One-dimensional band-edge absorption in a on doped quantum wire T. Ihara1, Y. Hayamizu1, M. Yoshita1, H. Akiyama1, L. N. Pfeiffer2, and K. W. West2 1 Institute for Solid State Physics, University of Tokyo and CREST, JST, Chiba 2778581, Japan 2 Bell Laboratories, Lucent Technologies, Murray Hill, NJ 07974, USA Abstract. Low-temperature photoluminescence-excitation spectra are studied in on an n-type modulation-doped Tshaped single quantum wire with a gate to tune electron densities. We find that the With non-degenerate 1D electron gas, band-edge absorption of 1D electron systems exhibits a sharp band-edge-divergence peak structure of induced by the singularity of 1D density of states (DOS) divergence. When the dense 1D electron gas is degenerate at a low temperature, we observed a Fermi-edge absorption onset without power-law singularity. In stark contrast to theoretical predictions (and to non-doped-wire experiments), excitonic (or correlation) effects in the optical spectra are suppressed by 1Delectron-gas filling. We show that these results can be explained by the free-particle-model with inverse square root 1D DOS and carrier distribution functions. Optical spectroscopy of 1D electron gas formed in ntype doped semiconductor quantum wires has been a subject of exciting challenges intense research in the past two decades [1-11]. Pioneering tTheoreticalies works have pointed out some interesting kinds of phenomena inherent in 1D electron gas, such as appearance/disappearance of band-edgebottom singularity induced by inverse square root 1D-DOS divergence, and also strong 1D many-body interaction effects [4-7]. Experimentally, observations of strong Fermi-edge power-law singularity effects [8,9] and 1D band-gap renormalization effects [10,11] have been reported. However, no experiment has shown one has achieved the direct observation of band-edge singularity induced by 1D-DOS divergence. Thus, a question of whether the 1D band-edge singularity appears in optical spectra still remains unanswered. In order to study clarify such fundamental properties the lineshape of DOS in detail by optical spectroscopy, we need to measure both emission and absorption spectra at various temperatures and electron densities. This is because emission and absorption the optical spectra of in doped systems selectively occur for occupied and unoccupied conduction-band states, respectively. exhibit not only DOS but also the effect of carrier distribution. However, it is difficult to measure absorption spectra of quantum wires because of its small volume. Thus, there have been no systematic experimental studies of temperaturedependent absorption spectra of 1D electron systems at various electron densities. To investigate this unexplored subject field, we developed a measurement system of resonant high-resolution photoluminescenceexcitation (PLE) spectra measurement system, which allows us to get a clear lineshapes of absorption spectruma of a single quantum wire. This letter reports the first observation of band-edge absorption singularities induced by 1D DOS divergence probed by the low-temperature PLE measurements on an n-type doped single quantum wire with a gate to tune electron densities. The sharp bandedge absorption peaks appear in the PLE spectra when the 1D electron gas is not degenerate at high temperature, or at low electron density. In the presence of dense electron gas at low temperature (5K), we observe an absorption onset at the Fermi edge of degenerate 1D electron gas. The absorption lineshapes agree very well with free-pariticle calculations, but surprisingly not with more advanced calculations including many-body Coulomb interactions. Our interpretations are supported by good agreements between the experimental results and free-particlemodel calculations with inverse square root 1D DOS and carrier distribution functions. The sample structure of an n-type doped GaAs quantum wire is illustrated in the inset of Fig. 1. A single T-shaped quantum wire was formed at the crosssectional area of 14nm-thick for the Al0.07Ga0.93As/Al0.33Ga0.67As quantum well (stem well) and 6 nm-thick for the GaAs/Al0.45Ga0.55As quantum well (arm well). Delta doping of Si at a spacer distance of 100 nm from the stem well induced resulted in the formation of 2D electron gas with a density of 1 x 10 11 cm-2 in the stem well. By applying DC gate voltage (Vg) to a gate layer on the top of the arm well relative to 2D electron gas in the stem well, we tuned electron concentrations in the 1D wire. A more detailed description of the sample preparation is given in ref. 10. In our micro-PL and PLE measurements, excitation light from a continuous-wave Titanium-sapphire laser with polarization parallel to the [001] direction (perpendicular to the wire axis) was focused into a 1m spot by a 0.5 numerical aperture objective lens on the top (110) surface