(O c+(0s) of the incident radiation. See the discussion of [Dennis 72]. The 2o c and 2 0oc+o)s The 20 fashion to the spin-flip. (+,-) polarization. The 2 (oc+o)s and (+,z) polarizations. B =0, Raman scattering amplitudes are computed in a similar c process has At=2, and is maximum for the process has Ae=1, and is maximum for the (z,-) The cross sections for these processes are zero at and increase in proportion to B2 at small fields [Yafet 66, Kelley 66, Makarov 68, Wright 68]. The cyclotron resonance (coc) amplitude is zero at k =0, but is comparable to the 2 when kz=k =(tB)'. c Raman scattering scattering amplitude This scattering process was observed by Slusher et al. [Slusher 67] for conditions in which several Landau levels were occupied, and was explained by Makarov [Makarov 68]. 157 Numerical Results The weight factor |Af k =0 is presented 12 for the cs, 20c and in Figs. 4.1 and 4.2. 2 0c+0 Raman transitions at The first figure is for 10.6 gtm incident radiation at approximately half the band-gap energy, and the second is for near-resonant 5.3 gtm radiation. band parameters of [Littler 83]. The PB model calculations use the InSb They show the anisotropy which occurs in the axial model due to the warping parameter i. The dashed curve in the figures shows the spherical average which results when g. is set equal to zero. curve furthest remaining away from curves the average correspond opposite side of the average. corresponds to Bo [001]. to BII [110] and [111], moving away The The two on the Figure 4.3 shows the weight factor for the Oc and 20 Raman transitions as a function of k at B =50 kG. C Z 0 158 12 10 8 6 4 2 0 0 200 160 120 80 C E Cu 40 0 1000 800 600 400 200 0 0 20 40 60 80 100 120 140 160 180 Magnetic Field (kG) Fig. 4.1 Calculation of Raman weight Afo 12 versus magnetic field for 10.6 gm incident wavelength for three transitions at k z=0. 159 1004 1003 1002 1001 CJ 10o00 1004 0 1003 10o E 1002 10 06 1005 10os 1004 1003 0 25 50 75 100 125 150 175 200 Magnetic Field (kG) Fig. 4.2 Calculation of Raman weight IAf 12 versus magnetic field for 5.3 Lm incident wavelength for three transitions at k =-0. z 160 14- 2O(+-) a - (+,z) a c(z, a 12 -- 2mc(+,-) b -10 "o 8 6 (a(z,-) b 4 2 0 0 0.2 0.1 0.3 0.5 0.4 0.6 0.7 0.8 0.9 1 k z /'2 Fit. 4.3 Calculation of Raman amplitude up transitions 'a' and Af'b' versus kz for spin-down transitions incident radiation, where s-eB O/hc. 161 'b' c and 2 at B =50 kG for c spin- 10.6 Am Comments for Fig. 4.1, 10.6 gtm: * The SFR weight factor for (z,+) is larger than that for (-,z) because it has This resonance is associated with the a resonance at high fields [Dennis 72]. bC(1) intermediate state, which is nonresonant for (-,z). at the origin intermediate is due to the trail-off The states. weight The downward slope from resonance factor B 11[111] than for the other orientations. for (z,+) is with valence slightly band for larger It has a minimum near 90 kG, and then increases towards a resonance beyond 180 kG. The (-,z) weight decreases monotonically, and never reaches zero in either the PB or Yafet model. (The (z,+) amplitude crosses zero, in the Yafet model, when Os=o I and 02=0.) * The weight factor for 2 c (+,-) is zero at B =0, and increases as B2 reaches a peak near 45 kG where its square is about 1/3 that of SFR. It It goes to zero at B =115 kG, which is very near to the point where 2c =0 and o 2=0. The curve beyond this point absorption with (+,+) polarization. represents the weight factor for 2-photon (Note: If the Yafet model is used, the amplitude goes through zero at exactly the field at which 2oc = and 02=0. It is not known if this condition would occur in theories which go beyond the PB model.) Wright's prediction of a finite amplitude for the (z,z) polarization is an error, and violates the axial model selection rule of conservation of the total angular momentum component (photon plus electron) along B . If nonaxial the 2 0co scattering is considered, the weight factor for (z,z) scattering with transition is much smaller than that computed by Wright. * The weight factor for 2 0c+ s (z,-) reaches a maximum at 32 kG, and is larger than that of (+,z) which is maximum at 21 kG. factor is about 1/20 that of 2o c . The peak for the (z,-) weight This is in agreement with the prediction of 162 The amplitudes go to zero Makarov, but differs from that of Wright et al. near 100 kG, where 2oc+os0 = Wright et al. and o2=0, in disagreement with the prediction of (This is again exact in the Yafet model.) of finite amplitudes Wright's predictions for the (z,+) and (-,z) polarizations are also in error, in violation of the axial model selection rules. * The Yafet model calculations (not shown) differ from the dashed curves by amounts which are similar to the amounts for the solid curves. The present curves differ from the Yafet result by at most 5% in the region shown, which is about the same as the magnitude of the anisotropy. The SFR weight factors for the Yafet and PB models are the same at B =0. Comments for Fig. 4.2, 5.3 m: * The incident photon energy used in this figure is 232 meV. This is only 3.2 meV lower than the zero field energy gap between the cb and vb. (For hio >E the resonant condition for the scattering amplitude occurs at some ig finite field.) The Raman weight factor now peaks very sharply near the origin for all three graphs. A logarithmic scale is used on the y-axis to show the large variation. * The weight factor for SFR scattering at the origin is about 2 orders of magnitude larger than the peak values for the 2 the origin. c and 2 wc+os transitions near At 10 T the SFR weight factor is about 15 times larger than the 2o c weight, and the latter is about 5 times larger than the larger of the 20c+s weights. * Notice that the weights for the 20o and 2 +o s scattering transitions are of comparable size near the peak, with 2oc+o2 s now being slightly stronger than 163 2o c . At larger fields the strength of 20c+o) s decreases more rapidly, so 2o c becomes the stronger one, as at 10.6 gm. Notice the different scales used for 20 and 2o +o . c c S Comments for Fig. 4.3 - k dependence at 10.6 gtm: * The weight factors for the 0c and 20 functions of k out to kH-(eB /hc)1 /2 , for B 0=50 kG. the magnetic length the Fermi level Raman transitions are plotted as e kH is the reciprocal of , and is the approximate cutoff for occupied states when drops just below the n=l spin up Landau attainment of the quantum limit. level, i.e. on (The extreme quantum limit is attained when the Fermi energy drops below the n=0 spin down Landau level.) * The weight factor for cc scattering is zero at k =0. increases quadratically. At small B and 0 k z the c c For small k it scattering transitions result from the coefficients (c) and (f) in the decoupled scattering amplitude operator, which cause the 2o) and 20c+ s transitions, respectively. * Near kz=kH the weight factors for oc scattering are comparable to that for 20o (+,-) at k =0. The weight factor for the latter transition is smaller at kH than it is at k =0. The effective weight factor is the average over the occupied states [Makarov 68]. * I have also computed the weight factors for the other scattering transitions which are allowed by finite k Wc transitions, these are (+,-), with A=2, and 30c + 0c +o in the axial approximation. 0c+0s (+,+), s (-,-) and (z,z), (+,-), also with A1=2. In addition to the with Af=0, (See [Makarov 68].) (+,+) and (-,-) transitions at kZ=kH are weaker than co, in strength to 20c+cs (z,-) at kz=0. 164 c -m The and are similar The (z,z) amplitude is of order k 4, compared to k2 for (+,+) and (-,-), but it is of comparable magnitude at kH for B 0=50 kG. The amplitude of the CocC-co is weaker than o +o . and is weaker still. The 3o +o (+,-) transition is of order k 4, and (+,-) transition amplitude is of order k 6, It is exactly zero in the Yafet model, but has small but finite amplitude in the PB model. 165 4.3 Experimental Background Stimulated spin-flip Raman (SFR) scattering in InSb [Patel 71] was measured in magnetic fields up to 13 T for 10 gm pumping, and 18 T for 5 gm pumping. I have made measurements of the Stokes output power and threshold pump intensity as a function of magnetic field, pump wavelength, and crystal orientation. versus B For pumping in the 10 gm region, the curves of Stokes output show considerable structure which varies with both pump wavelength and crystal orientation. This was the first observation of the anisotropy of the output with crystal orientation ever reported. I also reported the first observation of stimulated SFR scattering with pump wavelengths between 9.6 and 9.73 jim in the P branch of the 9.6 gm band of the CO 2 laser spectrum, and with pump wavelengths between 4.75 and 4.87 gm obtained by frequency doubling these laser lines. The data indicate that all of the observed structure between the low-field and high-field cutoffs of the stimulated output is due to intraband This is in agreement with absorptions at the pump and Stokes wavelengths. previous work by Dennis et al. [Dennis 72] [Weiler 74] at magnetic fields below - and later by Weiler et al. 10 T, but is in disagreement with the work of Wachernig and Grisar [Wachernig 74] at fields between 10 and 14 T. At magnetic fields above 10 T, the Stokes output shows two minima at - 10.4 and 12.2 T for 10.6 gm pumping. Wachernig and Grisar [Wachernig 74] interpreted these minima as arising from the combined effect of intraband absorptions and resonant interaction between the electron spin and the transverse optical (TO) and longitudinal optical (LO) phonons, respectively. spin-phonon interactions, if present, would be 166 These resonant electron expected to occur when the electron spin-flip frequency phonon frequency, WoTO os becomes equal to the zone-center TO or LO or COLO. [Koteles 74] I attribute the minima at - 10.4 and - 12.2 T to intraband absorption only. The results with 10 tm pumping show no evidence of any resonant electron spin-phonon interaction effects. This is further supported by the data obtained with pumping in the 5 gm region, for which intraband absorptions are essentially negligible. 167 4.4 Experimental Conditions The InSb samples used in the 10 gtm pump experiments were n-type, single crystals with carrier concentration ne=2x10 6 cm -3 and tellurium doped e=lxl105 cm2 V sec - 1 at 77 K. mobility They were cut from large ingots and lapped to the approximate dimensions 8 mm x 9 mm x 22 mm. The 8 mm x 9 mm end faces were polished plane parallel to within 0.250. The samples were held on the cold finger of a liquid-helium cryostat in the bore of a 4 in. Bitter The sample temperature was estimated to solenoid providing fields up to 13 T. be at - 20 K. The pump laser was a transversely-excited, atmospheric-pressure (TEA) CO2 laser equipped with an intracavity NaCI Brewster window for polarized output and a blazed repetition grating of rate - for 1 pps. single line operation. The output It showed was strong operated random at a self-mode locking, and the envelope of the pulse train was observed to have a width of - 200 nsec (full-width at half-maximum). Values for peak power were obtained by ignoring the mode locking and simply dividing Raman Spin-flip qpll q _B the average energy scattering and Ep II B was per pulse by the above done in the p distance configuration with where qp and qs are the propagation vectors of the pump and Stokes radiation, respectively, and E pump radiation. collinear pulse width. is the electric vector of the A 7 mm square aperture was placed in the pump beam at a 1.4 m in front of the InSb sample. The full beam width 2w 0, corresponding to l/e intensity points at the sample position, was measured to be 5 mm. The values for pump intensity, as used in this paper, were obtained 168 by dividing the peak pump power by tw 2 . used to filter out the pump Long-wavelength-pass filters were radiation from the Stokes latter was detected with a Ge:Cu detector at 4.2 K. radiation, and the The output voltage pulses from the detector were converted by a peak voltmeter to a dc signal which was displayed on a chart recorder. 169 4.5 Results and Discussion The SFR Stokes output and threshold pump intensity vs BII [111] for three pump wavelengths X = .10.59, 10.15, and 9.73 gm are shown respectively in P Figs. 4.4 and 4.5. The output data were taken by sweeping the magnetic field and the at fixed pump intensity, similar sweeps after attenuating data were threshold intensity the pump obtained with by making CaF 2 crystals of The output data of Fig. 4.4 were taken at pump intensities varying thickness. of 1.4, 1.3, and 0.8 MW/cm 2, respectively. 0.8(c) Xp= 9.73psm 0.6 0.4 30.2 0 a 0.0 _jI 20 40 60 80 100 120 140 C6 D O W 4 0 (p 2 '.-_2 W (p) 20 40 60 80 (s) 100 ,C-LO 120 140 S12E (a)Ep 10.59 " , I 2C+WLO . 20 Fig. 4.4. with carrier Relative 60 80 100 120 140 MAGNETIC FIELD (kOe) Stokes output power vs applied magnetic field for InSb concentration and qpll [110]. 40 n = 2x10' 6 cm 3 and oriented with E IB 11 [111] oe denotes the spin-flip frequency. 170 The low-field cutoff observed in the Stokes output of Fig. 4.4, and the corresponding sharp rise in the threshold pump intensity of Fig. 4.5, can be understood by the results of Fig. 4.6. For pump photon energies less than half the zero field energy gap, E (B =0), the cutoff results from the decrease in free-carrier the effective concentration for SFR scattering at lower magnetic For pump photon energies greater fields as discussed previously. [Patel 71] of the pump and than !E (B =0), the cutoff is due to increased absorption Stokes radiation by holes this shown, at disappears absorption as a result of two-photon Since the energy gap E (B ) increases with B ° absorption across the band gap. as 59] created [Kurnick sufficiently high B which for IE (B ) >hW . 2g 0 At threshold p fields magnetic pump intensity for cutoff the above the Stokes output and show considerable 10.15 gm pump and 10.59 point, I attribute the observed structure structure, as may be seen in the figures. to intraband absorptions of the pump and Stokes radiation by the conduction electrons, whether as the indicated. given The absorption p letter is for or the s in pump the indicates parenthesis radiation or the Stokes radiation. A comparison of the data for 10.59 and 10.15 pm pump shows that the observe structure in the Stokes output shifts to higher magnetic fields for shorter pump wavelengths, in agreement with the shift of the absorption peaks to higher magnetic fields [Weiler 74]. Our identification of the observed structure with intraband magnetoabsorption is consistent with previous work at magnetic fields below - 10 T [Dennis 72, Weiler 74, Wachernig 74]. 171 1200 (c) Xp = 9 .7 3pm . 800 N 400 SI >I- 0 m 20 a . I I .. 60 40 II g i 80 100 A I II 120 I- I 140 2 WC ' 400 Ia 3Wc (p) 0 O _C I () a. o .I m (b) Xp I(3.15 1 z I . I. 20 w400 40 I 60 . I 80 (s) I .100 . I 120 S()Xp= I0.59pm I 140 (+ I" 200 V Fig. 4.5. 20 Threshold 100 40 60 80 MAGNETIC FIELD (kOe) 120 140 pump intensity versus applied magnetic field for InSb with carrier concentration n = 2x106 cm e and qpll [110]. 172 3 and oriented with E II B II [111] p 0 1 o 120- I S100- o I [100oo] "H II [Ill ] H II (110] L- 800 6040- o 20J 115 120 125 PUMP PHOTON ENERGY, Ep (meV) Fig. 4.6. photon 130 Low-magnetic-field cutoff for stimulated SFR scattering versus pump energy for InSb with carrier concentration n e = 2x106 cm - 3 . Also shown is the field-dependent energy gap calculated from the band parameters given in [Weiler 74]. 173 In the magnetic field region between 10 and 13 T, two minima are observed in the Stokes output at - 10.4 and - 12.2 T for 10.59 gm pumping. These minima were attributed by Wachernig and Grisar [Wachernig 74] as primarily due to resonant interaction between the conduction electron zone-center TO and LO phonons, respectively.[Koteles 74] spin c + os , pump absorption, where oc, the Instead, I attribute these minima to intraband absorptions only: the minimum at 2c and is the cyclotron 10.4 T to the frequency of the conduction electrons and the minimum at - 12.2 T to the strong Co + oLo Stokes absorption. phonon field The minimum at - 10.4 T cannot be due to the electron spin-TO interaction because (i) expected for this changing pump wavelength. it is not observed at the value of magnetic interaction, and (ii) it changes position with The minimum at 12.2 T cannot be due to the electron spin-LO phonon interaction because it shifts completely away from 12.2 T for 9.73 gtm pumping [Fig. 4.4(c)]. These observations are supported by the threshold data of Fig. 4.5. One significant difference between the Stokes output data of Fig. 4.4(a) for 10.59 gm pump and that of Wachernig and Grisar is the strength of the minimum at 10.4 T. Whereas I observe a weak minimum at that point, they observe a complete disappearance of Stokes output. The reason for this is made clear in Fig. 4.7 where I show the relative Stokes output vs applied magnetic field obtained with 10.59 gm pump intensity of samples oriented with B0 1[111], of the observed qualitatively, structure in 1.4 MW/cm 2 from [110], and [100] directions. the Stokes output correlates, with the observed anisotropy in magnetoabsorption Fig. 4.8 for 10.59 jim radiation. 174 The anisotropy at least as shown in (c)HII [10 n- 0)( 8 F- (s) / 3,c, 2w+,La 4 \ (s) (s) \ I F- , ir I/ /, 20 -(b) 0 I , 40 HII (1101 2" Zc+We (p) 2 2Ic ss) 1 I 60 80 (s) (p) \ -, + . 100 I/ , 120 140 I' I ~ I I 2 / I" m -124 wc 4 34&c,2WC+WLc'~~jI~s Cs Cs), r(S) 2 "€, I •]s) L , I ,"/rA2' I - 20 , 2,c+('.e C+LO 1 (s) ,c "(P) i , -- ;-s ., I -- 40 e -- 100 80 60 120 1 140 -(a)H II [IJI cr_ 2 c+L (s) s)) 2c+ weC 4C (s) SI 20 Fig. 4.7. I , I , I 40 60 80 100 MAGNETIC FIELD (kOe) , 1 120 Relative Stokes output power versus applied magnetic field in InSb with carrier concentration n e = 2x10 6 cm - 3, for pump intensity of 1.4 MW/cm2 at 10.59 gm, and qp 11 [110]. 175 2wc 0.500.0 o 0.0 : 20 41 (b) EpIIR 0.3 -0.2 - [10], S H-11[ S 0.1- 0.0 Fig. 4.8. 