Optical processes and excitons •Dielectric function and reflectance •Kramers-Kronig relations •Excitons •Frenkel exciton •Mott-Wannier exciton •Raman spectroscopy Dept of Phys M.C. Chang Dielectric function, reflectivity r, and reflectance R Response of a crystal to an EM field is characterized by (k,), (k0 compared to G/2) Experimentalists prefer to measure reflectivity r (normal incidence) E ' r () E Prob.3 n 1 ( ) r () R () ei n 1 Eei ( kx t ) E ' ei ( kx t ) where the refractive index n() ( ) It is easier to measure R than to measure measure R() for () (with the help of KK relations) n() () Kramers-Kronig relations (1926) KK relation connects real part of the response function with the imaginary part examples of response function: j ( ) E Ohm’ s law P ( ) E polarization •does not depend on any dynamic detail of the interaction E ' r () E reflective EM wave •the necessary and sufficient condition for its validity is causality Example: Response of charged (independent) oscillators For the j-th oscillator (atom or molecule with Z bound charges), Fd mG H dt 2 j 2 i IJ K d 2j x j Fje it , dt x j (t ) x je it Fj Z j eE steady state p j Z j ex j j () E electric dipole Z 2j e 2 j () m j 2j 2 i j d i Figs from http://www.physics.uc.edu/~sitko/LightColor/10-Optics1/optics1.htm Collection of oscillators Z 2j e 2 1 1 P Z j ex j ( ) E ( ) , (1) V j V j m j 2j 2 i j d 2 2 nZ e / m for identical 2 oscillators 0 2 i 1 4 Some properties of (): 0 (1) () has no pole above (including) x-axis. ( ) (2) d 0 along (upper) infinite semi-circle (3) ’ () is even in , ’ ’ () is odd in . z i 1 ( ) P From (1), (2), we have i (can be , or , or... ) z z ( s) ds s ' ' ( s) 1 '() P ds s ' '( s) ' ' ( s) 1 P ds ds 0 s 0 s i 2 s' ' ( s) ' () ds (2) 0 s2 2 z Also, FG z H 2 ' ' () z z 0 IJ K ω property (3) used '( s) ds (3) s2 2 z z z A few sum rules: 2 ' ' ( s) ds ' (0) 0 s An example of the “ fluctuationdissipation”relation From (1) and (2), >>1 (Prob. 2): 2 1 s' ' ( s)ds = f j , 0 V j Z 2j e 2 Thomas-Reichefj m Kuhn sum rule From (3), >>1 (Prob. 4): and many more…, e.g., (4)+(5) (next page): 2 ' ( s) ds = lim ' ' (), (4) 0 z 0 1 2 ' ( s)ds p 8 By Ferrel and Glover (1958) KK relation for reflection E ' r () E ln r () ln R1/ 2 () i ( ) Why take log? See Yu and Cardona for related discussion ln R( s) then ( ) 2 ds 0 s 2 1 s d ln R ln ds 2 0 s ds •constant R(s) doesn’ t contribute •s>>, s<<don’ t contribute ref: Cardona and Yu Conductivity of free electron gas (j=0, with little damping) 1 e2 ( ) V j m 2j 2 i j d i LM N ne 2 1 ne 2 1 ( ) = lim i ( ) m0 i m OP Q (KK relations can be checked easily in this case) 2p ( ) 1 4 ( ) 1 2 1 i ( ) Recall that (chap 10) =1+ 4 i ne 2 1 4i m Real part of DC conductivity diverges (compare with ne2 /m) i ( ) , (5) Drude weight D Other sum rules (Mahan, p358): For a clean conductor at T =0 (or superconductor), 1 2 s Im ds p 0 ( s) 2 ( ) D ( ) reg (), 1 1 Im ds 0 s ( s ) 2 then D lim ''() Related to the energy loss of a passing charged particle Dielectric function and the semiconductor energy gap (prob.5) band gap absorption (due to nonzero ’ ’ ) can be very roughly approximated by ''() ( ) p2 (g ) 2 2 p p2 '()=1 2 g2 p2 '(0)=1 2 g Si ’ Ge GaAs InP GaP 12.0 16.0 10.9 Eg (theo) 4.8 4.3 5.2 Ex (exp’ t) 4.44 4.49 5.11 (ref: Cardona and Yu) Figs from Ibach and Luth 9.6 9.1 5.2 5.75 5.05 5.21 Interband absorption for GaAs at 21 K Tight bound Frenkel exciton: (excited state of a single atom) •alkali halide crystals •crystalline inert gases Excitons (e-h pairs) in insulators Weakly bound Mott-Wannier excitons Similar to the impurity states in doped semiconductor: e 4 En E g 2 2 2 , 2n 1 1 1 me mh CuO2 Raman effect in crystals I () nk 1 u nk 2 nk 1 I () nk 1 u nk 2 nk I () n k e / k B T I () nk 1 1930