of the sample. The PL emission in the [001] direction was detected via a 0.5 numerical aperture objective lens and a polarizer set in the [1-10]- Fig. 1 Normalized experimental (a) and theoretical (b) spectra of PL (dotted line) and PLE (solid line) for 1D wire at various temperatures. FE and BE corresponds to Femi edge and band edge, respectively. polarization direction to cut intense laser scattering. Normalized PLE spectra at various temperatures in the presence of dense 1D electron gas are shown by as solid curves in Fig. 1 (a). The gate voltage was fixed to 0.7V, which corresponds to the electron density of about almost 6 x 105 cm –1 in the quantum wire. At low temperature (5K), we observed a single absorption onset (FE) at 1.575eV with a long low-energy tail. We assigned this onset as the Fermi edge (FE), which separates the occupied and unoccupied state in the conduction band. A large absorption by the arm well showed its low-energy tail at around 1.578eV. As the temperature was increased, the FE onset was smeared disappeared and the low-energy tail increased its intensity. At 30K, another absorption onset was formed at 1.565eV. At higher temperature, this onset increased its intensity and formed a sharp peak structure (BE) at 50K. We assigned this BE peak to the band-edge (BE) singularity induced by the inverse square root 1D-DOS divergence. Dotted curves in Fig.1 (a) indicate PL spectra. At 5K, we observed an asymmetrical broad PL peak at 1.565eV. We assigned this PL peak to the band-edge emission. Here wWe observed a large energy gap of 10meV between PL peak and PLE onset at FE. As the temperature was increased, the PL peak shifted to lower energy without any remarkable change in its lineshape. This kind of red shifts with increasing temperature also appears in bulk GaAs [3]. At 50K, we found that the PL and PLE peak appeared exactly at the same energy of band edge denoted by BE. To check the validity of our assignment of FE as Fermi edge and BE as band edge, wWe calculated optical spectra with a free-particle - model formulae. This model includes the 1D joint DOS with the energy dependence of 1/ E , Fermi distribution functions for electrons and holes, broadening function of Gaussian lineshape, but neglects any kinds of many-body Coulomb interactions. Figure 1 (b) shows Nnormalized emission (dotted curves) and absorption (solid curves) spectra calculated for various temperatures for electrons and holes, Te (= Th), with parameters of broadening () of 1.0 meV, the effective mass for electrons of 0.067 m0 and that for holes of 0.105 m0, where m0 is electron mass in vacuum, and the electron density (ne) of 6 x 105 cm–1, are shown in Fig. 1 (b). The band gap energies at various temperature, Eg(T), were estimated roughly by those for bulk GaAs [3]. The absorption spectrum at 8K, shown as bottom solid line in Fig. 1 (b), exhibits an onset at the energy of Eg + 10meV, which corresponds to the Fermi edge. The low-energy tail of this onset corresponds to the slope of Fermi distribution function at 8K. The emission spectrum exhibits a peak at the energy of Eg, which corresponds to the band edge. At higher temperature, the Fermi-edge absorption onset disappears while another low-energy absorption onset of the band edge appears at the same energy of emission peak (Eg). At 40K or 50K, the absorption spectra exhibit a sharp asymmetrical peak at the band edge. This peak originates from the 1D-DOS divergence with broadening of 1.0 meV. We found that the experimental results agree well with are analogous to these free-particle-model calculations, which supports our interpretations of BE as the band edge and FE as the Fermi edge. The sharp absorption peak at 50K clearly demonstrates the 1D band-edge singularity induced by 1D-DOS divergence. We also studied electron density dependence of PLE spectra at low temperature (5K), using the same sample of a doped quantum wire. The solid curves in Fig. 2 (a) indicate the normalized PLE spectra at various Vg. The bottom line at Vg = 0V corresponds to the zero-density. The top line at Vg = 0.7V corresponds to the highdensity, which is the same as the bottom line of Fig. 1 (a). As we have already mentioned, the single absorption onset (FE) at Vg = 0.7V corresponds to the Fermi edge. As the density was decreased, the FE onset shifted to lower energy. The photon energies of the FE onset are plotted by solid inverse triangles in Fig. 3 (a). At Vg = 0.4V, band-edge another absorption onset appeared at low-energy side (1.566eV). At V g = 0.35V, this low-energy onset increased its intensity, and so that a characteristic double peak structure was formed. As the density was further decreased, the Fermi edge peak merge into the tail of the band-edge low-energy peak, and formed a single asymmetrical absorption peak structure at Vg = 0.2V. This asymmetrical peak became a