20 4( Mt ,GNETIC FIELD (kOe) Magnetoabsorption coefficient with n = 2x1016 cm - 3 at 10.59 gm. [a(B ) - a(0)] versus B 0 for InSb Sample No 17 with qpll [111], others with q Ip [110]. 176 For unambiguous observation of possible electron spin-phonon interaction effects near 11.4 and 12.5 T, it is essential to use pump wavelengths in the 5 gm region to avoid interference by the strong intraband absorptions just By doubling the frequency of a TEA CO 2 laser in a crystal of discussed. second harmonic tellurium oriented for phase-matched generation, I measured the Stokes output of the SFR laser using pump wavelengths between 4.75 and 5.3 gtm concentrations 18 T. fields as high as at magnetic InSb samples with carrier of ne=2 x106 and 5x1016 cm - 3 were studied at peak incident powers of 4 to 7 kW. No structure was observed either in the Stokes output or the tuning behavior of oa versus B which could be attributed to the electron spin-phonon interactions. Figure 4.9 shows the Stokes frequency shift as a function of magnetic field up to 18 T for an InSb sample of carrier concentration ne = 2 x 1016 cm 3 . For fields above -10 T it was essential to use pump radiation at wavelengths shorter than 5 gm in order to take advantage of band gap resonance enhancement [Mooradian 70] since the effective band gap increases with magnetic field. Note that there is no discontinuity in the tuning behavior or "pinning" near 12.5 T where o s = cOLo. Such pinning had been observed in the polaron case when the cyclotron frequency coincides with (OLO [Dickey 67]. Figure 4.10 shows the relative Stokes output as a function of magnetic field from -10.5 T to 14.5 T for the above sample with pump wavelength X =4.867 jLm. The pump beam of -4 kW peak power was focused onto the InSb P The Stokes radiation was sample with a BaF9 lens of 32 cm focal length. separated from the pump radiation by passing the output beam through a Perkin-Elmer Model 98G monochromator and detected with a liquid nitrogen 177 cooled Ge:Au detector. The monochromator slit width was set at 2 mm and the drum was swept manually to track the Stokes frequency. The Stokes output shown in Fig. 4.10 has not been corrected for the instrument function of the monochromator. The dips indicated by the arrows are due to atmospheric water vapor absorption [Plyler 60]. magnetic field region Note that there is no anomalous behavior in the around 12.5 T where = Lo, indicating that the resonant electron spin-LO phonon interaction is either nonexistent or too weak to affect the Stokes output. 250- E 200 i, 150 W 100 o X p 4.867 sm I00P aX p 5.I59um 500 Fig. 4.9. I 20 I 40 I I 60 80 MAGNETIC I I I 100 120 140 FIELD (kOe) I 160 180 Stokes frequency shift versus applied magnetic field B II [110] for InSb with n =2 x 10 16 cm.-3 e 178 1880 STOKES FREQUENCY (cm - ) 1870 1860 1850 1840 MAGNETIC FIELD (kOe) Fig. 4.10. Relative Stokes output power versus B 0 II [110] pumping from an InSb sample with n e = 2 x 1016 cm - 3. atmospheric water vapor absorption lines. 179 for 4.867 p.m Arrows indicate the In conclusion, ne=2 x0l6 cm 3, I have shown that for InSb with carrier concentration the structure in the Stokes output power as well as that in the threshold pump intensity for the InSb SFR laser pumped with radiation in the 10 gm region, can be attributed to anisotropic intraband magnetoabsorption of the pump and Stokes radiation. Furthermore, I have not observed any effects of resonant electron spin-LO or TO phonon interactions on the SFR scattering in InSb. Wachernig et al. [Wachernig 75] have reported the observation of a small anomaly in the tuning behavior of the InSb SFR laser around 12.4 T in a sample with ne=5x1015 cm -3 . If this anomaly is indeed due to the electron spin-LO phonon interaction, our results would imply that this interaction is shielded in samples of higher carrier concentration. 180 5. CONCLUSION A effect magnetic-field-reversal significant 2 oc+O s magnetoabsorption at 20 c and in the electron conduction in n-InSb has been predicted and observed. The only previous observations of field reversal effects in magnetoabsorption for were interband absorption in n-InSb absorption in [Hopfield 60] CdS Chen 85]. [Dobrowolska 83, and spin resonance previous magneto- Three absorption experiments done at MIT did not focus on a field-reversal effect. These were [Weiler 74], did not report observation in either polarization of 2oc+Cs geometry, nor 2o c in the i polarization. suggests the sample geometry would may have been oriented with B II [110] made the field-reversal detect [Chen 85]. a field-reversal relatively small for Other experiments which did [Grisar 78], [Johnson 70], are effect effect and This (see absorption data). compared with some other orientations. 2Oc(a_) not have in the Voigt The absence of 20c 0+ in the a 1 q II [111], as in the case of my Sample #17 orientation The first of these [Favrot 75,76] and [K. Lee 76]. and It is not clear whether the effect is actually observable under The experiment of Johnson the conditions of these three latter experiments. and Dickey [Johnson 70] observed the 2oc(al) transition in Te-doped n-type InSb with n e 1.4x1015 cm - 3 at T = 20 K with B II [110]. Wavelengths of 66.1 gm and 42.0 gm were used, on opposite sides of the Reststrahl absorption, and the 2oc(a 1 ) transition was observed at B ° = 1.2 T and 2.0 T, respectively. The The B 11[110] orientation is not sample thickness was about 2 mm. optimum for the field reversal effect, but should produce an observable effect for q II [110] or [111]. absorption electric data The effect would not occur if q II [001]. for InSb #16 quadrupole mechanism and #17.) is too 181 weak Johnson's to cause observation the 2o c (See my that the absorption (although his numbers are incorrect) suggests the possibility of an unknown absorption mechanism, since my calculations show that the EQ mechanism has a larger probability interesting than the inversion-asymmetry to repeat Johnson's experiment mechanism. It would be to see if the field-reversal effect can be observed under his conditions. The magnetoabsorption experiments of Chen et al. [Chen 85] were done with n-type InSb samples with ne lxl014 cm - 3 to 5x105 cm - 3 in from many orientations, at T = 4.5 K and wavelengths of 96.5, 118.8, 163 and 251.1 gm. These wavelengths are all longer than the Reststrahl band from 51 to 54 Lm. The sample thicknesses varied from 1.9 to 4.5 mm. This paper only discusses the spin resonance absorption, but the following paper in Physical Review by Gopalan et al. [Gopalan 85] states that the field-reversal effect was not seen for the 2o or 20c+ transitions s in any of Chen's data. information would be required to find the reason for this. Additional A possibility is that the absorptions were too weak for unambiguous observation of the effect. The weakness relative to spin resonance results both from the larger linewidth and from the decrease in absorption strength at low magnetic fields. unknown factor field-reversal is how effect, occupation since of additional calculations have Landau been conditions, which would not apply for the 2%o based and 2o +o Another levels affects on quantum the limit transitions at low fields in Chen's higher-concentration samples. The magnetophotoconductivity experiments of Grisar were done in InSb samples with ne= 8x1013 cm 3 wavelengths The B01 [001], of 9.54, 10.26 and [110] and [111]. 10.59 gim. et al. [Grisar 78] at T =12 K and CO2-laser sample orientations were The main differences between their experimental conditions and mine, then are the low conduction electron concentration, lower 182 temperature, and use of photoconductivity the light absorption. instead of transmission to detect It would be useful to repeat these experiments to see whether the field-reversal effect can be observed. It has taken a considerable time to develop a general treatment for the orientation carrier dependence of the warping magnetoabsorptions. inversion-asymmetry-induced The and inversion-asymmetry-induced complete spin-changing angular dependence transitions, of neglecting free the the B-reversal effect caused by MD and EQ contributions, was obtained by Rashba and Sheka in 1961 [Rashba 61a] via the decoupled effective mass approximation for the conduction band. Later work on the anisotropic magnetoabsorption using the coupled conduction and valence band (PB) theory largely ignored the work of Rashba and Sheka and its angular generality, focusing on the case of B in the (110) plane. Pikus, Following Suzuki and Hensel, [Suzuki 74] and Bir and [Bir 74] Trebin et al. [Trebin 79] produced the invariant formulation of the Pidgeon and Brown model which was needed for application of the general rotation approach of Rashba and Sheka to the coupled-band case. They also gave a symmetry-based characterization of the magneto-optic selection rules in InSb, which extended the work of Suzuki and Hensel on valence band transitions in germanium. A N + F They emphasized the importance of conservation of the quantity in the axial approximation, and the breakdown of the axial model selection rules when warping and inversion asymmetry are considered. Gopalan et al. [Gopalan 85] applied the analysis of Rashba and Sheka to the spin-conserving obtained all of magneto-optical asymmetry. magneto-optical the transition absorptions in the transitions matrix in the conduction elements conduction band needed caused to by band, and find the inversion A connection was made between the matrix elements of the velocity 183 operator and the components of the second-rank irreducible tensor formed from the components of the kinetic momentum operator k. The theory which I have presented is the first to make the complete connection of the work of Rashba and Sheka with the formulation of Baldereschi and Lipari. irreducible tensor La Rocca improved Rashba's rotation technique by including the third Euler angle, which simplifies the treatment of cases where the optical propagation and polarization are arbitrary. I have attempted to combine the different approaches to obtain a better formulation of the magneto-optical problem for free carriers, including the anisotropy, and considering both the coupled model for accuracy and the decoupled model for simplification and for verification at low B . 4x2 off-diagonal matrices La Rocca's coordinate with model rotation to all terms of the Hamiltonian. functions in the PB I have pointed out components of the By factoring the 2x4 and I made in Trebin's it simpler to invariant expression the connection irreducible tensor apply of the operators, angular and have related this to the selection rules for the magneto-optical transitions. After achieving this general formulation of the PB model in a rotated coordinate frame it was discovered that the EQ or MD contributions to the 20cc(a) and 2oc+0s(1r) field-reversal Voigt transitions were sufficiently large to produce a effect in the magneto-optical absorptions. The experiment was set up and carried out, and the resulting data showed large changes in the absorption which were even greater than those seen previously in the spin resonance absorption. The comparison between experiment and theory indicates agreement 50%, to within with stronger than what is predicted. the observed absorptions being generally Some of the uncertainty in the prediction comes from lack of knowledge of the multiple parameters in the PB model which 184 Better theoretical and, hopefully, are needed to compute the matrix elements. experimental estimates of the inversion asymmetry parameters G and G', C and and N C', N are needed, with consideration of deviation from the single group approximation which sets G = G' and P = P'. Work should also be done to find the influence of exchange effects on experimental determination of the parameters. experimental results and the The linear-k parameter C in the valence band block Hvv of the PB Hamiltonian is expected to be small compared to the off-diagonal-block linear-k parameter estimate of the off-diagonal C' in Hvc, based on Cardona's spin-orbit interaction parameter A. Additional work should be done to determine both of these parameters more precisely. More work could be done on measurements of the 2oc(al) and 2c+s Voigt absorptions. (tn) The measurements should include the use of higher magnetic fields and shorter wavelengths, and should use exchange gas cooling to reduce stress in the sample. orientation, temperature, They should involve greater variation of wavelength, doping and concentration, and should include photoconductivity detection as well as transmission. 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B 1, 2668 (1970). 193 Appendix A Extended Pidgeon and Brown Hamiltonian In this appendix I will derive the Pidgeon and Brown (PB) Hamiltonian with the extensions made by Weiler et al. using the invariant expansion approach of Trebin et al. [Pidgeon 66,69, Hamiltonian contains 20 spin-orbit splitting A. Weiler 78,81, parameters besides Trebin 79]. the The energy 8x8 matrix gap E and the g Of these parameters, four are associated with terms of order k and sixteen are associated with terms of order k2 , where k - p+-A C is the kinetic momentum of an electron located in a vector potential A which results from a constant electromagnetic field. background magnetic field plus a perturbing The invariant expansion formalism is a generalization of Luttinger's formulation for the valence band of germanium, based on work by The invariant formulation allows the Pikus and Bir [Luttinger 56, Bir 74]. separation of Heff into terms which are manifestly spherical, octahedral and antisymmetric tetrahedral, and simplifies the expression of the Hamiltonian in coordinate frames which are rotated relative to the cubic crystallographic axes. The PB Hamiltonian has the form [Trebin 79] Hcc HH Hcv Hef cs Hvc Hvv Hvs Hs Hsv (A.1) ss in which the individual matrix blocks are 2x2, 2x4, 4x2 or 4x4. wave functions of the form 195 It acts on fc(r) X(r) = (A.2) fv(r) fs(r) where f3 (r) f fc(r) = f(r)(r) f6(r) If(r) (r) f2 (r) fs(r) = fv(r) = f 5 (r) L 7( J f 4 (r) (A.3) The indices c, v and s refer to the heavy hole valence respectively. band 6 conduction band (F6), Fs light and (T), and F7 split-off valence The numerical indices refer to the Luttinger-Kohn states, as labeled by [Pidgeon 66]. band (v), (LK) basis The basis states will be discussed below. Hermiticity of Hef requires that Hcc = cc , Hvv = Ht vv and Hss = H ss (A.4a) HSC = H CS and Hsv = Htvs (A.4b) and H VC = Ht CV , The wave function is often represented as W(r) = . fi(r)ui(r) where the sum involves (A.5) the eight (LK) basis functions ui(r) for conduction and valence bands at the center of the Brillouin zone. the The spatial character of the basis functions, including the periodicity, drops out of the 196 [Luttinger 55] mass theory final effective being effectively replaced by the Equation (A.5) is the same as Eqs.(A.2) and (A.3) if the band parameters. functions ui(r) are replaced by 8-component unit spinors, each with seven zero elements and a single unit element. The LK basis functions uI through u8 are the conduction band-edge and valence band-edge eigenfunctions of the crystal Hamiltonian at k=O, with the The conduction band basis functions ul and spin-orbit interaction included. u2 form a basis for the 16 representation of the Td point group. functions u3 through u6 form a basis the for I8 The basis representation of T associated with the light and heavy holes, and u7 and u8 form a basis for the F7 representation, associated with the split-off valence band. The three The basis functions for these three Iv 8 and t v. bands at k=O are denoted f, 7 6 basis functions of the full D and D bands transform like the D rotation group R(3), 1/2 3/2 1/2 respectively corresponding to spin j=1/2 even parity, j=3/2 odd parity, and j=1/2 odd parity, as was pointed out by Trebin et al. The association of the actual basis functions with the D+1/2, D-3/2 and D-1/2 basis functions is a mathematical basis functions transformation do properties not with convenience, definite possess respect to become particularly clear in Appendix C.) R(3). or artifice, parity (The or since the actual definite 'convenience' group will In the tables of Koster et al. it is the D +3/2 basis functions of R(3) which are used for the TF 8 basis states, and this caused Weiler et al. to conclude that the 16 and 1F7 representations were reversed in Koster's tables of coupling coefficients. By reordering and changing some signs it is possible to make the D3 2 basis functions transform like the D_ 3/2 functions with respect to the discrete Td operations, and vice 197 versa. In the present case it is better to make the valence band functions transform like D 3/2 and D_1/2 rather than D+ and D because this maximizes 3/2 1/2 the part of Hef which is isotropic (spherically symmetric). the D3 the and D/ single-group bands representations result from the spin-orbit transformation of basis functions (representations F 1 and functions with respect to T. of 'parity' This is because S, X, Y, Z for the conduction F1 5) which transform like (See [Kane 57,66].) and valence atomic s and p If one particular choice is made for all the F8 bands, all the off-diagonal matrices of the spin-orbit Hamiltonian between F8 bands will be proportional to the 4x4 unit matrix 1j. the The double-group basis states actually contain some admixtures of functions F ®D , 12 1/2 F ®D+ 25 and 1/2 F ®D 2 1/2 due to the spin-orbit interaction, but are principally composed of F ®D+2 and IF @D+ , where D I 1/2 1/2 15 1/2 represents the ordinary spin of an electron. For our representation Weiler's basis functions of the basis functions uI through u8 I will use multiplied by i. This and D/1/2 differs by an overall the functions Notice that this choice for slightly, and does not change the Hamiltonian. D2 3/2 simplifies sign from the usual Clebsch-Gordon [Anderson 89??]