symmetrical peak (X-) at Vg = 0.15V, which is we assigned to trions (a bound state of two electrons and a hole). This X - peak lost its intensity as the density approached to zero. Instead, another asymmetrical sharp peak appeared at higher energy (1.569eV), which became a sharp peak (X) at 1.569eV at Vg = 0V. We assigned this X peak to neutral excitons (a bound state of an electron and a hole). The full-width-of-half-maximum of X peak was 0.9 meV. The splitting of the X peak is probably due to monolayer thickness fluctuations in the stem well. In Fig. 3 (a), we plot peak energies of X- (solid triangles) and X (solid circles). Dotted curves in Fig. 2 (a) indicate PL spectra, which are almost same as those we reported in detail in a previous paper [10]. At Vg from 0.7V to 0.2V, we observed broad PL peak which shifts to higher energy with decreasing electron density, which represents the band-gap-renormalization shift. The photon energyies of the BEPL peak at BE are plotted by solid squares in Fig. 3 (a). At 0-0.15V, we observed PL spectra also show sharp PL peaks of trions (X-) and excitons (X). The Stokes shift between the PL and PLE peaks of excitons was less than 0.2meV. Figure 2 (b) shows Here we want to demonstrate the free-particle-model calculationsed too. Nnormalized emission (dotted curves) and absorption (solid curves) spectra calculated for with the free-particle model assuming various electron densities (ne) and with parameters of Te (=Th) = 8K, = 0.4 meV are shown in Fig. 2 (b). The assumed electron density (ne) in the calculations and corresponding Fermi energy, 2 2 ne 2 Ef are plotted as a function of Vg in Fig. 3 8me (b) as blank squares and blank circles, respectively. The calculated emission spectra exhibit almost no change with ne. Thus, they do not reproduce the change in the experimental PL data. However, we found good agreements between the experimental PLE spectra at Vg > 0.2V and the calculated absorption spectra with the free-particle model. In particular, the characteristic double peak structures of the band-edge and the Fermiedge absorptions at Vg = 0.35-0.4 V are almost completely reproduced by the calculations. The calculated absorption curve for ne < 1.0 x 105 cm-1 represents the inverse-square-root 1D-DOS shape with broadening of 0.5 meV. It is remarkable that observed optical-absorption responses of electron gas with estimated densities above 1.0 x 105 cm-1 are apparently the same as those of free electrons except for band-gap renormalization. We plotted the electron density (ne) and 2 2 ne 2 corresponding Fermi energy, E f as a 8me function of Vg in Fig. 3 (b) as blank squares and blank circles, respectively. The top lines of Fig. 2 (b) correspond to high-density (5.9 x 105 cm-1), which exhibit the Fermi-edge absorption onset and the bandedge emission peak. As the density decreases, the Fermi edge absorption onset shifts to lower energy due Fig. 2 Normalized experimental (a) and theoretical (b) spectra of photoluminescence (PL: dotted lines) and PL excitation (PLE: solid lines) for 1D quantum wire at various electron densities. X is assigned to excitons and X- is assigned to trions. BE and FE corresponds to the band edge and the Fermi edge, respectively. to the decreasing Fermi energy. At ne = 4.2 and 2.9 x 105 cm-1, an absorption onset appears at lower-energy side, which corresponds to the band edge. At ne = 2.2 x 105 cm-1, a characteristic double peak structure of the band-edge and the Fermi-edge absorptions appears. At lower densities, the Fermi-edge absorption merges into the high-energy tail of band-edge absorption. At ne < 1.0 x 105 cm-1, the solid curve exhibits an asymmetrical band-edge absorption peak. The lineshape of this peak represents the inverse square root 1D-DOS with broadening of 0.5 meV. The emission spectra exhibit almost no change with decreasing ne. We found good agreements between the experimental PLE spectra at Vg > 0.2V and the freeparticle-model calculations for ne = 1 – 5.9 x 105 cm-1. This indicates that the PLE structures in the presence of electron gas with density of more than 1.0 x 10 5 cm-1 can be understood by the free-particle model without any kinds of many-body effects. From this point of view, the sharp low-energy peaks at Vg = 0.2 – 0.35V corresponds to the 1D band-edge singularities induced by 1D-DOS divergence. And the higher-energy peaks, or onsets, which evolved from FE onset at V g = 0.7V, corresponds to the Fermi edge. Hence, the double peak Fig. 3 (a) The position of peaks and (b) estimated electron density and corresponding Fermi energy are plotted as a function of gate voltage. structure at Vg = 0.35V corresponds the coexistence of band-edge and Fermi-edge absorption peaks. On the contrary, the free-particle model cannot explain the sharp symmetrical absorption peaks of trions and excitons observed at Vg = 0 – 0.15V