. coefficients The basis functions then are 6 Su 10 - D+ iS I 1/2 (1 2 u2= ]iSj> rV: U = u = (A.6a) , - x+i) (X+iY) 30 8 + 2 3 (3 [(X+iY), - 2ZT] F60 198 32 3/2 ) [(-iY)' Uso = - (, --) + 2ZJ 2 [= u80 = F5(x+irY)l+ tV: 7 U )- D 1/2: z] [(X-iY) - Z . = (A.6b) ( ,(A.6c) These functions may be regarded as the zero-order LK basis functions with respect to the spin-orbit interaction [Pidgeon 66], represent the properties. actual LK basis functions and may be considered to with respect to transformation Here S,X,Y,Z are real functions which may be regarded either as as LK basis states for the f and Tv conduction and valence bands neglecting spin, as mentioned above, or as atomic s and p wave functions. and % denote the spin-up and spin-down ( spinors The arrows (). and functions are ordered so that m decreases from top to bottom. The basis The label on the right is (j,m)+ of the atomic basis states, with the superscript denoting the parity. The numbering [Weiler 78]. associates This odd gives numbered is assigned consecutive basis according numbers states with to the to time [Pidgeon 66,69] reversed a-set so-called pairs and and ('spin-up') axial model wave functions at k =0, and even numbered basis states with the ('spin-down') b-set wave functions. (The axial model will be discussed later.) An advantage of the present formulation is that the basis matrices can be constructed purely from the Clebsch-Gordon coefficients contained in the basis functions uio(r). The chosen phases and ordering of these functions produce the standard representations for total angular momentum L+I 199 when the basis states are viewed as atomic wave functions. Here L = rxp , and ax, y and a are the standard Pauli spin matrices are the standard Pauli spin matrices Ox=( 1 01) , a = (0-i0 1-01 , ,0 which operate on two-component spinors. the D" 1/2 bases are just - 2 (A.7) The matrix representations of L+- , and the matrix representation in the D in basis 3/2 is J, where 3 0 O0 0 2 2 0 0 V3 Jx = L0 0V3 0 0 -2 i0 0 0 0 J Y 20 0 O' O' 0 1 2 v0 0 VS 0 0 -1 0 0 0 -3 J (A.8) Note that 0+ 00) a=( (A.9) o0 and 0 0 0 0 V3 0 20 0 0 0] 0 J+= 0 0 0 0] J I, (A.10) L0 The basis matrices for the cc and ss blocks are 1, ax , ay, a or 1 and (; ) . (A.11) The basis matrices for the vv block are (see Appendix B) 1 , J",j), (A.12) J2) (3), 200 is the irreducible spherical tensor or rank I formed from the J() where [Luttinger 56]. The Cartesian matrices obtained from j(2) and j(3 ) are given in Table A.1. The components simple of J, was as demonstrated by Luttinger numerical representations of the J(f) matrices makes them easier to use than the Cartesian ones. Terms in the invariant expansion of Hef have the form C a )K( teff - )* as discussed by Luttinger, and further developed by Bir and Pikus, and applied to InSb by Trebin et al. specifies the basis function Bir 74, Trebin 79]. numerical, and K Here e labels a single-group ,irrep of Td and u of ('partner') the representation [Luttinger 56, a matrix operator which Here X represents is purely represents a spatial operator formed from the components of k or B or both, or also the electric field E. Basis matrices for Hcv can be found from the representation of k p in the Here k is taken to operate only cv block, which will be abbreviated (k.P)cv on spinor components fi(r), while p operates only between the basis functions Ui(r), so (k-P)cv could be written as k pcv . The k-p matrix is (k -p) = P 2 + R 6 (A. 13) - where P - <iS pxlX> = <iSI py Y> = <iS PzIZ> . The matrix of k-i , where lattice potential, has the h = p + -2 mc same form. 201 (A.14) xVV(r) and V(r) is the periodic crystal The contribution of the term proportional to exVV to P is so small that it is generally neglected. The invariant representation of (k p)cv is (k -P)cv = Pk t , (A.15) where the components of t are t F-i t = t (A.16a) , O i 0 (A. 16b) 0 - 0 0 = (A.16c) -0 0 0.- with t+ =2 (A. 17a) 0 2 2 0 0 - O (A.17b) 0 0 0 The ti matrices are proportional to the matrices Ti defined by Trebin et al. [Trebin 79]. couple the They transform like a polar vector (negative parity) since they DI basis states with the D+ basis states. The remaining matrices required for a complete set for Hcv are obtained from the second-rank tensor (at)(2 ) formed from the products 202 a.t. . ii Note that t. J is a cv cross-space also operator while a i operates in the c subspace, in the cv cross-space as desired. Trebin's matrices proportional to a.t. and a.t.+ a.t. [Trebin 79]. II t. =- 3T.; I Ij = o.t. I j I -3T.: II T.. and T.. are The relations are ot + at xy 1 so the result is yx =- 2ViT xy and c.p. (A.18) Basis matrices for the Hvs block of Heff are found from the matrix representations of L, ( and L ( 2 ) in the vs cross space. For the vv, vs and ss blocks we find [Luttinger 56, Suzuki 74] vv ss L.1 2 -J-. 31 2 3 . 2 -J. 3 1 --.3 1 1 1- 1 1 2 1 (A.19) -- u.1 1 (o)(2) 0 J(2) L(2)_ vs 3 3 Here u.I = t l. (A.20) numerically, but u is an axial vector, like 8 and J, instead of polar, since it connects DT 3/2 with D. 1/2 Notice that the sum L.+ c. 1 2 1 gives J., 1 1 2 1 and 0 in the three blocks, as one would expect for the total angular momentum. (See the last transformation section of [Luttinger 56].) of products of L. Suzuki and Hensel [Suzuki 74]. the entry 3ilx should be - 3ilx .) The complete spin-orbit and L L. with a. is given in Table I of (In the second to last column of this table, The basis matrices for Hvs are obtained from u' and (Ua)( 2 ). (A.21) 203 Finally the basis matrices for Hcs are found from (A.22) 3+ 3 - where (A.23) t' Here pi is numerically equal to o i but p is a polar vector instead of axial [Trebin 79]. The remaining basis matrix is IP which is a 2x2 unit matrix transforming like a pseudoscalar. In summary, the complete set of basis matrices is : H Hvv : 1 1, and (o7) ) j( 2 ), (3) (even parity) (A.24a) (even parity) (A.24b) Hss : 1a and (Y0 ) (even parity) (A.24c) Hc Cv t( l ) and (ot)(2) (odd parity) (A.24d) (odd parity) (A.24e) (even parity) (A.24f) Hcs : 1p and p(l), Hvs vs or 1p and t' 1) u(1) and (uo()(2) . The Cartesian decomposition of these is given in Table A.1 along with the time-reversal properties. Note that the components of j(2) are reducible with O h and T , so that the set {3J - J2 , V3(j 2 -_ 2) transforms h d z x y according to F+12 of O0 h and F12 of T d , and the set {{J ,J}, {J ,J {Jxy,J } yz zx respect to transforms according to F+25 of O h and F 15 of T d 204 Reductions of the other Table A.1. Irreducible basis matrices for PB Table II of Trebin et al. [Trebin 79]. Block CC Hamiltonian. Parity / Td basis R(3) basis +/+/+ rF: J , J , J J 25 j( 2) j( 3) x F: 12 3J2Z - r {J 155 V3(j2 -j 2 X J } y z rF : JJJ 2 r 1 yxy : CV t(l) zxz +/+ , , az tx, t r +/-/- t (2 ) -/+ (ot) rF: 25 cs 1 t (1) u( ) vs rF : : 15 r2F: 25 (uo) (2) +/- and c.p. 1 25 : R and c.p. X -JJJ F : JJJ Ga +/- zyx F25 : J3X _J 20 25 +/+ and c.p. +JJJ xyz 15 +/- z y yt + ot yz zy 1s -/+ 1 -I+ t', t', t' x y z -I- ux X, u o yz +/- Uy, uz ) Z F12 : 3u 3 ZY Z, F : and c.p. V(uxx -u G + uo L zy 205 and c.p. Time rever sal +1+ 1 :1 vv Adapted from +/+ +1+ sets of components oxt = - it , so are given in the table. these combinations 7-t = 02x4 Note that of components give no new and matrices. = 04x2 and uxo = - iu . Similarly u The following algebraic relations among the basis matrices are useful: 00 = 3() , J-J = -(1) , JxJ = iJ o-t = t-J = 0 , oxt t- t txt(tt)(2)= = 2(1) tt t These xo = 2io , J(4 )= , -2tx 5 (A.25b) (ot)(2) = 2(tJ) (2 ) ; t)(2) 1j( used in decoupling for the 2 3 (t3t)2) Hamiltonians (A.25c) 0 ; 4 may be (A.25a) 0; =it 15 relations effective , G( 2 ) = 0; (A.25d) (A.25e) ). the PB conduction and Hamiltonian to valence bands. obtain Relations involving u are found from Hermitian conjugates of relations involving t. The Cartesian decomposition of the second-rank equations may be used to obtain t tl = t tt and xx yy relations like In the present case, with respect approach to to the T like invariant t t =-t tt. xy yx where irreps the crystal basis of the full expansion may be functions rotation applied connection with cubic harmonics and Cartesian tensors. considers and cubic all possible (octahedral invariants and obtained tetrahedral) etc. 206 by group, which a has different a direct In this approach one polarization invariants like ui(r) transform 2 r, of 4 r, the spherical xyz, x 4+y4 +z4 Using the definitions of the band parameters given by Weiler et al., the components of Hef are (with h = m = 1) = Egl H H VV _=- 2 + (F+-)k 2 k J 21 + [{kk + (N+)B a 22 + yk 2 XX + k2 J y Ik 2 Hs = (-A)1 + k 2 ZZ - k 2 2] 3 xJ -- q [B + c.p.] - }{,JJ C[k {J , J 2 - + 2 YY (A.26) 2 + ByJ + B } + c.p.] (A.27) z (A.28) (Ic'+)Ba Hcv = Pkt - iG[{k,k}t + c.p.] zz +c.p.] yy + ¢-t) 2 x (at - FiN[B H CS (at + t ) + c.p.] (A.29) (A.30) = P'kt' - iG'[{k,k }t'z + c.p.] X Y Hv = -v ' y[k2U ax + kUy a + kZuo] V- yk[{k,k }(ua 23 x y xy +"I where {a,b)} e(c"+1)B.u + ab + ba + Uy yx x) + c.p.] iC'[kx(uy z + uz is the anticommutator. completely general as written. + c.p.] (A.31) The above components are The choice of the numerical coefficients makes the primed and unprimed band parameters, except for C and C', equal in the 207 limit of small numerical spin-orbit constant free-electron coupling (single group approximation). The associated with F results from the contribution of the - 2 kinetic energy to the effective Hamiltonian, and the constants , I and 1 associated with N, x' and K" result from the free-electron Zeeman 2' 2 term. Notice that factors of i are required in the off-diagonal terms H(G), H(G'), H(N) and H(C') in order to satisfy the time-reversal symmetry requirement. We can use irreducible spherical tensor components to reexpress Hef t in a form which unambiguously separates [Lipari 70, Baldereschi 73, 74]. H cc the spherical and H SS and anisotropic parts contain no anisotropic terms to second order in k, and therefore remain unchanged, except that the +, -, and z components of all vectors should be used in place of the usual Cartesian components. H , Hcv , H , and H may be reexpressed as vv cv cs vs H VV 1k2 yK 2 ) . j(2 ) C Hcv = Pk t - +q)Bj 1 - 20 j( 2 )] (4) C e [B(10) . j( 3)]( 4) 2C [k(')® j(3 )] (3) CC VA e [B' = P'k -t' - V3G'[K(2)( (A.32) 6N [K(2)( (at)(2)](3) A F CS 2[K(2)® V3G[K(2) t(1)] (3)- A2 C 3 H - -1 2 - Cv + 2 (ot)(2)] (3) A t'(1 ] (3) A (A.33) (A.34) A 208 '+1 -~(2'.(u)(2) + ~2C ("+)B Hvs = -V + 2V3 g'[K(2)® (UG)(2)](4) +V C C'[K(')® (uo)(2)] (3) A 2 (A.35) where - 2 3 SY + (A.36) 3' and r I (3 (A.37) 2) . Here, I use the tensor dot product [Edmonds 74] (_l)m K(2) j( K(2)j(2) _ m 2 ) -m (A.38) = (k 2 + k2 ) + ({k,kS} { J,J} 2 + h.c.) + l3k - k2)(3 2 . I also define the irreducible 4th-rank octahedral invariant T(4)(ABCD) =ABCD +ABCD +ABCD c xxxx yyyy zzzz (A -1 .CD. + AB.CD. + AB.CD) ij + [T 44 + T(+4) -4 _ which is 4 th 4 6 T 04) "5 (A.39) order in the components of four vectors A, B, C and D. I similarly define the 3drank tetrahedral invariant T A(3)(ABC) V3 [A (B C + B C X y Z Z + c.p.] (A.40) = T ( 3) - T ( 3) 2 -2 which is 3d order in the components of A, B and C. 209 The above expressions can be regarded as the complete polarization of the irreducible cubic harmonics x4 + y4+ Weyl 46, Von der Lage 47].) - 3 4 and (See [Edmonds 74, xyz . The first expression has full octahedral (Oh symmetry if the set of vectors (ABCD) contains an even number of polar and an even number of axial vectors. The second expression has tetrahedral (Td) symmetry and is odd under inversion if the set of vectors (ABC) contains an odd number of polar vectors and an even number of axial vectors. expression is easily generalized to include the case of This latter four vectors replacing A, B or C by the cross product of a pair of vectors D x E. by This may be used to obtain invariants of the form A B (C D - C D) + c.p. = -V3[(AB)(2) (CD)(2)] ZZ Yy xx (A.41) (3) A and k (JJJ I use the - J J J ) + c.p. = -[k() standard definitions [Edmonds 74, Anderson 81]. k are and k factor , of for k+- -{, k , -,(3k k2) than the smaller [Baldereschi 73, 74]. (A.42) irreducible tensors and tensor products For example, the components of k(' ) are -l k , where 3 J(3)(3). k ik. The components of K 2 ) k ,k}), and definition used k2 - k+ , [k(')® k ](2) This definition is a by Baldereschi et al. Care must be taken when vector components fail to commute, as with k and J. Expressions for K(3) and j(3) are given in Appendix B, along with some useful tensor products and expressions. In order to change H(y2) and H(y3) in Hvv from irreducible Cartesian form to irreducible spherical form one uses the relations 210 2 + k 2 j 2 + k2J 2 -!kJ H(y) = ,2[k2J ]2 2 2 yy ZZ 3 =-2 [K(2).j(2) + [K(2) (2) (A.43) 4)] and H(y,3 )= ;Y[{k, k }{J Jy } + c.p.] S73 [K(2) J( 2 ) - 2 K(2). j( ) Notice that K(2). j(2) = kJ2 2 xx [K 2 (2 )] 4)] . (A.44) can be written in Cartesian components as + k 2J 2 yy + kJ2 2 zz - 3 k2 + 2 [{kX ,kY }{JX ,Jy + c.p.] (A.45) and also as Compare eB -k2j2 K(2).j(2) = (k J)2 LC 3 [Luttinger 56]. This . (A.46) last expression can be obtained from the recoupling relation (a-p)(b.q) = (a-b)(p.q) + (axb) (pxq)+ (ab)2).(pq 2), which is valid if the components of b and p commute. (A.47) Notice finally that 2 is often expressed in the literature as -k2, i.e. Jk2J 4 ik22 = 3 -k2, 4 (A.48) which is true when j=32 Note that H(g) = - 2j[K(2)® =- 24k2j 2 xx 2 j( )] (4) C + k2j 2 + k2j 2 yy zz k2j2 _ - 3 211 K(2) (2) 5 . (A.49) and 2V3jg'[K(2)0 (U) H(3') = = 2VL (2)] (4) C Xa + k2u y + k2u 2zC K( (A.50) () Similarly H(q) = - -q [BJJJ] (4) + C C 5C [BJJJ]4) + - (3J 2 B.- where we used [BJJJ](4) c [B J3 + B J3 + B J3 y x 1)B-J] -1(3J25 zz (A.51) and (3J2 - 1) = 41/20 , The simplified representation by the for j= . of H (A.52) of the PB irreducible spherical model in tensor 8x8 matrix form is formulation. This is particularly true for the axial part, which contains only the m=0 components of the tensors T(3) and T m( 4), but it is also true for the nonaxial terms. m reason for this is that the basis matrices of the elements along a single diagonal or off-diagonal line. finite elements only at positions 11, 22, elements only at positions 13 and 24.) 33 form Xm() The have finite (For example, j(02) has and 44, and j(22) has finite In addition, the spherical components of the operators k and K(2) are optimum for acting on Landau level wave functions of the axial model, since they operators. 212 function as raising and lowering The axial part of Hef is obtained by keeping only the spherical terms, and the m=O components of the nonspherical terms. The inversion asymmetry terms in Heff are usually omitted from the axial approximation, so that both the axial and nonaxial parts are treated by perturbation theory. The warping terms, which involve the parameters I, i' and q, are all of order k 2 . The first two contain the components of K(2), and the third contains the components of B. The axial parts are (see Appendix C) HU( )= - 2(W 0 - k2J - k k {J+'JQ + 1(3k - k 2 )(3J - 2) 2-2 lk k{J_,J} + 1+-) 'k 2 +k-{ H (L') = 2 '(W + H= - )-k2ua ( - 4(3k - k)( 4 )3 )(W - kk(ua + uo) J2 B+(5J + 5J e -3B k (ua + uo) 2 + - + 2)J + 'B (5 2 (5J -5J- J2 + 2)J_) If we include axial part of H(g) with H(y) we get H(, ) = H(7) + H(L) = y' [(3k + y"'[ -J 2)] + y"[(kY + h.c.)] k2)(3J k k {J,J} + h.c.] , 213 ()41e - + 6k2U 12 G_ - 3 2 + 1)J BJ where - (= 2 0 5 y'" = 7 + 2g(W 0 - 3) 5 Notice that H (7,g) is obtained from H(y) by replacing y by y' along the 4x4 matrix diagonal, replacing places removed from j by y" along the off-diagonal the diagonal, and replacing j lines which are 2 by y"' off-diagonal lines which are 1 place removed from the diagonal. along the We similarly find Hax (y,')= H(T) + H (') ax ax _)] =y'[(3k2 -k2)(3u%)] + y"[J(k2u a + ku +y"'[ 1 k_k(ua+ + u,) + 1 kk(u_ + _)1. Here I avoid the use of a second level of primes by invoking the single-group approximation, which sets y'= y and obtained from H(Y) by replacing g'= g . Once again, H (T',g') is ' by y' along the Am=O "diagonal," replacing Y' by y" along the off-diagonal lines which are 2 places removed from the "diagonal," and replacing Y7 by y"' along the off-diagonal lines which are place removed from the "diagonal." Finally we have H ax (K,q) = H(K) + H ax(q) S- s (K + q)J + ( )(5J- 3J 2 + 1)J A where I have chosen B O to be directed along 214 .,and used s-eB 0/hc. 1 [Pidgeon 66, Weiler 78,81] Axial model Hamiltonian and su Terms proportional to k21 , k21 , so , sJ in matrix form. The and similar [K(2)0 j(2 ) (40) complicated. Notice that proportional terms terms only H Cv in and H to are easy to express j(2) k -t, K(2). are slightly more anisotropic axial and H VS H contain and components, proportional to [L, R' and q, if the inversion asymmetry terms are omitted. Pk-t in Hcv is given by Eq.(A.13). P'k t' in Hcv is given by Eq.(A.22) with P replaced by P'. For Hcc ,' HCV and Hcs we have the 2x8 representation: A hc(1,1) = E + s[(2F+1)(N + 0.5 + 2) + (N +0.5)] N -> hc(2,2) = E + s[(2F+1)(N + 0.5 + 2) - (N +0.5)] N - A aft hc(1,3) = Pv2- V172 at e+1 vq hc(1,4) = - Pv'2~ V273 a -- > hc(1,5) = - Pv2s VI-6 a T hc(1,7) = PZ VTIT3 7 hc(1,8) = PV2s vT3 a a hc(2,4) = PV2 at" V'T6 at - /e+1 Ve+ 1 VVT-2 hc(2,5) = -Pv2s vT273 hc(2,6) = -PV2-s v2 a a" hc(2,7) = PV2sZ VT3 at VV+-r hc(2,8) = -PV2s V1T73 I For Hvv H and H (valence band blocks) it is straightforward to derive the following 6x6 representation: following 6x6 representation: 215 A hv(1,1) = -s[y,(N + 0.5 + ~2) + 1.5 K + y'(N + 0.5-22)] A A hv(2,2) = -s[y(N + 0.5 + 2) + 0.5 hv(3,3) = -s[y (N + 0.5 + A hv(4,4) = -s[y(N + 0.5 + N ---> -1 A - y'(N + 0.5- 22) N-- --2)0.5 K - y'(N + 0.5- 22)] N- A e+1 A -_2)1.5 K + y'(N + 0.5-22)] N- +2 2 hv(1,3) = sy"V.3 a2 a --- > e(+1)TT( hv(2,4) = sy"V3 a2 a2- hv(1,2) = 2sy"'V3 a a -- > II hv(3,4) = - 2s y"'3 a a -- hv(2,5) =- sV2[0.5(+1) + y'(N + 0.5 - 2(2)] N --> A A hv(3,6) = - sV2[0.5(K+1) - y'(N + 0.5 - 2(2) N -t ve(+1 t2 -_(+l) hv(1,6) = - sy"6 a2 hv(4,5) = sy"A6 (at)2 hv(1,5) = - s (y"' 2 (at)2 a a -- hv(3,5) = 3s y"'2 at at ____ hv(4,6) = - sy"'6 at at - 2) + (+0.5)] N --> hv(6,6) 2) - (K+0.5)] N -- 0.5 + FT __ __---- A hv(5,5) =-A - s[y (N 4 0.5 + (N 4 ( +1)(/ +2 a hv(2,6) = 3s y"'2 a =-A- s[ VN+2 A +1 The replacements indicated on the right are the ones which occur when the Hamiltonian operates on a multicomponent wave function of the form which diagonalizes Haxia, described below. The unspecified elements hamiltonian are the hermitian conjugates of the ones above, or zero. used 5 to represent the wavevector along B0 divided by V2s Sk /V2s . 216 of the I have Axial model wave function fc ( r ) f(r) = fv(r) fs(r) with f(r) = exp(ik g)exp(ik ) [ci fy(r) = exp(ikl1)exp(ik ) ] 6 Cs Pe+ C4(P f (r) = exp(ik)exp(ik ) Here, t pn oscillator [ 8 1 +2 +i is an abbreviation for (pn(4+(krlIs)), which is a simple function (hermite-gaussian) centered quantities, or quantum numbers, are e, k at and kr. - (k Is). The harmonic conserved Notice that in the Landau A gauge, with A=Bo0 r , k is a raising operator for the single-component LL wave functions with the form exp(ikrrj)exp(ik )(p (4+(ic Is)). When Hial operates on a wave function of the above form, then the energies can be found by the diagonalization of the numerical matrix obtained by making the substitutions indicated above. The numerical Hamiltonian may be regarded as the eth block 217 of the representation of Haxial among basis functions of the form (pXi , where seven Xi is a unit spinor with zeros and a single corresponding to the LK basis function ui(r), When nonaxial components one for components, remembering that e= of Heff are considered, the blocks values of t become coupled. n+mJ -2 of different [See Evtuhov 62, Trebin 79, Pfeffer 90.] For k =0 the 8x8 numerical Hamiltonian matrix decouples into two 4x4 blocks [Pidgeon 66, Weiler 78] corresponding to the a-set and b-set solutions. The corresponding wavefunctions have only four nonzero components. subspaces are coupled both for finite k The two and for finite inversion asymmetry. This means that at least some of the magneto-optical transitions which are induced by the lack of inversion symmetry are also induced by finite k . [See Trebin 79.] Band parameters We now consider the band parameters. The parameters which are finite in the single-group approximation of the PB Hamiltonian are F, P=P', G=G', " =( , 2- '3 which includes 14 parameters. K==33 Those parameters which are finite only as a result of corrections to the single-group approximation are N1 , N2 , N, These are spin-orbit all q, C and C'. to spin-orbit proportional couplings between combination of the two. splittings the valence band of higher bands, and higher bands, or to or to a The differences between the primed and unprimed parameters which are finite in the single-group approximation are proportional to these same splittings or couplings, as well as to the spin splitting A of 218 the valence band. Notice that since C and C' both result from the spin-orbit interaction there is no reason to expect them to be equal. The coefficient of C' was originally chosen so it would be equal to C if both parameters resulted exclusively from the off-diagonal spin-orbit coupling between the T v band and higher T 2 bands above the conduction band. valence (Cardona has recently stated that C results primarily from F12 levels among the core states deep in the valence band [Cardona 86].) The largest contribution to C' probably comes from the off-diagonal spin-orbit coupling A between the tv valence band and the Tc15 higher conduction band, which does not contribute at all to C. [Kane 57] and [Bell 66]. For the estimated location of the (See single group levels at the Brillouin zone center see [Dresselhaus 55] and [Cardona 66].) The set of band parameters which I have used in my calculations is the one which was determined by Goodwin et al. and by Littler et al. for intra-cb and intra-vb processes, respectively [Goodwin 83, Littler 83]. The parameters are listed in Table A.2. Table A.2. Band Parameters for the PB model. [Goodwin 83, Littler 83] E = 0.2352 eV, g F = - 0.2, l = K= 3.25, -1.3, A = 0.803 eV, E = 23.2 eV p N = -0.55 ' 2 = -0.20, 73 = 0.90 q= 0 219 Estimates of some band parameters based on k p perturbation theory in the 5-level model: See Groves et al. and Suzuki and Hensel [Groves 70, Suzuki 74]. Also see Cardona et al. and Pfeffer and Zawadzki [Cardona 88, Pfeffer 90]. See Dresselhaus et al. for the single-group parameters [Dresselhaus 55]. G P Q - -1.0 E 2 QA= C'V3 E 0.033 1 C= 0 1 Q N N 3Y1/2 E 2 3 2 - -- [P1A1 - PA-] 1 1 (small, depends on the sign of A-) 4 Q2 - q 0.12 - E2 9 P N _ 3E2 [-P A + 2PA-] (small, depends on the sign of A-) 1 Here E l is the energy of the 1 S band relative to the top of the valence band, neglecting the spin splitting. it involves coupling to I have set C to be approximately zero because 2 and r bands above ' uncertainty in the sign of A- and hence of C'. . Note that there is an Cardona et al. [Cardona 86a] assign a plus sign, but this causes too large a magnitude for the cb inversion asymmetry parameter 50. 220 Appendix B Irreducible Spherical Tensors In this appendix I define some irreducible tensors and tensor products which are useful in the expression following Hamiltonian. The Baldereschi 73,74, Pertzsch 78, and references rotation are Trebin 79, Condon 35, of the effective useful: Edmonds 74, mass [Lipari 70, Anderson 89]. First consider a vector operator A with cartesian components A x , Ay and The irreducible first-rank A . spherical tensor formed from A is denoted A(1) , with components A'm ) defined by A (I ) = o A") A Z IA , where A+ - Ax iA Y Higher-rank tensors are formed by use of the tensor product and the vector coupling, or Clebsch-Gordon coefficients. (AB) (2) [A(') (ABC) (3) _ [A(1)' B()] (2) We use the definitions: ; B()® C()](3) ; etc. 221 and A(n)= [A(1) A(n-l)(n) Here '®' denotes the tensor product. The coefficients in the expression for A(n) are given in Table 3.3 of Condon, reproduced in Table 5.2 of Edmonds. The above expressions represent the highest-rank tensors which can be formed from sets of vectors, so the result is independent of the order in which the vectors are coupled. Note that A(n)n =A +)n and A(n) = ( A_)n The tensors R (n) formed from the coordinate operator r have the components ( (2n- !11/2 • 1)!! RRm ) = 4Tn rr n m(00)1 ' where Ym(0, ) is the spherical harmonic of rank n. The components of A (n ) may be obtained by expressing rnY (0,4) in terms of x+ and z, symmetrizing with respect to these components, then replacing them by A+ and A symmetrization is unnecessary if the components of A commute. The components (AB) m(2) of the tensor (AB) (2) are m =2: AB 1 m =-1: m =-2: 2 j~AB+ 6 1 -1 -1 B) + + + = -(A (AIB + AB I) m = 1: m = 0: = A+B 1 3 A0B0 Af(A B + A_B o) - - A B Bz+ AzB+) j(3A B - A-B) (AB + AB) 2 2-- -1 -1 222 - . The The superscripts '(1)' on A(1) and B(1) have been omitted for brevity. m m The first rank product obtained from two first rank tensors is B(1)1) [A(1)( (AB)(1) with the components m= 1: m = 0: m =-1: (AIB o- AoB ) !(A B - AB !'(AB- Note that =- (A Bz - AzB ) 2 +Z Z+ ) = - 1(A+B_-- AB+) 8 + -AA_ 1Bo = B). 2(AB-A Z- Z (AxB) = (AB - AB), so AB+ Z 2 + I (AxB)) (AB)(1)_ where 'x' denotes the ordinary vector cross product. The zero rank product of two first rank tensors is [A(')( B(1)](0) (AB)() = 3 (A11B+ AB - AoBo) -1 -1 1 0 =-f AB. Here A-B is the ordinary vector dot product A-B = 1(A+B+AB+) +AB 2 + zz The general tensor dot product is defined by [Edmonds 74, page 72] A (n)B(n ) _ (1) m which also equals m ( Am(n ) B -m n) (- 1)nV2nT-T[A(n)® B(n)] ( 223 ). Some additional tensor products which will be of use are K(2) ] ( 3 ) [t(')( m = 3: m=2: m=l: tK 1 2 tK + 11 302 -5 1 t 1K 0+ 715 t0 K 1 + ]it15 m = 2 0 -tK -1 + 511 m =-1: m =-2: m =-3: The tK J-- 5 t K 2+ 1 -2 StK + -1 K 2 toK o + - tlK 0 0 5 -11 3 5 tK 5 0 1 +- - t1 -1 -1 K° Et K t-1 K -2 superscripts '(1)' and '(2)' on t ( m ) and K ( 2) have been m brevity. [K(2) m = 4: (2) 1 (4) KJ22 m= 3: (K2 J1 + KJ 2) m=2 (KJ+ KJ 2 ) + 14 i-714 K1J 1 m = 1: ]-(K2 J+ m = 0: ]-(K J + K J2 ) + ]s(K J + K J ) + -70 etc. (For m ---- K J2 ) + -(K -2 2 70 J + KoJ 1) 1 -1 -1 1 37 K J 70 0 0 m , change signs of subscripts m and m2. ) 224 omitted for IK(2)() M(2)] (3) m =3: -(KM - K MM2) m = 2: '(KM o- KM 2 ) m = 1: I2(KM - KM2) + 10 2 -1 -1 2) m =- 0: (K2 M 2- K 2M2 ) + m =-: J-(K1 M - K 2M ) m =-2: J'(KoM_2- K2Mo) m =-3: where - (KIM 2- M (2 ) = ((CV) -2(K M - K0 M ) (KIM- KM 1 ) K1M 0 ) + J(KM- 40 0 -1 - KM_ ) (2 ) The tensor products given above contain tensors K(e) up to rank 2 formed from the components of k, and tensors J(I) up to rank 3 formed from the components of J. We will later also need tensors K are listed the components of K for J. and J() of rank 3 and 4. Below for I up to 4 for K, and up to 3 I have included P(t) to demonstrate the form of the tensor components The components of K when the vector components commute. obtained by symmetrizing the components of P() components, and then using the commutation components. 225 ) and ) are with respect to the vector relations for the vector ( 2) (2) m K(2) m m 1 1 -2 2 2a+ 2 J+ - k k v"2po(P I{J , V(3J (Yj2 - J) k 2) - F(3k } F 6 k k_ V2P0 P 1 1 2 2 2 P-1 K( p m(3) 1 2 2 2 - - 3) j( 3) m m 13 V3p 2 3p + B(2p2 + 5 o0 F(5k o(k p_-)po P l1 - k 2 + s)k+ + P P_- )P f(2p 5(p kkk ) f348 j2- 5J + 2)J+ - 3k 2)k - 3J 2 + 1)J 2 - k - s)k _ f PoP-1 - -d(5J 1)J 2 + - A P-1 j2 + 5J + 2)J 2 (J + 1)J - For noncommuting components, as with Jm and km , one must make the replacements 2 POP1I PPo pp - - 2o + pipI 6(PPop - pP2) + 1op + P P- Po + c.p.) etc., before replacing p by J or k. 226 4 p(m ) K( 4) m 1k4 I+ 4+ 3 - 7kf k 2p (3p + F(2p -- (2p pP p)p + 3 F 2 (7k - 7(7k plp-I)Popl + 12pp P_l 1 + 3p2P_ ) 2O1 k2 + 2s)k 3k2 - (35k - + 3s)k k+ 2 30k 2k2 + 3k 4 + 3S 2 --(7 k - 3k - 3s)k k (2p + 3p p )pp_ - k2 - 2s)k 2 (3p2 + PP_ )p_ 2pop - 3 4 k4 P-1 4 - 227 Appendix C Rotation of the PB Hamiltonian In order to compute the Landau levels when the field B0 points in an arbitrary direction relative to the crystal axes it is necessary to perform a coordinate rotation from the frame xyz of the cubic crystal axes to a frame B is directed along A . 1rl in which This appendix shows how the rotation is accomplished, derives the angular functions which are required for the expression of Hef in the rotated frame, and gives the complete expressions for the components of Hef in this frame. generalization where It follows the derivation of La Rocca et al. which is a of the original derivation by Rashba and Sheka to the case the third Euler angle y is finite. Inclusion the of y simplifies magneto-optics problem by allowing the wavevector and polarization directions of the light to be along coordinate axes, without losing generality. The rotation of a term in Hef is accomplished by replacing all vector components in the xyz frame by their expressions involving spherical vector components in the rotated (Ti) k = RX+k+ + Rk reference frame. One makes the replacements + Rk +R Yk =R + Ry +k +R = Ry+kk k = R +k+ + R k , ,k (C.1) + Rz k, and similarly for the components of B0 and the matrix vector operators i, J, t, t' and u. The elements of R i1 are functions of the Euler angles a, 229 3, y, and were given by La Rocca et al. [La Rocca 88b] R = R* X,+ = X, le1 (cos R = R * = y,+ y,2 R This = R * Z,+ -e Z,- transformation + i sina) , cos 2 (sina cosP - i cosx) sin3 2 specializes to the unitary if Ri+ were replaced by V2Ri+ k+/v2 . (See [Rashba 61a].) k + = cosa sin Ry, = sina sinP ; Rz= case = 0 and y = 0 [Luttinger 56]. a = 7t/2 , Rx, , ; cosp ; (C.2) by when considered Luttinger The transformation matrix would be corresponding to replacement of k+ by This implies that the inverse transformation is 2R* + 2R k + 2R* k x+x y+y z+z' = 2R* k -x- x + 2R*- ky + 2R*z- k z k k = R + Ryk + Rk A~ Y zZ k xx (C.3) and also that RR -RR RRyR - Ry_R = iRZ- Rx R - RRx+ = iR x+ y- y+ x- = R 2 z ' (C.4) . These last equations are also valid for cyclic permutations (c.p.) of xyz. As spherical a first example terms in Heff, of this transformation consider such as k-t and B -J and K(2)-J (2). 230 its application to The expressions which result from the transformation are independent of the Euler angles of the transformation, as one would expect. Thus k.t = I(k+t_ + k t+) + k t 2+- (C.5a) B.J= (B+J + BJ (C.5b) -+ +) + Bo J and K(2) (2) = kkJ2 (k k ,k} J ,J + +( + { k_,k} {J+,J)) + I(3k - k 2)(3J-J2 ) . Several key direction of drop out. points of the transformation are the (C.5c) following. First, the A may be chosen to be along B so that the terms containing B ± 0 Second, k+ become raising and lowering operators for free-electron Landau level wave functions, satisfying [k ,k ] = 2s where (C.6) s = eB /hc , and (C.7) [ki,k] = 0 . Third, the basis functions may be requantized so that the matrix operators have the same expressions (representations) in the rotated frame which they had in the original xyz frame. This is what causes the spherical terms to be The requantization is obtained by truly independent of the coordinate frame. A applying the transformation U(apy) = exp(iqn-F) to the basis functions, where i F. is the 8x8 matrix obtained by placing J. and 1 . in the 2x2, 4x4 and 2x2 diagonal blocks of the 8x8 matrix filled with zeros. Trebin et al. [Trebin 79].) Here A (F was defined by p and n may be expressed in terms of the 231 Euler angles; the transformation is found by applying successive rotations by each of the three angles y, 3 and a. The transformation are just the rotation matrices for j- diagonal blocks of and j-2 spinors. The rotation of the nonspherical terms in Heff is more complicated. will use Hvv(C) as an example. the Following La Rocca, we We substitute the expressions for ki and Ji into [k {J ,J 2 H(C) = - X (C.8) + c.p.] 2 z Xy Defining the coefficients (rk;gv) by RxRx (R (KX; gv) =(R 1R- R - RzR R - RyIyIRxR) = 1 EijkRiRiRj ijk ) + c.p. + c.p. (C.9) .-.R we find k J (J2 (K;Rv)kKJkJJ + c.p. = - z) + c.p. (v (C.10a) )kK and k (J2 X Y - )J + c.p. ZX I 1c2V (1C;g)kJgJJ (C. 1Ob) One then gets C H(C)=- I /3- I(X4V (iX;gv) kK{J JX, 232 ' (C.11) The coefficients (C;giv) were defined by La Rocca, and may be expressed in terms of four complex valued functions of the Euler angles, which F3 , are a generalization functions of the of F , F 1 , F2 , Rashba and Sheka [Rashba 61a] to the case of ganeral y. Setting F0 F -++; (++;--) , F -- 4-(+;,), 2 F = (++;+) , 4 (C.12) direct evaluation gives [La Rocca 88a, 88b] F = -T6 sin(2a)sin(20)sin S= 2= F3 = 16 , (C.13a) ei cos(2a)sin(2P) + i sin(2a)sino(3cos 2 -1)] 2 e2i[2cos(2a)cos(20) + i sin(2a)cosP(3cos 3 - 1)] 3i-e[cos(2a)sin(2P) + i sin(2a)sinp(1 + cos 2 )] (C.13b) (C.13c) (C.13d) The coefficients are found to have the following properties: 1. ( X;jgv) is symmetrical in the interchange of Kiand A, and of gt and v. (ICX;g v) = (XK;Lv) 2. (X;gxv) second two. = (rX;vgL) = (XK;vL) . is antisymmetrical on swapping Thus (C.14) the first two indices with the Thus (C.15) (K;gxv) = - (pyv;X) This implies (C.16) (-;K&) = 0, 233 = (++;++) = (+ (+;+) 3. (1&;+ -) = - ( ; = ... = 0. =;+) (C.17) )/4. (C.18) ;)/4 = 0 . (C.19) Thus ( 4. (- ;+ -) = ;) - ( (- -;) = (+ ;Q)*, = (++;*, etc. (C.20) i.e. Swapping plusses with minusses is equivalent to complex conjugation. The finite coefficients with non-negative total index, then, are (++;+) = F3 (++;) = - 4F (++;+-) = F2 (+S;T) = - 4F (+5;+ -) = F (+;-) = - 2F0 (++; - r) = 3F 1' (++;--) = F • ' where the total index is the sum of the spherical indices. (C.21) The negative-index coefficients are determined by the symmetry and complex conjugation properties listed above. (+;- Notice that ) = (-A;+) = -(-SA) (C.22) , which implies that F 0 is pure imaginary, i.e. (C.23) F o = -F*.0 One can define negative-index coefficients by F -m - -F*.m (C.24) 234 The functions Fm are proportional to the angular functions obtained by Rashba eim'y . and Sheka multiplied by exponential factors Rashba's functions Bijk stand for - + (The indices 123 on respectively, and 1 must be subtracted from the sum to get the index on the corresponding function F m .) The magnitudes of the functions are shown in Figs. 3.1 through 3.4 as functions of P polar angle and azimuthal angle a. about the c-axis, rotations prominent feature the of The angle y, which gives coordinate are drops out when the magnitudes is functions that vanish they taken. in A certain high-symmetry directions. IF0 1 has maxima in the [111] directions, and nodes along [001] and [110] directions. IF1 I has maxima along the [110] directions and nodes along [001] and [111] directions. IF I has maxima along the [001] directions and nodes along [111] and [110] directions. IF 3 I has maxima along the [111] directions and nodes along [001] directions. The magnitudes in the high-symmetry directions are summarized in Table C.1. Table Magnitudes C.1. inversion-asymmetry of functions Fm(a,,y) along directions of high symmetry. [111] [110] -3= 0.1443 0 [001] IFol0 0 IF1 0 IFI IF 33 12 0 = 2 = 235 0.2041 0.0625 0 0 - 0.125 0 1 3 16 = 0.1875 When these functions are substituted into the expansion for H(C) in the rotated frame and terms associated with each function are collected, one gets the expression for H(C) obtained by La Rocca, and given at the end of this appendix. The set of terms associated with F are found to be proportional to the mth component of the irreducible spherical tensor (see Appendix B) [k(1 ) 3 j( 3 )]( ) (C.25) . In the xyz coordinate frame, with Euler angles o = 3 = y = 0, the angular functions are F = F = F 0 1 3 = F 0, - 2 We see that H(C) contains only the 8 m = +2 tensor components, and evaluates as ) H(C) = - (C/I)[(k(@ j( 3 ) (33) (k1)@ 2 j( 3 )) (3 -2 ) (C.26) The functions Fm can be related to the rotation matrices for third-rank irreducible spherical tensors. For any third-rank tensor we have T (3) m = D (3 ) m,m T(3 ) (C.27) m where T (3 ) is the tensor formed from the vector spherical components in the xyz frame, and T(3) is the tensor formed from the spherical components, such as k+, k_, k H(C) = , in the 4in - (Cv3) frame. (D(3) 2,m We then have D (3 ) (k(1) -2,m 3 3 j( )) ( ) m (C.28) By comparison with the expression for H(C) at the end of this appendix we find that 236 F3 - F = 2 8 8 F1 F 0 2,3 D(3)) ; -2,2 2,2 F (D(3) - D (3) ) * ;F 2,1 -2,1 (D(3) - D(3) 40 - 2,0 -2 (D(3) 6 8 -3 -2,3 (D(3) - 40 - F (D(3) - D (3) - -1 2,-2 40 D (3) -2,-3 2,-3 (D( 8 - - D_) ; -2,-2 D (3) (D(3) 2,-1 )* -2,-1 (C.29) . -2,0 This may be verified by direct evaluation of the D's. [Tinkham 64, p1 10.] of the F functions for certain directions of P may be The vanishing A understood very easily. When is along a [001] direction, one obtains a C4 rotation by keeping the angles ca and 3 constant while letting y change by R/2. But X1 has Td symmetry A C2 rotation is obtained by letting y change by xi. and is invariant respect with to C2 rotations about [001] directions changes sign under C4 rotations, which are contained in Oh but not Td. symmetry axes about proportional to e 2i in its The direction. This does not lower the is directed along ( because B remains true when B but functions F and F 2 are and therefore satisfy the above requirements, while none Therefore F of the other functions do. 2 may be finite along [001] while the Similarly, when other functions must vanish. A is along a [111] direction R A is invariant with respect F - 1 and F+ 3 - e vanish when A 3 yi to C3 - e 3iy. about This r. , but not by the other functions. is along a [111] direction. 341 changes sign under C2 rotations. F rotations Therefore When A is satisfied by Therefore F+ 1 and F is along a [110] direction This is satisfied only by F+1 ~ e i F and F+2 vanish. 237 Note: 2 and F multiplies terms with A m=3 in R. by (p therefore results in multiplication by a Rotation about phase factor e3ip and similarly for terms with other values of m. The effective Hamiltonians H(N2 ) and H(50) may be rotated in a fashion analogous to H(C). The main difference is that H(N2 ) contains the tensor product of two second rank irreducible tensors instead of first and third rank tensors. The results are given at the end of this appendix. The Hamiltonian terms associated with the parameters C', G, G' and N 3 have the form of the general tetrahedral invariant Ax(ByC + BC) + c.p. (C.30) as shown in Appedix A, where A, B and C are three vector operators, or one vector and two axial vectors. In the case of H(N) the operators are B, a and t, where B is the magnetic field and a and t are matrix operators defined previously. The rotation of this invariant is easier than the previous which contained four vectors, one of which was axial. Ax(B C + BzC) + c.p. = one One now has 7t (C1g)AC 'Cg (C.31) where the symmetrical coefficients (rxjg) are defined by (q.Lv) Rx(Ry RLz + R zR ) + c.p. (C.32) Evaluation of the coefficients gives ( = 8iF8) f ; (+5) =-8iF (+ ) f ; (+ - ) =-2iF0 = -f ; (++-) = 2iF =- ; 8iF41 238 (++) = -4iF f2 ; (+++) = 2iF =3 ; (C.33) (-() = (+() , (C.34) with etc. with negative The last equation allows one to define the angular functions coefficients by (C.35) fm-- fm and implies that fo is real. Notice that (C.36) (c+ - ) = - (K )/4 . These coefficients analogous are to the coefficients B(o1y) [Rashba 61], although the labelling convention here is simpler. of these symmetrical coefficients to the coefficients (Ic&;gLv) defined by The relation may be found through the application of Eqs. (C.4). The rotated expressions for H(C'), H(G), H(G'), and H(N3 ), are given at the end of this appendix. Notice that an invariant of this kind cannot occur in a diagonal block because respect to time reversal. a factor of i is needed for invariance with [See Trebin 79.] Finally we note that the squared magnitudes of the F 's can be expressed in terms of cubic harmonics. This was pointed out by [Rashba 91]. 239 The expressions are F1 2 IF 1 2 F2 (yz) = 2 r , 2 +y 2z 2 + 1 2 2= IF 3 2 = (C.37a) I [r6 - 4r2 (x 2y2 + yz 2 64 2 9[r (x 2y 2 2 2 9x 2 2 2] r 6 , 2X2 ) z (C.37b) + z2x2) + 9xy 2z2 ] / r6 2 2z 2 ] 2 2) / 6 (C.37c) , (C.37d) , where reducible forms of the cubic harmonics are used for simplicity. Von der Lage 47.] [See Here, x, y and z may be expressed in terms of the azimuthal and polar angles a and P via x = r sin3 cosa , y = r sinp sina , z = r cos3 . We (C.38) next consider the octahedral (Oh) terms in Yeff" The general rotation applicable to these terms was first done by [Sheka 69], but the Euler angle y was again set to zero. The present derivation follows the procedure used by La Rocca for the tetrahedral terms H(C) and H(60). We note that an octahedral invariant (cubic harmonic) of the form ABCDX + AB CD + ABC D x x x x y yyy z zzz 5 (AB.CD. 1i + AB.C.D. + A.B.CD.)) j I j j i ij (C.39) 240 is irreducible. This may be regarded as the complete polarization [Weyl 46 or Edmonds 74] of the cubic harmonic 4 + y4 3 4 4 (C.40) 5 Using a technique similar to that used on H(C), and first carried out by Sheka and Zaslavskaya [Sheka 69, in Russian], we write ABCD xxxx +ABCD +ABCD yyy y z Z Z = O (&y) ABCD (C.41) where ( R R R )R XKCxX4L XV RR R + RyyXyyVZ1Z + Rz R zRzRzv ZV (C.42) These new coefficients are completely symmetrical in the four indices, and are in terms of five complex-valued expressible W , with W° , W ,..., 0 1 4 W -m functions or the Euler angles: = W* . Evaluating the coefficients we find m (++++) = W ; (+++ = W3 (++5) = w ; (+rr ( (+++-) = -W/4 ; w,; (++- ) = - W /4 ; ) = W; (+ - ) = (1 - W)/4 ; )= (C.43) (++--) = (1 + Wo)/16 ; with (- ) = (+ (C.44) ) , etc. (Complex conjugate interchanges all +'s with -'s. 241 W is real.) Explicit evaluation of the W's gives = (Cos 4 W + sin4X)Sin 4 p COS4 + = (cos40 + 3)sin4P + Cos 4 P W W1 =8 eiY[(cos4c (C.45a) sin 2 3 + 7 sin 2 p - 4)sin cosp + i sin4a sin 3 3 2W 16 cos (cos 2 + 1) + 7 cos (C.45b) 2 - 1)sin 2 P + i (2 sin4oa sin 2 p cosl3) W3 = e3iy [(cos4 (4 - sin 2p) - 7 sin 2 3)sin (C.45c) cos3 + i (sin4ca sin3 (3 cos 2 3 + 1))] W4 64 cos4 (C.45d) sin + i (4 sin4ca cosp (cos 2 3 + 1))] Polar plots of the magnitudes of these functions azimuthal angle a are shown in Fig. 3.5 through 3.9. high-symmetry directions are given in Table C.2. 242 vs. (C.45e) polar angle P and The magnitudes in the Table C.2. Magnitudes of warping functions Wm(xa,j,y) along directions of high symmetry. [001] [111] [110] 1Wo1 1.0 0.3333 0.5 W1 0 0 0 IWl 0 0 0.125 1W1 03 1W4 1 W is just 4 + y4 +z 4 )/r4 IWl z = r cosp. 0 0.125 ( 0 0.1179 V 12 with 3 = 0.09375 x = r sinp cosa, y = r sino sina, and vanishes in all three high-symmetry directions. It has a maximum value of 0.1403 in the (110) plane for P = 25.50, and equals 1/8 in the (100) plane for 3 = 45(n+4) degrees, where n is any integer. The nodes of the Wm may be understood in the following manner. Wm is associated with terms in the Hamiltonian which are multiplied by eimy when A rotated by y about 5. If A points along [001], 3 rotations because of the Oh point group symmetry. is invariant under C4 The factor eim s/ 2 equals 1 for m = 0 and +4, so W4 , Wo and W 4 may be finite for ii [111] II [001]. For the factor eim(2 / 3 ) equals 1 for m = 0 and ±3, so W3 , W 0 and W-3 may be finite. 2, and A Finally, for II [110] the factor eim 4, so W , W , W , W2 and W4 may be finite. in the table above. 243 t equals 1 for m = 0, All of this is confirmed Expressions for H(g), H(g'), H(q), H(%) and H(y ) are given at the end of this appendix. We note that W occurs only in the combination (W- 1) when 0 0 5 the Hamiltonians are irreducible with regard to R(3). From the perspective of irreducible tensors, the rotation of the irreducible cubic parts of H(o) or H(y0 ) is accomplished as follows: - = H (a) C K(4) 0 C - 0 -4 K4), 0 5 3 y,[B(l) 0 ((1)( 0 K(2 ) ( 3) =eH 2C S0 [K (4) + + K(4) +V + (4) C (C.46) (C.47) We use the convention T(4) T(4) + 1 [T(4)+ C 2 4 -4 + (C.48) T(4)] 5 0 Notice that the irreducible tensor involving B and a is a partial polarization of the K (4) irreducible tensor. If we use the D matrices as before to carry out the transformation to the coordinates of the rotated frame, we find 1 [D(4) + D(4) 4 3 4,4 8 W- W 1 = 28 4,3 [D (4)4 128 4,2 + 0,4 + "7 5 [D(4) -4,1 + D(4) 4,1 -4, 1 (4) 0,3 5 -4,3 -4,2 (C.49a) D(4)] 5 D(4) + D(4) + 16 '- 2 + -4,4 + D 5 (C.49b) (C.49c) (4)] 0,2 D(,4) 0, 1 244 (C.49d) W W 28 [D((4) [D = + D (4) (4) + -4,-1 5 4,-2 -3 S 16 + (4) + D(4) -4,-3 4,-3 1 [D(4) + D(4) -4 8 (C.49g) 0, 2 (C.49h) D(4) ]* 5 0,-3 D(4)]* + V 5 -4,-4 4,-4 (C.49f) * 0,-1 D(4) -4,-2 28 W D(4) 5 + -2 (C.49e) 0,0 5 -4,0 + D(4) 4,-1 D(4)] D(4) + 4,0 - -1 [D(4) + 2 3 5 0 (C.49i) 0,-4 The square magnitudes of angular functions Wm are given below in terms of reducible cubic harmonics [Sheka 69]. (X4 + y4 + Z4)2 / r8 (C.50a) SW 012 0w W 2= 1 [r 2 (X 6 2 |W3 - 2 12 4 4-2[(x y 64 + 4 [r2(x + 6 + y 4 z 4+ 4 z6) - (x 4 4 - 4 2 + Z ) ]/ + 2 r 2 2 2 y ] / r (C.50b) r8 8 (C.50c) + 4 6) + + y6 + Z _ (x + y4 + 4)2 24r2x2yz2] /r 8 (C.50d) S 12 [r 8 + (X 8 + y8 + z 8) 2 - 28r 2y2 245 8 ] / r (C.50e) In this final section of the appendix we catalog the general rotated form of all the terms in the PB Hamiltonian to order k2 , as well as the anisotropic terms to order k 4 in the decoupled conduction-band Hamiltonian R . The rotations were obtained by applying the technique of [La Rocca 88b], which generalizes the technique of [Rashba 61a]. component B We assume that the uniform dc A of the total magnetic field B is directed along C, which allows us to set [k+, k] to zero, and [k, k+] to 2s = 2eB0/hc. However, we have retained terms containing B+ since these are needed to demonstrate all of the tensor components, and also to describe magnetic dipole transitions when perturbing field is present. is that a unitary An important aspect of the rotated Hamiltonians transformation basis functions causes a ("rotation") applied to the Luttinger-Kohn all of the matrix operators in the rotated frame to have the same numerical expression which the corresponding operators had in the original frame. resentation Thus, for example, {J+, J } has the same numerical rep- with respect to the "rotated" basis functions had with respect to the original basis functions. subscripts on the Hamiltonians H(x) below. which {Jx+iJ , Jz We have omitted the band The parameters F and NI are in Hcc; P, G, N2 and N are in H ; P' and G' are in H ; Y , are in H ; vv Y and i' are in H; ss ~1c, ', I' and C' are in H . expressions below, h.c. means hermitian conjugate, (+ by '-' and vice versa, and c.p. means cyclic permutations. 246 , ic, g, vs q and C In the -) means raplace '+' Spherical terms: 12 H(F) = (F + $)k2l H(N 1) . (C.51) ; o = H(Ne -(N1+ )BGi c (N+ 2) (B+ + B+ I (C.52) ) + Beo] H(P) = Pk-t = P [(k+t_ + kt ) + k t%] (C.53) H(P') = P'k-t' = P' [(k+t' + kt4) + k t] (C.54) 1 H(71 ) H() (C.55) 2 = yK( 2) . j( 2 ) [(k = + k2J 2 - + ) k2)(3J + l(3k 6, - J2) (C.56) + H (Kq) S H(y') e -- (K C =-k21 -q)B. + 41 20 o H(K') = - e(K'+ = - J e(K + (k+k{J , J } + h.c.)] 2q) [(B+ + B_) + Br ] (C.58) ; = )B- ( H(') = - V3 Y"K(2).(UG) (2) (C.57) =- 3 - (K+ ) [(k u (B c + B- + k2 u + I(kk((u a ) + B (] ; (C.59) +) + -(3k - k2)(3u a) + u%) + (+ -)) ; (C.60) H(K") = 2C (K"+ 1)B.u = e (K"+ 1) (B+u + Bu+) + Butj ; (C.61) 247 Cubic (octahedral) terms: j(2 )] (4) H(g) = - 2[K(2) (C.62) H(t') = 2V3jg'[K(2)® (u)(2) (4); H (q) = (C.63) j(3)]( 4 ) e q[B'(1) C (C.64) C Antisymmetric tetrahedral terms: H(C) = - (2C/V3)[k(@ j( 3 )] (3), (C.65) H(C')= (3C'/2)[k( 1 )® (uo)(2)] A(3) (C.66) H(G) = - /3G[K(2)@ t(1)] (C.67) (3), A H(G') = - "G'[K(2)& t' ( 1) ] (3) H(N2) = 2 H(N) = - f 6N[K(2) 2 ()] N[B"® 3)A 2 (C.68) (3)(C.69) A(C.69) (C.70) (at)(2)A3) (C) In the cubic terms (point group Oh) and antisymmetric tetrahedral terms (point group Td) we use T ( 4) c T xxxx + T + T yyyy zzzz S[T(4)+ nd-4 2 (4) + 5 T(4)] 0 1 5 ij (Tiijj.... + T.... + Tij.) d9 (C.71) , and 248 and T ( 3) =A (T VF xyz = T (3) - 2 + T + c.p.) xZy T ( 3) (C.72) -2 where Tijkl and Tijk , here, stand for polyadic quantities like A iB CkD and A BICk. In terms of the rotated components we have T(4) = C D 4 C a,,y) T (4 ) m m (C.73) m is the mt h component of T (4) with all of the vector components where T ( 4) m replaced by the corresponding components in the rotated frame (e.g. Jx + iJy is replaced by J+ = J + iJ); we define D4C = 1 [D(4) + D(4) + m where 2 4,m Dmm ( 4 (ot,3,y) D(4)]* 5 -4,m is the e = 4 representation matrix of the proper rotation group R+(3) given by [Tinkham 64] and [Edmonds 74]. T(4) m m , (C.74) O,m' Note that T m4I) D mm((C.75) (oM, },y) (C.75) ( l implies, from this, that [Edmonds 74, Eq. (5.2.1)]; the unitarity of Dmm ( 4) Tm = m , Dmm (4 ,y) T4 m ) (C.76) . The functions D 4mC are related to the functions Wm defined in Eqs. C.43 and C.45 by 249 W 1 1 W W 2 3 4C 1 1 -2 D4C , 8 4 4 W 3 D4C -1 -1 W 2 - W 4C 1 - W 1 W 4 D4C = W* - 1 - W* 2 -1 I D4C -2 = W* -VD4 3 8 -3 -3 4 -4 4 (C.78) (C.79) (C.80) 1 D 4C 4 -4 (C.81) 4 -4 In a similar fashion we have ( 3) A D 3 A(3,) = T(3 m Mn (C.82) m where Dm3A (C.83) D(3) -2,m ]* (3) [D2,m These functions are related to the functions f m defined in Eqs. (C.12) (C.13) by f3 fo0 5 - iD3A (C.84) 0 Sfl* iD =- 3A 5 f2 2 , f 3 4 4 2 iD 3A 3 and f 2 f 3 =f2 *=f f * =3 The f m functions are related to the F m functions by 250 -1 iD3A 1 -2 6 4 iD 3A -3 (C.85) (C.86) (C.87) The f m functions are related to the F m functions by f = 8iF , f = - 8iF , f 2 = - 4iF2 , f = 2iF . (C.88) The functions for negative m are given by (see Eqs. C.24 and C.35) f -m fm* m , (C.89) =-F*. (C.90) = and F We give, below, the rotated terms in the PB Hamiltonian. technique and octahedral and antisymmetric The rotation is accomplished by La Rocca's [La Rocca 88b], using the coefficients (1yLiv), (2g.) the relationships among tetrahedral the coefficients and Eqs. (C.34) and (C.36). 251 described and (X;LV), in Eqs. (C.14)-(C.20) Rotation of Octahedral terms in 3eff H(g) = - 2g xx yy =- 2 k k J J (KXg) - 3 9v =-2 +WI- + (W 0 k2j2 - j(2) K(2). _ 2 5 j(2) {J+,J}) rJ+ 3 14 +t + K(2). 5 + W (2k+k J+ +k [W4 kJ +W 2 (3k 2 k2j2 _ 1 k2_ zz 3 + k22+ k2 2 k 2 )J_ + 2k+k {J,J} + k(3J' J2) 2+ lk k rJj + (3k& - k 2 ){J ,J} + k+k<(3J - J 2 ) + 3 (W5 ) Ik2j2 - 16 - + -k k{JJJ} + (3k2 - k2)(3J 4 2 -+ - +W*I( lk 2 {J,J - +,( _ 2 2 } + kk<(3J - - J2) + (3k +J 2 &r2Jj k + W* 2kk J2 + k 2 {J ,J 3 ( - 2 - 2 1k 2 {JJ } 2) k k {J l + , -16 j2" -k2 + -) k 2 ) {J_,J }- lk k J2) -3k)J_) + W*k 22] 4 - - (C.91) 252 H(2) = 24 k2 u (y + k2 uy (idgy) =2/3' + k2u kkXua 2 Y K(2). (UG)(2 K(2). -2 Rotated H(g') is the same as H(g) with the replacements J2 {J+,J } --- 32 - J2 z g - g', and 2 +_ + (C.92) (U)(2) u+ 3u + u % , { J_,J I uO + u _. (C.93) . 253 The irreducible, e = 4, octahedral part of H(q) is Hc(q) eq [B J + B J3 + B J - I(3J - 1)B.J] c 5 xx yy zz - - (l4Lv)B I J J Jv - -(3J - 1)B-J e W4 cq Bq C 4+J + w 3B (J (5J + W2 24 J +w4 B+(5J + Wl{ + (W o - ) - - 1)J4 + B J - 5J - J + 2)J+ + 3B (J 2 + 1)J + - 3J 3 B(5J - 3J 2 + 1)J + WB_(5J + 5J - 5J - - B_J3 2 + 2)J+ - - J + 2)J + 2B (5J 2 - 3 B (5J + 5J - 1+W B (5sJ - 1)J J B_(5J 2 - 5J - J B_(J + 1)J J + 2)J + !B(5J + 5J - J2 + 2)J - + 2)J - 1)J+ B ( + 1)J- 2 + 3B (J + 1)J - - 4B3) +_j) + W* 3B_(J + 1)J2 + BJ3) + W] 4 -:- (C.94) 254 Rotation of antisymmetric tetrahedral terms in Reff H(C) = (2C/V)[k(J J J - Jzxz J J) + c.p.] x yxy = (C/V)[k x {Jx ,(Jy2 J2z)} + c.p.] = (C/3) = (2C/) (&lg;4v) kK{ JJlJv}. [F 3 (k+(J - 1) +- k J+ + F (- k+(5J - 5J - 2 + 2)+ + 4k (J - 1)J - kJ+ + FI -2k+(5J2-3J 2+ 1)J + k(5J- 5J~-J2 + 2)J - 5k (J -1)J +F + F (- k(5J+ 2)J + k(5J -5J 2k_(5J - 3j2+ 1)J + k (5J~+ 5J - + F* -k(5 + F* (k(J 3(C) 5J -J2+ + 5J - J+ 2)J + 4k (J -J + 2)J' 2+ 2)J - 5k+(J + 1)J2) + 1)2 - k+) + 1)J2 - kJ3. (C.95) 255 H(C') = (iC'/2)[k (u xyz = (iC'/2) + u zy ) + c.p.] (KiXg) k u o = (iC'2) [f3 k+u++ + f 2 (k+(u+% +f + uo+ + ku++) ( 3 k (u + k(u ++ u o(5 + u~C_) + + " 2* k(ua +f3* k u k - +k (uao + uo_) 2ku + % uo_) +k u_ 1 ku+]+ )- - k (u ( + u ) 1 k+uca ) . (C.96) 256 H(G) = -iG[t {k , k } + c.p.] - iG (01t) t kkt S- iG[f3 t+k + f2 2t+k+k + t~k+J + f (t+(3k- +f( -t + fl* (t 2- k2) + 2tk+k - k (3k2 + f* (2tkk + t%(3k - k2 ) - k 2) + 2tk k - - t k+2 tk k t k2) 4+- + tk 3* t k2]. (C.97) H(G') is obtained by replacing G by G' and t by t'. 257 (C.98) - V2N 2[ xx t (ky2 - k z) + c.p.] H (N2) - - V2N 2 S-V2N 2 + F 2 (KXl; v) c t EF 3 2+kk (2+t+(k- 3k) + F, (6 tk + F0 k + F* 6t6_tk - (o+t + 6 + 2(a%t+ +t+k2 -4(o+t k tk v + ot)k tk + ot )(k2 - 3k ) + 12 t k k - 3(T t + a t_)k2 +o t+)kk + 4(ot + ot)k+k - + 2(ot + t)(k - 3k ) + 12 t kk k - tkt - 1-)+ - 3(+t + t+)k2' + F* 20 t (k2 - 3k ) + 60tk2 +F2 (Gk -+ )k] + F*2(yt k - k - (Cyt + Gtj) 3 (-(C.99) 258 i e N [B (yytz + Ot ) + c.p. H(N) yz 3 AcC e N3 (;g) BKGt Sc + f(B+(++ (3 + %t+) + B G+t+) B +B( f +f+- B(i B () t +f*( B5ct - +f2 + t) + tt)- 1B_ oat)+ Bot t -B(t t +- %t) + +f2* B_(at + +f* B t - 4 _t + B+tJ I t]. (C. 100) 259 The fourth-order (in k) anisotropic terms in the decoupled conduction-band Hamiltonian are [Ogg 66, McCombe 69, Barticevic 87, Kim 89]: H(() o = a[Ik 2, k2 + {k2 , k2 + {k2x , k2 ] o y z z x y 4 0[(k + - ky4 + k)z - k4] (C.101) and H(yo) 2 2 C 0 x B k2 + oyB k2 B k2 y y y xx Z zz . (C.102) The irreducible, e = 4, octahedral part of H(cx) is H (%o) c = - a [k 4 + k4 + k4 - I(k 4 + ox y Z 5 = - ( (Kgv) k k WkW4 0 + 4+ kkv 4W k k3 + 3 + S2)] - k4 + s2) -W2(7k 2 - k2 + 2s)k + + WI(7k2 - 3k 2 + 3s)k k+ + (Wo- k2 )[35k4 - 30k + 3(k 4 + S2)] + W*(7k2 - 3k 2 - 3s)k k + W*(7k2 - k2 - 2s)k 2 + 2 4W*k k -3 + W*k4 3 4 (C.103) 260 The irreducible, e= 4, octahedral part of H(y) is -((aB)k2 + 2((;k)(B-k)] k2 - 51 k2 + B 7OB k2 + TB (y 2 C~Yoxx y yy Z Z C 0S - e = Yo[% l) [W4 Bk 2 CYO + W2 (3a2B (B + W(- k k a2 7(0B k - k)(B-k) + 2( + W (a+B + ;B+)k< + 2Y+B+k+kJ -2( k B +(3 + oB)k +!(aB +aB )(3k 2( + B )k+ - -B " W*(- 2 + W* (oBr + (3 + aB )kk 2 - ( 5Bk -)2(a B B 2 - B)(3k B)k BS - &B)kk )k2 + 20aB k)k S(C.104) + + k2) + !B kk - k2) +-BAk )(3ka -k 2 ) a+Bkk%+)3(a B2+2B (W+ - B - (3 + B + - k2) + a B )k k + jB(3k B)k + 2(B - + 2(+.1%4) 261 + - B 3a B~ + W aBk2] (cB k2 + asB )kJ .B)kk2) The third-order antisymmetric tetrahedral term in the decoupled conduction- band Hamiltonian is [Rashba 61a, Ogg 66, McCombe 69, Barticevic 87]: H(8 0)= 50[a(k k k - kzk z) + c.p.] S12 [cxY{k ,(k' - k )} + c.p.] Oxx y z = 9 S- = 0 (ily;Rv) (Y {kk k k I [F3 [+k<k - ok+] + F2 [o+(k2 -Sk-s)k + F [2a (3k 2 - 5k2)k + 4o k k - ok+] - a (k 2 - 5k - s)k+ - 5ak2k ] (k2 - 5k -s)k+] + F[o (k2 - 5k2 + s)k_ - + F* [2a(3k - 5k )kr - a~(k 2 - 5k2 + s)k - 5a+k2k] (k2 - 5k + F* [ + 4s)kk + s - - 2- + F*[o k2k - kk2k 3] Ak k3] (C.105) The relationship of Eqs. (G.23) - (G.31). a 0, yo and 8 to the PB parameters is given in Corrections which go beyond the second-order PB model are expected to be of the order of a few percent. 262 Appendix D Kane and Yafet Models The Kane and Yafet models are simple analytical models for the interacting conduction and valence bands in InSb which take account of the spin splitting of the valence bands and of the k-p interaction between the these bands and the conduction band, but neglect coupling to higher or lower bands. The models have spherical symmetry with respect to the crystal orientation, and axial symmetry Hamiltonian Yafet 59, in the presence applied magnetic field B . The and omits terms of order k2 or higher [Kane 57, 66; is 8x8 66]. of an The effective equation, but has two hole bands with spin hole band with spin . equation Schridinger 3 resembles the Dirac and spin I instead of a single The Yafet model is significant for having predicted observable spin-flip Raman scattering in InSb. The effective Schr6dinger equation is g -E Pk-t Pk.tt -E Pk-t ' t 0 Pk-t' fc 0 f -A - E = 0. (D.1) f Here k-t= 1 k, and 263 (D.2) k k-t' k 3 Z 3 - (D.3) Here k is the kinetic momentum operator in a magnetic field. matrix equation functions fc , fv (D.1) as three equations in three If we regard the multicomponent unknown and fs, we may use the second and third equations to obtain Pk -t f E f- (D.4) and Pk.t't f (D.5) f . E +A c Substituting these into the first equation gives S E+A E E) Using Eq. (2.142) and the algebraic relations of Appendix D we have (k-t)(k-tt) 2 3 k2 (k.t')(k.t' t) = 1 eB o , (D.7) 3C0 k2 + ' B.- . (D.8) Thus E E)+P2k2 3m 2 2 + EE 1 + A P2 3m 2 1 E 1 e E + Ac o f c (D.9) which has the form of the effective mass Schrodinger equation for conduction electrons in the decoupled approximation. 264 A significant difference is the presence of the energy E in the denominators. For E = it is useful to write this as ( 9 - E) + k 2m*(E) + 2 g*(E)gB B 0 f C(D.) = (D10) where - 2P2 m 2 + 3m m*(E) E (D.11) 1 E + A is the reciprocal conduction band effective mass, and 4P2 1 3m E g*(E) 1 E+A) (D.12) is the effective g-factor. (We have restored factors of the free mass m.) The case of a finite uniform magnetic field was first treated by Yafet In this case the problem has axial symmetry and the operator [Yafet 59, 66]. A N + F is conserved [Luttinger 56, Yafet 73, Suzuki 74, Trebin 74, Rashba 91]. Note that N is the number operator for Landau levels in the absence of spin, and F is the 8x8 matrix with m along the diagonal, so the sum represents the total orbital plus spin angular momentum in the direction of B . S= n + m 3 the operator 2 We define as the good integer quantum number (ef _-2) associated with N + F - ~. For a given t the wave functions have the form 265 'c3Pe-1 f(r) = , fc(r) = C2 et+ fS(r) , C6 (P C5 = c8 , (D.13) C7+'C7+1 C4Pt+2 where q n represents Eq. (2.373). a Landau level wave function with the form given in Now k is an operator instead of an ordinary vector. If we A choose B to be along e , then Eq. (D.9) becomes 2 + ,+P2k2 3m 2 P2s 3m 2 E +A E 1 E 1 E + A (D.14) Three types of solutions exist [Yafet 66], corresponding to the cases fc ~ The fc ~ n first two cases n (D. 15) c~ ' apply when E 0 and the heavy-hole solutions which have E = 0 for all k . last case applies to the For the first two cases, multiplication of (D.9) by E and E + A gives E(E - where g )(E + A) ) -- k 22((E the upper sign applies applies to the second case (b-set). + p 2sA A) 3 = 3 to the first case 0 , (D.16) (a-set), and the lower sign Here s - eB 0/hc (D.17) k2 = (D.18) and s(2n + 1) + is evaluated for n = e for the a-set case, and n = +1 for the b-set. 266 The solutions of the two cubic equations give E(k) for the conduction, light-hole, and split-off bands. The multicomponent wave functions are found from 2x2 Pk .t E Pk - t f(r) = (D.19) E+A with the normalization condition <fc 1 3m k2 2 f3m 2 2 E I E P 2s( z 3m + E + A =1 E + A)fc Designating the a-set (spin-up) wave functions of band-index g., by IgnT>, with f1 a = c , we have NO a[( (Pn 0 VTi Pk /E IJl'> - 1 -~T2 PkI/E Na - Pk IE T PVMT 1 (Pn + 0 V N --VYT a /E Pk Pn/E 9, --PVs( £+1 )/3 IE Pn+ 1 ............................... I.............. P k / (E+A) ViT 3Pk VI/T Pk + /(E+A) PV/sCT+l) /3 / (E+A) (Pn / (E+A) Pn+l, (D.20) 267 Here p2k2 N2a =1+ 2 1 P2s P2 1 (E + A)2 3 E2 + E2 and g may be c, +, or s, corresponding split-off bands, respectively. 1 (D.21) (E + A)2 to the conduction, light-hole and (The subscript 'a' also applies to the energy E, but has been omitted to simplify the notation.) For the b-set (spin-down) wave functions with C 1 [ Nb n f and = n-l, we have 0 1 0 1 Ignj Nb Nb Pk /E 1 - V2 Pk /E Nb -V-i2 Pk /E I /6 113 -1i3s --v2/3- Pk Pn- 1 /E -PV s( n+1 ) / E Pn + PV'2sn3 / (E+A) Pk /(E+A) Pkk PVsn73 /E (E+A) 1 Pn- 1 -- vT7 Pk / (E+A) (pn (D.22) Here P k2 N2 b = 1 + 3 2 E + E2 1 P2s 1 (D.23) + (E + A) 2 268 3 (E + A) 2 where k 2 is evaluated for n = e + 1 . A special case exists when n=0. In this case the split-off band wave function IsOj> has an energy which equals -A at k =0 and is approximately I2ki/(2 -A- msI) for small k The energy . denominator E + A in the expression for the wave function then is proportional to k for this particular state. Normalization requires multiplication of all of the components by a factor which is proportional to k limit. in the small-k The largest components then are the m = I component in f , which is f, which is approximately (p for small k , and the m = proportional to k for small k . component in This wave function is therefore seen to be the first member of the a-set Landau ladder rather than the first member of the b-set. Its designation then is aS(O). Note that it differs from the other as(n) states in that it has a finite m =-I component in the conduction band. This component is zero for all the other states, which are pairwise degenerate with b-set states in the low-B 0, low-k limit. The heavy hole solutions have E = 0, and wave functions which are determined by f=f o (D.24) , and (D.25) (k-t)fv = 0 . 269 The a-set heavy hole wave functions are + k 2 + 3s 3k 1 (4k 2V3 k k ShnT> Na a 1 Pn-1 V'3 k2 N + + 2s(n+l)) 'Pn-1 2V96si krp a n 2sv3n(n+1 ) 9Pn+ 1 0 0 0 0 0 (D.26) with N 2 = (4k2 + 6s)(3k2 + k 2 + 3s) a (D.27) = [4k2 + 2s(4n + 1)][4k2 + 2s(n + 1)] Here k= s(2n + 1) + k2 has been evaluated for valid for n 2 1 . (D.28) n = e-1 . The state The expression for the wave functions is with labelling. 270 n = 1 is a-(2), using the standard The b-set heavy hole wave functions, with E = 0, are given by 0 0 0 0 0 0 v/3 k2 1 1 Ihnj> Nb - 2V 3k k_ k + k Nb 2sV3(e+1) pe-1 -2V6s( e+1) k Pe (4k' + 2st) 9+l - 3s 0 0 0 0 (D.29) with Nb = (4k2 -6s)(3k + k2 - 3s) , (D.30) = [4k2 + 2s(4n + 3)][4k + 2sn]. Here k2 = s(2n + 1)+ k has been evaluated for valid for n 2 -1 . labelling, and equals (D.31) n = e + 1. The state The expression for the wave functions is with n = -1 p u4 (m = - 2) for all k. The state with n = 0 is a+(0), which is actually in the a-set, not the b-set. This state differs from the other a-set heavy hole states in having a finite m = low-B , low-k limit the u5 (m = -) component is q component is proportional to kpl 271 using the standard is b+(0), 2 component. In the and the u4 (m=-) The Kane model result for B0 = 0, neglecting coupling to higher bands, is easily obtained from the finite-B0 results by making k+ and k numbers instead of operators, and replacing the Landau-level wave functions c(p by 1. For small values of n and f we make the following connections between the wave functions of the PB model [Pidgeon 66, Weiler 78, Luttinger 56] and those of the Yafet model. S= -2: b+(0) = h(-2)1> (E = 0) ; S= -1: a+(0) = h(- 1)j> bc(0) = c(-1)> , b+(1) L(-1)j> , (D.32a) (E = 0) , aS(0) = Is(-1)j> (E =-A at k = 0) ; e= 0: b-(2) = Ih(0)J> (D.32b) (E = 0) , bC(1) = Ic(0)1> , b+(2) = IL(0)>, bs(0) = Is(0)1> . aC(O) = Ic(0)'> a+(1) = IL(0)T> (Lowest cb level at k = 0) , (Highest light hole at k = 0) , aS(1) = Is(0)t> ; = 1: b-(3) = Ih(1)j> D.32c) (E = 0) bC(2) = Ic(1)1> , b+(3) = IL(1)> , bS(1) = js(1),> a-(2) = Ih(l)t> . (E = 0) , 272 aC(1) = Ic(1)IT> a+(2) = IL(1)T> , aS(1) = Is(1)t> . (D.32d) For small B the energies are determined by (E2)k2 g 3m 2 2 +___ P2s 1 G G + A g g 3m 2 & 2 P 2 k2 3m 2 3m 2 3m _ 2 g (D.33b) 1- 3m 2 + A g (D.33a) cb g S1 (E + A) - 0 1 32s g 1= . (D.33c) s-o + A g The wave functions and energies for small B and k =0 are: Conduction band: fc = (n aC(0) = ((P 0) for the a-set, and (0 9 ) for the b-set 0) a E = I = n+1 bc(0) =(0 (0n ) a-(n) = ( a 3Pn-2 Valence band: where a 3 = [3(n - 1)/(4n-3)] 3 a+(0) = ( 0 0 Po a5 Pn 5p9 a-(2) = ( (Po 0 0 5) mc (D.34a) 4gco ] Ig ho c= co (D.34b) 0 ) 5 e =-1 ) 92 c 1 /2 and a = - [n/(4n-3)] 0 ) a+(1) = ( 0 a+(2) = ( - 0 /2 0 Eb m E a =0 Ea 0 ) 0 ) S=1 e.= 1 273 Ea = Ea = 0 2 mL M+ 4 LCO L]hco (D.35) etc., where Valence band where b-(n) = ( 0 b6c n_ 0 b4pn ) b6 = [(n - 1)/(4n-1)] 1 /2 and b4 = - [3n/(4n-1)] 1/2 b+(0) = ( 0 b+(1) = ( 0 b+(2) = ( 0 b-(2) = ( 0 0 0 0) 0o - c 0 o0 0 p e =-2 E e=-0 Ebm [ b ) m m 'gh] gL CO co mL e=O 262 e=0 F)2 (D.36) etc. Split-off band aC(0) = ( 0 bc(O) = ( (P n fs= (0 (nn2 ) C) and e= ((pn 0 ) n+l E a = L2 m a 0) 2 m + I hI CO s] hO)C 4Sj (D.37) (D.37) Here the masses are determined from Eqs. (D.33). Note that the valence band wave functions are the same as those obtained from Luttinger's model with I= 272= 273 = 2K = 2P2/3 274 . Appendix E Magneto-optical Matrix Elements for Scattering and Absorption If H 1 is a small perturbation, the perturbed wave function is o (H)io p= o + E -E. (Pi + i o I Z (E.1) If V is a component of the velocity or the scattering operator, and V is the perturbation to V due to H then 0 1 <fl(V +V )Io> = < (f + E if (H). -E.o 1 I(V+Vl)I (o + S 1 E> E -E.J E-E. (Pi f I j0o o (H) if (Hf(V)ioo_io )Io + : (H) =(V E-E. if f > +... (V ) (H) E -E. I i#O 0 I (E.2) = (V)fo + [Vo,iS ]fo where (S l)jj = 0 , and I 11 i(Hd) E.-E -jk Jk (E.3) for jsk . This first order perturbation theory approach is valid for the cb but not the vb. We now consider some examples of absorption and scattering. (Example la) Let V = k lm*, and V = v We + then have1+ We then have 275 (H)f(k). [V0 , iS]f = S(l/m*) (k )f(H ).io E.-E Ef- E i = (l/m*) 1 E (k)fi(Hl)io (H) (k)io Eff (E 0 + ho)c = (l/m*) and (EF- haO) f c - E o (E.4) [H ,k ]fO H+fo fo- Use [k - ,k+ ]=2s O °c [H ,k ] 1 = +12s(8H8lak - ) = sv 1 to get [V , iSIfo = (V l+)fo ho)c ifo - hoc CE ho C fo _ C 0-0c (0-0) (V) . (E.5) fo C This implies a 'correction factor' of (3 (0 1+ (0-0 (0-0) (Note that (0=fo for absorption.) fo (Example ib) For V0 = k /m* (E.6) the correction factor is 0) 1- (E.7) C O + ) C (0+0) (Example lc) For V = k /m* 0 z (Example 2a) Let VWe= A , and then1 the correction factor is V = A ,with We then have 276 1 - 0 = 1. A 0 = ih6KSave (axb)+ (Ao)f(H) io E.-E 1 0 (Hl)f(Ao)io E -Ei (E.8) = [Ha_] iiKs(axb)+ [HI-f fo s For A = 2ih-Ks(axb)z (Example 2b) we get z [H ,z]fo (E.9) 2iiK (axb)z Ofo (Example 2c) For A 0 = ih iK S(axb)_a + we get [Ho] iOK (axb) [H +f s fo (E.10) In Example 2c consider the case of inversion asymmetry, with H( 8) = 80[oa(kkk - kkk)k 1 x yxy zxZ + c.p.] (E.11) 8 F [oa (k2 -5k 2 + s)k 00 + 2- -o(k 5k2 -s)k] + + . Then [H ,] since = 4Fo(k 1 00Z + 2 - 5k - s)k [_,+] = 2i[ [o,oy] =-4 -+xy + . . . (E.12) . (E.13) zz Note that E K = - (P/3)E [1/E 2 - 1/E'2] = 15.6 in InSb. gs g g 277 (E.14) We then obtain the result i[A ,S ]f = i6Ks(axb)0 0f s [H ,+]fo s fo (E.15) 1 icK (axb)= where F This treatment + -= 0.1443 parallels s [46 Foy(k 2 - 5k2 s)k 00 +f when B ll[111]. 0 that of Rashba and [Rashba 61a, Gopalan 85]. 278 Sheka, and of Gopalan et al. Appendix F Matrix Elements of exp(iq.r) for MD and EQ Transitions The matrix element of exp(iq.r) between Landau level wave functions is 8 (k+ q - k') e (k + qy - k') Z Z y KZ K <ezq-r p -iqx(k + k')/ 2s -q e Y / 4s M, n (F.1) where y_b -y+b_ e < n'j ee MMn n = (F.2) n>, with + = (qx + (F.3) iqy)/ v'Ts . This result corresponds to the gauge A = B0 xy and Landau Level wave functions A A A It was which are localized in the x direction, and extended along y and z. derived through the normal ordering of raising and obtained by application of the Baker-Hausdorf theorem. lowering operators, This theorem states that eA+B =e -[A,B]/2 eeA B (F.4) if the commutator [A,B] commutes with both A and B. The quantity M , may be expressed in terms of Laguerre polynomials [Bass and Levinson, 1966]. To first order in q, neglecting higher and lower orders, we have M , n n = < n' y_b+ - + y+b_ +- (F.5) n > 279 If we notice that (q x k) = (q k-qk +) (F.6) we see that interlevel effect of exp(iq.r) to first order in q is the same as that of (q x k)z eiq-r (F.7) to lowest order in q. A For q = qy , we have, by simple expansion, <' leiY = K(k ( + q - k') 8 K(k - k') < n' -iq(b + b_)/ v7- I n > (F.8) If we neglect q in the first Kronecker delta function, the result is the same as that of <w - iq(k + k_)/ 2s Ir> = <lI' - iqkx 280 s I> . (F.9) Appendix G Decoupling of the PB Hamiltonian We now consider the decoupling of the PB Hamiltonian to obtain effective Hamiltonians for the and conduction valence Decoupling bands. of the conduction and valence bands from other bands to order k2 is the basis of the usual effective-mass The resulting theory. effective Heft Hamiltonians are useful for computing optical and transport properties of electrons in a single band if hco and he c and E f c compared with g, as in are small compared to 8g. g the case of interband If hfo transitions, is not small it is still possible to use the decoupled wave functions to compute optical transitions as was done by Roth et al. [Roth 59]. For narrow-gap semiconductors like InSb, it is relatively easy to have experimental conditions in which the cyclotron energy hOc or the Fermi energy Ef is a sizable fraction of the energy gap, in which case the decoupled scheme becomes deficient. This is why the coupled models of [Kane 57, 66], [Yafet 59] and [Pidgeon 66] were developed. cases, the In these decoupled Hamiltonian is still useful for determining the optical and transport properties in the limit of small B or small E . Rashba and Sheka [Rashba 61b] considered Hef for the conduction band of InSb to order k3. those of the 8x8 They obtained the parameters of the decoupled model from Kane model, valence band blocks. neglecting the Luttinger parameters in the In particular, they found expressions for m/m*(E) and g*(E) as functions of P and 8g and A, and the expression for 80 as a function of C, C' and G (which they call K, Q and G). They incorrectly assumed C'= C. Ogg later obtained Hef to order k4 [Ogg 66], including warping as well as 281 inversion asymmetry terms, taking account of the tensor transformation properties of the operators and matrices occurring in the Hamiltonian. This approach was further generalized by [Braun 85]. The result of the decoupling equivalent to that obtained process described from ordinary perturbation by [Rashba 61b] theory is if one allows k-p to be a matrix (containing the spatial operator k) and takes care to make the result hermitian [see Braun 85]. To fourth order the Wigner-Brillouin perturbation theory (WBPT) expansion is E + V+ = Eo + V+ n n nn + V V nm mn + E - E0 n In V V V nm ml In 0 (En - E mIn ) ( En - E ) Vnm VmlV k Vkn E) (E - EOk )(E (En - Eo m n I n k (G.1) summed over man, l4n and k-n. The Rayleigh-Schr6dinger (RSPT) expansion is obtained by expanding (E -E m)Zn m with the result En = Eo + n 0 V + nn V Eo n E V V V Vnm Vml Vn (Eon - E m + V ) ( E n - m Vnm Vm n Vnn E) (Eon1 - Vnm VmlV 1k Vkn o) (Eo - Eo) (Eo - E ) (Eo n m n I n k 282 Em )2 Vnm Vmn Vnl V n (Eon - E m0 ) 2 n - Eo) (E n 1 (En - 1 V nV Vnm Eo n Eo) (E - Eo n m 1 E o m V V (E Eo - Eo l n o n (Vn n 2 - )3 E m (G.2) summed over man, ln, ken. degenerate. Here we have assumed that all levels are non- When degeneracy exists the expression becomes a hermitian matrix which is an effective Hamiltonian for the degenerate subspace. ordering The correct of the matrices within the expression requires an analysis like that of [Luttinger 55], [see also Kjeldaas 57 and Yafet 63], which uses successive unitary transformations. The result is Hn = Eon + Vnn + V V nm V + VV V lnmIn 9 nm &nl V V +VVV nm mn nn nn nm mn 29 2 nm VVnmVlml V lkV kn V V VV Vnmmn Vl In nm nl nk 2nm nl nn nm mil n n Im mn nn 2nm nl + 1 1 nm nl i nm V V V V nn nm mn nn nl (G.3) 3 nm summed over man, ln, k-n, with 8nm - Eon - Eo m (G.4) 283 This result contains some fourth-order [Braun 85], given by terms which are and do not contribute additional to those to order k4 to the decoupled conduction band Hamiltonian. When time derivation of described by dependent Heff requires [Foldy 50] Bjorken 64.] fields the and use potentials of for the case i(V -V V conduction electric V i( nm mn - Vnm mn n2 2 nm to the correct transformations as [See also The correction to the above result due to time dependence of the summed over men. respect time-dependent present, of the Dirac equation. perturbing fields, to third order in h2k2/2mg H Hn are and hOo0 g, is ) (G.5) (G.5) The dots over the V's stand for partial derivative with time. This electrons proportional term gives to rise the to a transverse spin-orbit part of interaction the for perturbing field. The largest part of the decoupled conduction band Hamiltonian Hc may be obtained by considering the spherical Yafet model in which terms quadratic in k are neglected in the effective 8x8 Hamiltonian [Yafet 59, 66]. The PB Hamiltonian then reduces to [see Rashba 61b, and Kim 89] H = S g C C" Ct 0 0 C. 0 -A (G.6) 284 with and C = Pk.t C' - Pk.t' . (G.7) The partial derivatives where t and t' are defined in Eqs. (x.xx) and (x.xx). of C and C' with respect to time are C = P e At = -PeE T -t (G.8) C and C'= peC A-t' = -PeE T (G.9) t' where ET is the transverse part of the perturbing electric field. To fourth order in perturbation theory we find cct H =g1 c g 2x2 + C'c' + g g (CC ) 2 3 (C'C't) 2 h.c . h + +2 ( + A) g C-hc. h.c. + + ---- g gg g +- 1 1 - + + g CC' + CCtC'C't + 2 (G.10) which we will evaluate below. We have included fourth order time-dependent terms not given by Eq. (G.5), and have assumed that the perturbing field is transverse, i.e. (p(r,t) = 0. 285 The most general expression for H for the 6 conduction and the s split-off bands, obtained by the method of invariants [Ogg 66, McCombe 69, Braun 85] to fourth order in perturbation theory, is [Barticevic 87] H eff = H +H + H 0 1 (G. 11) 2 with 2 k H =2m* + 2m tgBo.a - eo(r) , H1 = 8 [x (k kk - kk k)+ 0 X YXY zxz + e0 + (G.12) 2 k4 + ( [{ k2,k2 B c.p.] + c.p.] + g jo -B k2 + 2g".B(.k)(B .k) + YoL [oxBk + c.p.] , (G.13) and H2 = eKSaExk + eKD V-E + e2KE E 2 + eK[E {k ,k ) + c.p.] . (G.14) The terms in H are the kinetic energy and the electron spin contribution to the Zeeman energy. The term in H 1 involving 86 is anisotropic. symmetry and is odd with respect to inversion [Rashba 61a and 61b]. in HI proportional symmetry. to ao and Yo are anisotropic These are even with respect to inversion. 286 warping It has Td The terms terms with Oh The remaining terms in H possess spherical symmetry. not considered interaction term in the proportional proportional H contains terms which depend on E and were above references. These include the to a-Exk, the Darwin term proportional to the electric energy density at the spin-orbit to V-E, a position of the electron [Wolff 66, Eq. (5)], and an anisotropic term with Td symmetry which is independent of spin. Note that Exk must be symmetrized when components of E and k fail to commute, and that a small term proportional to E (a B +B ) + x yz zy c.p. has been omitted. If we consider the Yafet model in which the 1C, 6 FV and Tv7 interact only 8 via the momentum matrix element P [Yafet 59, 66], then Hc for c is spherical and may be expressed as [Rashba 61b] H = k2 g + + S2m*(E) o(E) BBo. , (G.15) with m 2P2 3 3 m m* ( E) 2 E + 1 + E + A (G.16) and 4P2 1 1 and with E measured from the top of the t Eqs. (G.12) (G. 17) , g 0(E) =- and (G.13) may be obtained v valence band. The coefficients of by evaluating Eq. (G.10), or by replacing E in Eqs. (G.16) and (G.17) by He and expanding about 9g [Kim 89]. The coefficients of Eq. (G.14) must be obtained by evaluating Eq. (G.10). results are: 287 The m* = m*(g) , o( g) ' go 1 d(m *) E o (G. 18a) (G. 18b) -2 - 8 dE 1 dg (G.18c) E=9 2 dE (G.18d) E=E- 1 d(g / m*) 4 dE (G.18e) E=g g 1 dg P2 4 dE E=6 3 K s g G2 4 P2 K dE (&g+ A)2 g 1 d(m / m*) KD D (G.18f) 1 E=g g P2 2 6 G2 (G.18g) g (Eg+ A)2] 2 (+ ) ] (G.18h) 8o = CC=yo = g" = K A = 0 . (G.18i) E 3 3 The coefficient K D is evaluated by assuming that a finite perturbing potential (p(r,t) exists so that the matrices V , V and V Vcc = V = - ep(r,t)12x2 CCSS2x2 satisfy (G.19) and 288 V= - eqp(r,t)14 (G.20) are considered in Eq. (G.3). The parameter g" is zero for the conduction band in the Yafet approximation, but is finite in the Hamiltonian for the split-off band Tv7 . It becomes finite for the conduction-band Hamiltonian if we include terms proportional to k2 in the decoupling. inversion 'v x Fv block of the PB Hamiltonian before The parameter 80 becomes finite for the conduction band when asymmetry terms in the PB model are taken into Rashba 61b]. The parameters a terms in the PB Hamiltonian. account [see and yo become finite as a result of warping The present approximation to Hc , obtained from the Yafet model, may be compared with that obtained by Wolff using the "two-band" model [Wolff 66]. The latter model may be obtained from the present one by dropping the terms which have & by itself in the denominator, and replacing g + A in the remaining denominators by g. g g We will now obtain expressions for 80, a(0 and yo based on the PB model. The expressions anisotropic are important conduction-band c(0 (G,N) + h.c. + g Hcv(P) H parameters determine in the low-field limit, the for a Starting with 8 we have [compare Rashba 61b] o) + these magnetoabsorption model which is easy to compute. Hc (P) H because Hc(P') Hs(G') + h.c. g HCV(P) Hv(C') Hc (P') + h.c. (C) HVC(P) + g(9 gg @2 g + A) (G.21) 289 As an example of how this can be evaluated, consider H (P) Hv(G) = -iPG[k.t][{k,k }t + c.p.] -iPG[k k k }t tt + k {k ,kt tt x z xy x y z xx + k k k }ttt + c.p.]. y y z yx This after evaluation of is simplified the matrix products. (G.22) The complete expression which is obtained for 60 is 8 = 8 (G,G') + 56(N0 0 0 2 ) (G.23) + 56(C,C'), 0 with 4 GP G' P' (G.24) 6 (G,G') = 3 9+ g g N P = -2v"2 6o(N) 0 2 (G.25) 2 & P 2C'P' CP S0(C,C') = (G.26) + g g g A similar analysis for o and yo begins with 290 Hc(ao, o ) = Hcv ( P ) Hvv (,q) H c(P) Hsc(P') + h.c. Hcv(P) Hvs (') g ( g+ A) gP 2 'P' gg (G.27) The result is 2P a = - Qo(R,4') + g (G.28) g g and (G.29) o =Y(R,R') + Yo(q) , with 12P 7o(g4,') = 'P' gP (G.30) _ g g g qP 2 (G.31) yo(q) = 3 g 291 Appendix H Effective Scattering Operator to Order k2 This operator appendix Ascat deals which with the derivation describes the limiting of an behavior effective scattering of scattering the amplitude Afo at small values of magnetic field B 0 and momentum k z along the field. The operator is obtained as a power series expansion in the kinetic momentum k, and acts between initial and final wave functions Io> and If> in the decoupled representation. The approach is especially useful for scattering from conduction band (cb) electrons because the effects of anisotropy are small and can be treated by first-order perturbation theory. be applied to valence band (=3 less accurate. (Accurate The same approach may vb or j=- sb) electrons, but the results are results require diagonalization of large matrices. See [Evtuhov 62].) Two methods are used. Both make use of invariant expansions and techniques of matrix and tensor algebra. (1) The first method is [Wolff 66]. conduction This band, a generalization approach including starts terms of the approach used by with the decoupled Hamiltonian containing the electric field obtains an operator Ac which describes intra-cb light scattering Wolff for the E(r,t), and in the limit where the incident photon energy is small compared to the valence to conduction band energy gap, ho1<<Eg. (2) The second method is based on the approach used by Yafet and Makarov [Yafet 66, Makarov 68]. It starts with the coupled-band effective Hamiltonian of Pidgeon and Brown [Pidgeon 66, 69] as formulated by Weiler and Trebin [Weiler 78, Trebin 79], and uses a k-p expansion of the multicomponent wave functions for the initial, final and intermediate 293 states. The scattering operator which results is valid for all values of the incident photon energy below Eg, but gives useful results for Afo only if the Raman transition energy is less than (Eg - ho). H.1 Computation of AC from decoupled conduction band Hamiltonian H C Here we start with the decoupled cb Hamiltonian computed from fourth-order k-p perturbation theory [Ogg 66, Braun 85, Barticevic 87], with electric field- dependent terms which result from the Luttinger-Kohn transformation [Foldy 50, Luttinger 55, Blount 62, Yafet 63, Rashba 91] 2 H - 2m + 1g*g B - + eK E (kx) + E k4 + g'gk 2B ' G + 2of3ZB2 + 2g"g K(2) (Bo)(2) + Iea 2{k 2,(E kx() } + bg E. kxB o [kkBY]() + eK[(Exk)kk](4) + eK[Ekk(ko) K (4)+ - + eK [Ekk](3) + egK [EB](3) + 6 [K()(3) (H.1) The term proportional to g" has been modified so that it has no overlap with the term involving g', and the anisotropic been made irreducible. terms in the last two lines have I have omitted terms of order E2 and higher, which produce terms of order 0 2 and higher in the effective scattering operator. The second-order k-p parameters m/m* and g*, computed from the PB model, are m - 2P2[2+ 1 + 2F 4P2I- -__ 1, (H.2) +2 - + 4N1 H3 294 K The The spin-orbit parameter Ks is E'-Eg+A. where P2 1 dg* _ 4 dE, s 1 3 1 2 E L C crystal) (isotropic axial-model fourth-order (H.4) E'2 parameters E' g' and P ,' computed from the Yafet model, are m d P4 _ 2 8 dEg m* 0 1 + 1 1 2 E' 2 4 9 E3 _ 2P 4 S1 d g* go 4 dE, m* 1 dEg 6 P a2 9 E' Eg E3 12 b 2 = 18 E144 1 9 E, E3E' 8 Ea2E' t, + (H.6) E E'2 Er2E' E' + 1 1 1 4P4 )2 -d (H.5) E'2 E2 (H.7) E2 7 3] + 3 EE'2 E'3 8 + E'12 E2E'2 3 (H.8) (H.9) E'14 The fourth-order axial-model parameter g" computed from the PB model is given by g S- P2 3 1 Kl P2Y E'2 Eg2 + 6E, Eg The fourth-order warping parameters E' 6 2 Eg EE' E'2 (H.10) o and y o, computed from the PB model, are given by = o( ,0') 2P E 2 E,- 22Wlp' EL+ , (H.11) 295 o(,) 2P = - (H.12) , (H.13) 2 y(q) = 3 P Eg2q The third-order inversion-asymmetry parameter 56 computed from the PB model is the sum of terms given by G, G') 3 , Eg (H.14) E' PN 80(N 2 ) = - 2V2 S(C, C') - E , (H.15) + (H. 16) I have assumed that P'=P for simplicity, where P' and P are the momentum parameters in the H and H blocks of the PB Hamiltonian, respectively. This may be corrected by replacing P by P' in a term wherever E' appears in place of Eg. Similar expressions exist for K and K4 , which are not important here. We next use first and second order perturbation theory to compute A c to order k4 . First-order perturbation theory: Replace k=p+-A 0 in H by k+eA, where A represents the perturbing fields at the incident frequency Co A 2 and EA. and scattered frequency 0o2. Then collect terms of order (Alternatively use the "polarization" of Hc obtained by applying the operator A-Vk once or twice [Weyl 46, Edmonds 74].) Thus 296 ---- (elc)2A 2 E -(kx) - (e2 /c)E -(Axo) = k4 - (e/c)2 [2A2k2 + 4(A.k) 2] = (elc) 2[LA2k2 + 4A(2) K(2) (e/c) 2 (A-B)(A-o) = (elc)2[A2(B-o) + A(2).(Bo) (k.B)(k.a) (e2/c)(ExA) -a etcetera. (2 ) (H.17) Next make the replacements A A 2A2 (e/c)2A2 - 2(el e*) (e/c)2A (2) - 2(e e)(2) 1 2 (e2/c)(ExA) 2i (e 2/c)(EA) , i(O - e e2 The bilinear expressions may also be written as (ere )(EA)). where 0 - (1/2)(01+02). (e2/c)(EA. I ] (H.18) (elxe*) --- The bilinear expressions may also be written as i( 01.2)(e .e2 +e .e ). .A J i) 11 2] Notice that the factor (co - 0 2) 1J 21 in the symmetric proportional to the Raman transition energy ef, product of E with A is which is of order k 2 (or Bo0) for intraband transitions. Results of first-order perturbation theory in A 2 and EA: Ac(m*) = (m/m*)(e,1 e*)l 20 A (K ) Ac ( o) 2iCK (elxe*) -a = 28[(e -e)k 2 + 4(e e*)(2)-K(2) (H.19) Ac(g') = (e/c)g'(e e2*)(a.B) Ac(g") Ar A ) + A )(2) 2(e/c)g"[(e )(02 -B I-[4k - {k,o.k} Ac(a 2) = ioa2(e 1xe*) 2 p (e xe*) -B Ac(b 2) = 2iwb2B I 2 0 297 0(2) Anisotropic terms (using a-e and b-e*): Ac(ao) = - 12a[abkk](4) Ac(y o) = (e/c)[yoabBo]( 4 ) Ac(K 1) = 4i0K [(axb)kk ](c) + o(k4) (H.20) Ac(K ) = - i@K2 [(axb)kkoa](4 + o(k4 ) A (8o) = 280[(axb - ayby)kzY = -(axb + ayb)(kxo) + c.p.] 238 [[(ab)(2)(ko)(2)](3' + i[(ab)(2)(kxo)](3)] - I have neglected the contributions of K and K which are of order k 3, due to the factor computed, ( in 1 - 02). analogy Additional to contributions the case due of anisotropic similarly for the contribution due to g".) to i[Aco,S 1] magnetoabsorption. must be (And The factor of i in the last term of Ac(8) occurs because (kxo) =(il2)(k a_ - k_ ). Second order perturbation theory in (e/m*c)(A-k) + eK E -(kxa): In the second-order terms in Ascat, make the replacements A e1 v A - A e*-v -2 e [(k/m*) + io K (kxo) , (H.21) A e* -[(k/m*) - i) K (kxo)] 2 Neglect Ero and E 2 S in the energy denominators, relative to hw 1 or h'c 2, since the intra-cb energy differences are of order k 2. With these approximations we have 1 A ^ ^ Ac(2nd order p.t.) - - 1^ (e*.v)(e *v) - (e -v)(e* -v) . 298 (H.22) Use the following expressions to simplify the results, where R-kx: (0) a. = 3(1) (1) Cyxo = 2io (1) kxk = - i(ec)Bo (0) k-R - R-k = - 2i(elc)(B- 0) (H.23) k-R + R-k = 0 (1) kxR - Rxk = {(k-&),k} - 20k2 (H.24) kxR + Rxk = -i(e/c)(B xy) (2) [kR] ( 2 ) - [Rk](2)= i(e/c)[BG](2) ( 2) [kR] (2 1 + [Rk](2) = - 26i[K(2)C] (0) RR = 2k 2 1 (1) RxR = i[{(k-&),k} - (e/c)Bo0y] (2) [RR](2) = - K(2)1, + (elc)(B - + y) (elc)[B0 (H.25) ](2) The number in parentheses specifies the tensor rank of each expression. Note that a factor of the Bohr radius squared (a0 ) must be restored to give R dimensions of length. Second-order perturbation theory results, to order k 2: A (2nd order p.t.) = (i/o)(e/c)(m/m*)2 (elxe*) Bol + 2(elc)(mlm*)K[(2/3)(e . e*)(Bo) S - + iK(e A 1 A 2 0 e*) - [(e/c)B ol - {k,k-}] S 1 2 0 G 299 - (e e*)( 2). (B 1 2 0 )(2)] (H.26) Summary of first and second-order perturbation theory axial terms (see Table (H.1)): C = (m/m*)(e 1 .e*)1 2 + (a)(e e*)k21 1 A A A A A 2 + 2ioKS1(e xe*) -a 2 G + i(b) (e xe*) -B 1 Cl 2 0 + (c)(e e*)( 2). K(2)l 12 + (d) -(e .e*)(.B) - i(e)(e xe*). k2 - i(f)(e 12xe*).{k, -k} C + (g) 1 2 1 0 e(ele*)(2 ). (B 0 2 (2) (H.27) where (a) = (20/3)E (b) = (1/l)(m/m*)2 + C(K2 + 2b) (c) = 8 ° (H.28) (d) = (4/3)(m/m*)K + g' + (2/3)g" (e) = - 4ca (f) = 2 (KS + a2) 2 (g) = - 2(m/m*)K s + 2g" If ) in the zero-order term is replaced by co then an additional term occurs to order k2: eA A (h) (exe*) -(xB) , (H.29) (h) = (1/2)g*K (H.30) with . 300 Table H.1 Contribution of axial terms in the decoupled cb Hamiltonian Hc to the scattering amplitude operator Ac . Component of A c Terms in Hc (2nd order) Term in He (1st order) 0 (m/m*)A2 1 0 KS ExA o Co 0 E (A-k)2 (e 1 e ) A A - i(elxe*) c 1 2 ^A (a) (el1 e*)k 2 A 2 A m 2 0 A.k), Ks(E R) A (d) (e .e2)(B o.) A A (e) - i(e xe*)ok A {k,k-a} (e A )(2) - (B )(2) eo(A k) 2 1 'A2 (Bo.) 1 and H(g") o Ks(E-R), Ks(E-R) a2(A -k)(E R) Co -(A k), Ks(E R) A R O a2 (A-k)(E-R) 2g"A ( 2) (B 1 (2) 1 KExA- a 0 (h) (e xe*). (Boxo) where b2 ExA -BB 0 A (f) -i(elxe*) (g) 2 /o 0 A k) Ks(E-R), Ks(E -R) Ae)(2). K(2) 1 0 k), m(A -- (A k), (b) i(exe) -B (c) ( n a2Okxo , and a 0 is the Bohr radius. The anisotropic terms in Ac are given in Eqs.(H.20). There are contributions from second-order perturbation theory to lowest order in k. The part of A c which contributes to [Ac, iS1], to lowest order in k, is SA A - (H.31) A = 2ioK (e xe*)). S 1 2 0 301 In order to evaluate [Ao,iS]fo 0 fo one may use the relations H ]fo [a+,iS fo = [O E +hw fo s ,islfo .J [,iSlfo [[ H ]fo E - n1 fo (H.32) [a ,H]fo E Efo These are computed from first-order perturbation theory in H 1, the anisotropic part of the decoupled cb Hamiltonian. 302 H.2 Computation of A scat for finite hoI 1 from coupled Pidgeon and Brown Hamiltonian To find the effective scattering operator, we proceed by first expanding the multiband wave function for each band in a k-p expansion applied to the The multiband effective Hamiltonian is then used to decoupled wave function. If the PB model evaluate optical matrix elements between the different bands. is used, we have A m 2 tv)fr( e CV > ro [(Y (f *-v e =4m A fo 2 - Ofr 2 2 E fr hO) ro I r The V hW -E r) o (e*.v)_1 (eVfr + (e Vk)(e2 *-V ef 1k 2 k)Heff evaluation of A scat to zero order in k is (H.33) to the simple relative A higher-order The cases. operator occurs in sums the over A A A which e v, intermediate levels with e replaced by e or e*, is given by 0 e- v = (l/m) A A e'pcv e*pcs . 0 (H.34) .Pv 0 0 SPsc The momentum matrices are pc It is = Pvc= Pt Pt usual approximation to set Ps is P'=P, which [Weiler 78]. The P P' 2x4 = consistent matrices t , (H.35) P't'. with the 'single-group' ty and t z are given t'y and t'z are given by t' = (1/V3)p Appendix A, and the 2x2 matrices t', x where px in , Py and pz are numerically equal to the Pauli spin matrices, but the vector p is polar instead of axial [Trebin 79]. The zero-order (in k) initial and 303 final wave functions for intra-cb scattering are FcoI V = c [O and , [v] (H.36) where co and XCf are the decoupled initial and final state wave functions, Oc and Os are 2-components zero vectors (or 'spinors'), and 0v is the 4-component zero vector. The intermediate states in the light-hole heavy-hole valence band (vb) and split-off valence band (sb) are r = Xv Os (H.37) Ov r and , Xsr We substitute these wave functions into Eq. (H.33) for A The sum over intermediate states is accomplished by neglecting the k-dependence (or B and k dependence) of the energy denominators, and using the completeness relations for the two-component and four-component wave functions in the intermediate A bands. A We find, neglecting (e Vk)(e2 V )Hef , A fo = (1/m) <XC c C() x(1 NO - E 2I OI -E 2 X > -CO I (H.38) where o may be w , (02 or an average, since the difference is of order k 2 . operator part of this expression, The which acts between XCf and Xco, may be written as A c P m + fr hO - Eg ro 2 fr( I h + E, P2 2 m (e*-_t' fe t')fr( he + ')r ' I (e - t')fr( ro e*') 30hO - E' 304 ')ro 1 (H.39) This may be simplified by using the algebra of the t. and t' matrices (Appendix A), along with the recoupling identity (a.p)(b.q) = (1/3)(a-b)(p-q) + (1/2)(axb).(pxq) + (ab)(2).(pq ) , (H.40) which is valid if the components of a and b are ordinary numbers, or more generally if the components of b commute with those of p. After simplification, and inclusion of (e- V )(e* -V )H, we obtain I k 2 k CC A= 2F+ 3--m+ () + El 92(w) el'e 1o 11 - iho- where and E' (0) Eg+A. used by Makarov 9 ((o)=l 1 (PE(o) - 2E'22 ( Eg 2 (o) (ho))2 - a xe) . E2and - 2 () (H.41) 2 (H.42) The definition of the resonant function (p2(o) differs from that [Makarov 68]. and (p2(o)= when -=0. I have defined the functions The constant (1+2F) associated with free mass and higher-band terms in H [Weiler 78, Trebin 79]. so that both in the first term is of the extended PB model When co-)0 we obtain A c = (m/m*)(e.e*) 1 + 2ioK(e xe*) X as was obtained previously from the decoupled Hamiltonian He. 305 (H.43) A scat to second order in k: We now consider the second-order dependence of Ac on k. For this we must compute the k2 dependence of the wave functions, interaction Hamiltonian and energies, and must include conduction-band as well as valence band intermediate states. F wave-functions: 6 12 1 KK cv vc E2 2 K 1 KK cs sc E'2 vc (H.44) Eg K sc E' F8 wave-functions: F7 wave-functions: KKcv K cs E' K K VC xv CS E'A K K SC CV EgA 1 2 306 sc cs E "2 xss (H.45) Here, K Pt -k, K P't'-k, K Pt k, K -P't'-k , (H.46) and we again assume P'=P. Next use these wave functions to compute the optical matrix elements of the A -v optical interaction and substitute into the expression for Afo Additional dependence of A on k comes from the energy denominators in This dependence becomes much stronger, near resonance, the expression for Af. than the dependence of the wave function components on k. In evaluating A we must consider terms like AB fr ro hO) - E 1 ro and AB fr ro ho - E 1 fr (H.47) These may be expanded to order k 2 as follows. First we write the denominators in the more symmetrical form hO -E ro = h + E + E - E r 2f 20 (H.48) ho -E - (E 2f (H.49) So and fr = h + 2 0 Er) . We then separate each energy on the right into a band-edge energy plus an energy relative to the band edge. The latter energy will be obtained allowing the decoupled Hamiltonian to act on a decoupled wave function. the case of initial and final states in the cb and intermediate vb, we write 307 by For states in the (hf 1 - Ero) =(h + Eg + EC + E - E (H.50) , where the superscripts c and v indicate that the energies respect to the band edges. We then expand the right hand side in powers of (Ec + Eo Er)/(h(i + Eg), (It a term also contains considered.) noting that the numerator is of order k2 and higher. of order k if the linear-k term in the vb is To first order in the k-dependent energies we have (hI- E ) 1 are measured with ro = 1 hw + Eg 2f + +1Ec +Ec 2 0 fr ro r (H.51) + Eg) 2 (h Next we multiply this by A B - Ev and sum over intermediate states r in the valence band. In doing this, we make the replacements c = Ho co = Hccf ' ErXcr = HvXcr (H.52) where the expressions on the right involve the decoupled Hamiltonians and wave functions. Note that SAfBro (H.53) r depends on k because of the k -p expansion of the multiband wave functions, and that AfrBr(Ec + Eo - E ) (H.54) r depends on k because of the k-dependence of the energies. To lowest order in k, for r in the vb, and neglecting the k-dependence of the wave functions, we have A B fr (Ec + E c ro f o E) = <X r cf 2 HA C CV B VC + !A 2 B H -A CV VC C CV H B] V VC I > r (H.55) 308 Here A cv - P(a t) , A A A (H.56) P(b.tt) B VC an d A where a and b are e 1 and e*2 or e*2 and e 1 A B ro 'f A similar evaluation is used for h(o -E fr r To second order in k we find A scat 1 2P2 2 3m Eg - ihO E( 3m A ( ^^ 2 ) (e *•e*2 2 1 i-p2 Eg 2 A eA A A2) 2 + i(b)(e xe .B + (c)(e e )(2) K(2) + (a)(e -e*)k 0012 2 1 1 2C After the A- + (d) eA + (g) £(e e*)(2). (e e* )( C 12 traditional A A B ) - i(e)(e xe*) 2 A A k - i(f)(e xe*) -{k, (H.57) k} (2) 0 "straightforward but tedious" algebraic manipulations, using h=m=l and E-E', I have found the coefficients [compare Makarov 68] 309 (a) (a) 7 20 4P4 9 +I]i+ 3+ ] 2 3E,2 t (H.58) 7 5 92 + 3EE 3E E 8 4P4 (c) 9 1+ + .0t +- E 14 4 (d) 2P 4 9 L .3ECa 2 3 02 2 5 E, E, i2 + Eg 4 3E A 3EgE 1 2022 [ g+ + - + - E E4 2 3 (P2 E A E2 2 4 1 E Eg4 3E, (H.59) 2 (H.60) + [1 E2 (g) = 2P4 9 (b) - m (0 (m*)2 + 4 3EA i +2+ 0 + 1-E291 E,5 4 + -1 E E 1 7 3EE 2 P4 9 +6 9 EE E2 2 + 2 (P E 12 E, 2 + 2 E, 3E2 E 5 2 + 1 r22 3E E4 92 Eg E 2 E2 Eg 2 E 6 4 E E 922] (H.61) 2 (p 1 (H.62) + f2 E2 6 EE 2 (P2 EAI E 310 4 9221 E E3J 2P4 (e) = - 3 4 L Eg2 9 1 EgEEgA + 8 Eg 1 9 + E2 JEg2 - 2 P12 -EJE 3 (H.63) P4 (f)0= 1 9[ g + 5 E 1 + 2 2 2 3 E92 EgE 3( 1 3 AEg 6 PP EA 912 Eg4 42+4 4 (p22 E E3 E 1 2 3P2 - + -+ Eg E AE 3 (H.64) In the coefficients, o may be taken to be CoI or @, since the difference affects terms of order k4 and higher in A c. If 5 is replaced by Co in the zero-order it introduces an extra term of order k2. This term is part of A e A (h) -(e xe*) -(xB) Cl 1 2 (H.65) 0 where (h) = - g* 3)- 2E'2 Eg4 ( I ()2() - E'4(P2] (0) (H.66) (H.66) with g* = 4P2 I I 3m E E' (H.67) . Use of coI instead of 5 avoids the complication of the dependence of 6 on B 0, at the expense of an extra term in A c to order k2. In the limit of small expression for (h) approaches that of Eq.(H.30). 311 Co the For the anisotropic nonaxial part of A to order k 2 in the PB model, one must consider four contributions to the anisotropic part of Ascat 1) Anisotropic component of v in 2nd order terms. 2) Anisotropic component of energy in denominators of 2nd order terms. 3) Anisotropic component of VkVkHeff in 1st order term. 4) Anisotropic component of multicomponent wave functions. The warping contribution to A scat for conduction electrons due to H (g) and Hvs(g' ) to first order in g and g' has the form c ()[abkk] + c (co)(e/c)[abBoa]4) + ic (o)[(axb)kkoa (4) (4) (H.68) In the off-resonance, small-o limit, one finds = 24 I P 2-g 1 + 2 E E E' - = 12 , c = 4 P2 3 Eg Eg2 (H.69) 1 EgE' 3] E'2J This may be compared to the result obtained from the decoupled cb Hamiltonian H to order k2: C Ac(warping) = - 120o[abkk]( 4 )1 + (elc)o[abBo](4) + ico(4K - K )[(axb)kko]] 4) The parameters ao (H.70) and o of the decoupled model are expressed in terms of g, and q in Appendix G. 312 ' The inversion asymmetry contribution to Aset due to H (G), H (G'), H (C') and the smaller components HCv(N2) and H v(C), to first order in the parameters, has the form d ()[(axbx - ayb )k + c.p.] + d2()[(axby z In the off-resonance, small-o, limit one finds + ab )(kxc)) + c.p.] (H.71) d= -d = 28 , so A sct(asym.) = 28~[((abx - ab )kz a + c.p.) satam xx y yz - ((ab +ab )(kx) + c.p.) (H.72) The parameter 8 of the decoupled model is expressed in terms of G, G', C, C' and N in Appendix G. Light scattering from holes: The scattering from free carriers in the valence bands may be approached in the same fashion as Auyang 72,74] conduction band. light scattering from carriers in the cb. [See To order ko we only need to consider intermediate states in the For scattering within the j=3/2 valence band to order ko obtain both At0O and A~-2 Raman transitions at kz=0, which include we spin-flip, spin conserving, and heavy to light or light to heavy hole transitions. This contrasts with the case of scattering from electrons, in which the A-=2 Raman processes occurred only to order k2 and higher, and n is an approximately good quantum number. We also find scattering which produces between the two spin-split valence bands [Auyang 72,74]. 313 Raman transitions For scattering from holes in the A v = (e*-v) 2 (l/m) L * (e v) (e* -v) I cV VCr I vb, we find j=3/2 VU (e* -v) O 2 + (el'Vk)(e* Vk)H I ho + E W hco -E k 2 k VV Ecv in in cb (H.73) which simplifies to v A2 3 3m E j 0 + ( AA)(2) J(2) - ) ( 1 2P 2 1 + ihO 3m g 2 P 3m Eg2 t(e e)1 J + 2(ele2 . A 2 J ) (AA (E el e 2J) 1 2 ) (2) j(2) (H.74) - (2)(2 ) (2) (4) 4 Here [Littler 83] 2P2 3mE,, 32.9 g = 0.55 . y = 0.46, y, = 3.25 , The last three terms in A v , obtained from the PB model, are nonresonant. (H.75) In a more exact treatment they would contain resonances at interband energies higher than Eg and E'. For o -~O we obtain AV IL (e -e*) 1 2 - + 2(e e) )(2)2P(2) + ii L 1 2 4(e 12 )(2) (2) (4) C 2 3mEg g ( 1 J) 2 (H.76) , which may be obtained from the decoupled Hamiltonian H if an effective spinorbit term (P 2/3mE2)(eE.kxJ) is included. 314 Here YIL =(2P2 /3mEg) + YI (H.77) YL (P 2/3mE,) It is significant + . that spin-orbit interaction terms, proportional to E in the PB Hamiltonian and the completely decoupled Hamiltonians, contribute negligibly to the transition energy of bound amplitudes. states but contribute significantly (But see [Jusserand 95] for case of asymmetric quantum wells.) spin-orbit of large Additional theory [Evtuhov 62]. i[A , S1]. matrices, the Note that the contribution of the warping scattering results from warping on the decoupled valence band wave functions. diagonalization optical effects in parameter g. to the scattering amplitude is of order ko, but that smaller than y7 L and YL. to and cannot be . is much the effect of This requires the computed by perturbation So the contribution cannot be expressed in the form Approximate results may be obtained by considering pairs of axial model levels which interact strongly via the warping terms in H v [Pidgeon 69]. For initial states in the sb, final states in the vb, and intermediate states in the cb we find ( vs = (l V)v(e v) v)cs (e *-v) (e* -v)s ho - E- hCo + E 1 )(eV k 2 k)Hvs in cb (H.78) which simplifies to 315 p2 AvS -3m 1 1 hC -E' - ho,+ EgJ iP2 (2),.U G,(2) 2 AA 11 i2hm 1 + 1 (exe* -u ) 2 hao)+ E 2v4m hl - E' 2V3( ee( - 2 ). (UTG)(2) + [( 4v (H.79) A*)(2)®(U)(2) (4) This may also be expressed in the form (less convenient for computation) -2 2p2 2P As vsmE + 4 ~[(A (e e1 2 )(2)u + 2 3() 1 AA ^ u) 2 + VmE E -(C) e 1xe* 2 2)((U()(2)( (H.80) where (setting h=1), Tp() (H.81) , = with o2 + 1 2 )C0= 1 + 2 (H.82) A , and E= 2 (E'+Eg) = Eg + '. 2 (H.83) Two-photon absorption operators may be found in an identical fashion. The operator Avc for two-photon interband transitions between first order in k (to lowest order). the vb and cb is The one-photon transitions are of order ko (= 1). 316 ACKNOWLEDGEMENTS I am grateful to Prof. Don Heiman, now at Northeastern University, for being the kind of advisor I wanted to deserve. He has, in fact, been much better than anyone deserves. Perhaps I could have finished this work without him, but I can't quite imagine how. I appreciate his example of organization and hard work, his appreciation of things both physics and non-physics (most significantly art), for his caring, his time, and his determination that I should finish this thesis. I am grateful to Dr. Hector Jim6nez-Gonzilez for being a positive influence over the past ten years. His cheerfulness, and eloquence, and enthusiasm for life and for science have been uplifting, and have often pulled me up from depression. He has been a great help to me in discussions of magneto-optics, and in setting up the experiment on the field-reversal effect. I appreciate his sharing his family with me, many good times, and much good advice, scientific and otherwise. I am grateful to Margaret O'Meara for her friendship, advice, and helping to keep things at MIT in perspective. Also for lunches, Fourth of July outings, apartment moves, advice on plants and letter-writing, horseback riding, encouragement to focus and to "work, work, work." I am grateful to Dr. Oliver Shih for many wonderful discussions about irreducible spherical tensors, the Luttinger model, and magneto-optics, and for all those late-nighters in 1991-92 when he and Hector and I were the Three Musketeers, struggling together to complete our theses. (Mine just took a little longer.) I am grateful to Dr. Hide Okamura for all the friendship and encouragement he has provided, and for significant help in setting up the field reversal experiment. He set a great example of diligence for me to try to follow. I am grateful to him for discussions about physics, and for such finer things as music at the Boston Symphony and dinner at Dixie Kitchen. I appreciate the encouragement from, and interesting discussions about magneto-optics in quantum wells with Dr. Lushalan Liao, along with some memorable outings for horseback riding and chinese cooking. I am grateful to Dr. Sam Sprunt for keeping things lively on the fourth floor viruses, prions, with discussions about and many other interesting physics, light scattering, topics. I appreciated killer having a friend at the lab who had shared the "Williams experience." Sam, along with others, like Drs. George Nounesis, Manfred Dahl, Ulf Gennser, Xichun Liu, Alex Fung, Flavio Plentz, and doctoral students Zachary Lee and David Rovnyak, 317 helped make life at the lab much more interesting and bearable. I thank Zachary for discussions of physics, and for donation of some drafting software, and David for discussions of colleges, computers and magnetic resonance. I am grateful to Dr. Roshan Aggarwal and Prof. Benjamin Lax for suggesting the early experiments on magneto-optics and spin-flip Raman scattering. To Roshy for teaching me the experimental techniques and making me focus on physical concepts instead of mathematical techniques, and to Ben for teaching me about quantum electronics, and for supporting my research at the Magnet Lab for five years. Also to Dr. Margaret Weiler for teaching me about the Pidgeon and Brown model, and for sharing her computational techniques and her unpublished work on magneto-optics and SFR scattering. I am particularly grateful to Prof. Peter Wolff for his stimulating course on semiconductors which introduced me to the k-dot-p method for band structure calculation, following the approach of Kane, Yafet, Luttinger and Blount, and for agreeing to co-supervise my work, with Don. I am grateful to Prof. Mildred Dresselhaus for teaching me group theory, for reading and making useful suggestions regarding this thesis, and for taking an interest in my research and my career. I am grateful to Prof. Robert Griffin, who directs this Lab, for his friendship and interest over many years, and his hospitality in providing me with office space, particularly during the past three years. I am also grateful: To the staff of the Francis Bitter National Magnet Lab for significant help over the years. To Larry Rubin for scheduling, for help with instrumentation, for interesting discussions about the physics of levitation and other topics, and for bringing to my attention a wonderful address about "The University" given by A. Bart Giamatti at the 1988 MIT commencement. To Larry Sousa for assisting with my early experiments and sample preparation. For his enthusiasm, joie de vivre, and the positive example he set for me and everyone around him. To Dr. Thang Vu for discussions about physics and computers, and for helping set up the data collection in my recent experiments. To Jim Coffin, Jean Morrison, Nancy Tucker, Ed McNiff, John Chandnoit and Paul Emery for help with scheduling and apparatus. 318 To Dr. Simon Foner for his interest, concern, and numerous discussions. To Irene Ferriabough (Mother Superior) and Aldona Shumway for their help and cheerfulness. To Dr. Emanuel Bobrov for his Russian translations and lore, and in particular for his translation of the article, in Russian, by Sheka and To Dr. Georgia Papaefthymiou for her encouragement discussions about M6issbauer spectroscopy. To Dr. Yaacov Shapira for his interest, advice, conversations, both in physics and non-physics, over many Zaslavskaya. and good advice, and and many interesting years. To Dr. Jagadeesh Moodera for many discussions, and for a shared interest in physics teaching. To Dr. L. R. Ram-Mohan for a discussion about band decoupling techniques. To John Morris of Infrared Labs in Tucson, for lending me a KRS-5 window for the germanium bolometer. To Peggy Berkovitz and Pat Solakoff of the Physics Department for their help this past summer, and in previous years. To Prof. Tom Greytak for approving my readmission to MIT. To my friends at Tulane: Profs. Alan Goodman, John Perdew and Mel Levy who encouraged my pursuit of physics, and to Prof. George Rosensteel, who stimulated my interest in algebra. To my former teachers: Dr. Roy Ellzey, Prof. Fielding Brown and Prof. David Park, who set wonderful examples of concern, enthusiasm and accomplishment. Of the people at home, I am most grateful to Louise Pipes Byrne for being my It was largely her encouragement that best friend, encourager and advisor. nudged me back into physics. She has a heart of gold, and has been kind to share her life, her family and her concern. She has helped me in more ways than I can describe, or ever repay. My thanks also to Dr. Christian Byrne, and to my wonderful friend, Gifford. I am grateful to my sisters Bev and Joan for their encouragement, love and support; for being so nice and for sharing so much. Also to my cousins Michael Richardson, Sean, and especially Mary, for their patience, moral support, perspective on life, King Cakes, and best of times This work is dedicated to them (and also to when we've been together. others). 319 To my friends the Woodwards, to Barbara and Robert, who have been so much a part of my life both in Boston and New Orleans. I thank them for sharing their home, where I lived for four months, their children, their advice and support over most of the past 30 years. Special thanks to Laura for caring so much, and for sharing her friends and many good times. She helped me maintain some finite level of sanity. And thanks to Bo, Ann and Peter for all their patience, good wishes, moral support, and great times too numerous to count. I am grateful to my friend Dr. Annette Ten Elshof for caring and taking time to help and advise; for telling me I could finish, and for many good times in New Orleans, Covington and Denver. I especially appreciate her remark about the importance of friends in completing a Ph.D. thesis. My observations at MIT seemed to teach me the opposite, but I think she was right after all. To Nelva Van Sickle and her family for maintaining Annette's concern, for her good advice and encouragement, and many more fun times in Denver and N.O. She is among the best people I know. I am grateful to Dr. Ali Ahmadi for his friendship, encouragement and prayers, and for his diligence and faithfulness in completing his thesis years ago, setting a example for me to follow. To the Cooches, Dorans, Flowers, Montgomeries, Ruddocks, Tekippes, Ronald Woodwards, and many others who have cared. To Karen Seeley and Courtney; to Gail and Joe Richardson; to Renee and Marthe Mann, and cousins too numerous to mention. To Aunt Betty and Miggy and Chris and Paulette and their families. To my God-children, for their patience and encouragement: Neil, Peter, Richard, Michael, Sean, Audrey; and Gifford Glenny (Pipes) Byrne. To my parents, for believing in me and supporting me in my education, my research and my life; and for their great love. To God for providing me with family and friends, and more; for the "assurance of things hoped for, the conviction of things not seen." I know this work is not worthy of them, but I am grateful, and it is dedicated to all of them. .,. 320