are out of explanation of this free-particle model. In other words, we need to take into account Coulomb interactions between conduction electrons and a valence hole to explain these bound complexes. It is interesting that these excitonic peaks appear only at such low electron density. Qualitatively speaking, the absorption peak of excitons completely disappeared at ne < 1.0 x 105 cm-1. This small value of the density of 1.0 x 105 cm-1 corresponds to the Fermi energy (Ef) of 0.15meV, and also corresponds to mean distances rs between carriers of 8aB, where aB (=12.7 nm) is the Bohr radius of bulk GaAs. Note that it is hard to determine the density at which the trions disappear from the PLE spectra, since the trion peak evolves continuously to the band-to-band structures of BE and FE at Vg > 0.2V. Here we want to remark two important findings in Fig. 2 (a), which are inherent in 1D electron systems. One is the strong band-edge absorption observed at Vg = 0.2 - 0.35V. As we have mentioned, this band-edge absorption peak originates from the inverse square root divergence of 1D DOS. The other one is the remarkable decrease of exciton intensities, which is symbolized by the fact that the exciton peak disappeared at low electron density (1.0 x 105 cm-1). This indicates the strong effects of phase-space-filling and/or screening induced by dilute electron gas in 1D systems. As shown above, we demonstrated the first observation of the band-edge absorption singularities induced by 1D-DOS divergence. We expect that this result could not be achieved without the fabrication technique of high-quality doped quantum wire samples [13] and the development of high-resolution PLE method. Thanks to these techniques, we could achieve the observation of 1D band-edge absorption with less modification by carrier localization effects induced by interface roughness of hetero junctions. Note that the 1D-DOS divergence did not appear even in PLE spectra of high-quality non-doped quantum wires [14,15]. In the case of non-doped 1D system, the continuum absorption onset exhibited a step-functional lineshape due to small Sommerfeld factor [16,17]. In this sense, n-type doping was one of the important factors for the observation of 1D DOS. Finally, we want to comment on the comparisons with pioneering experiments reported by other groups. It has been pointed out that strong FES effects appear in the PL (or PLE) spectra of heavily doped 1D electron systems [8,9]. This result is in contrast with our observation of no remarkable many-body modifications at the Fermi-edge absorption onset. We speculate that this inconsistency is due to the difference of sample structures that determine the condition of 1D electron gas and a valence hole. In fact, some of the pioneering works of experiments [12] and theories [4,5] have indicated the necessity of hole localizations, and also empty higher subbands near the Fermi energy, for the observation of strong FES effects. Thus, it is not striking that the pronounced strong FES effect was not observed in our quantum wire, which contains 1D limit electron gas, with small carrier localization effects. メモ ファイ HF レベル計算や高際計算も試みたが、 フェルミレベルのところが強くモディファイされ 実験にあわない。小川理論では、実際、1 次元で はパワーローFES は強く表れると期待されている。 しかし、実験はそうなっていない。 温度ではないはず。 構造揺らぎでもないはず。 解らないが、何か本質的な理由があって、フェ ルミレベルでのクーロンエンハンスメントが消失 して自由粒子的になっているのではないか? これらのおそらく1D 特有の実験結果が出たの は試料の高品質が必須。 発光では特に局在は重要。 局在が発光ピーク位置を BE から FE にする理論 実験もそうなっているみたいだ。 エキシトンやトリオンがクエンチ vs エキシトンがトリオンに移ってクエンチ In conclusion, we performed low-temperature PLE measurements on an n-type doped quantum wire and achieved the first observation of 1D band-edge absorption singularities. We found that the freeparticle-model with inverse square root 1D DOS can explain the PLE spectra in the presence of dense electron gas with the density of more than 1 x 10 5 cm-1. We believe that our observation of 1D DOS, and also the observation of remarkable decrease of exciton absorption intensities in the presence of dilute 1D electron gas, indicates the progress in fabrication of ideal 1D electron systems formed in doped quantum wires. This work was partly supported by a Grant-in-Aid from the Ministry of Education, Culture, Sports, Science, and Technology, Japan. We wish to thank T. Ogawa, M. Takagiwa, and K. Bando for valuable discussions. [1] H. Haug and S. W. Koch, Quantum Theory of the Optical and Electronic Properties of Semiconductors (4th edition, World Scientific, Singapore, 2004). [2] C. Klingshirn, Semiconductor Optics (2nd edition, Springer, Germany, 2004). [3] W. W. Chow and S. W. Koch, Semiconductor-Laser Fundamentals (Springer, Berlin, 1999). [4] F. J. Rodriguez et al. Phys. Rev. B 47, 1506 (1993); 47, 13015 (1993). [5] P. Hawrylak et al., Solid State Commun. 81, 525 (1992). [6] T. Ogawa et al., Phys. Rev. Lett. 68, 3638 (1992). [7] A. Esser et al., Phys. Status Solidi B 227, 317 (2001). [8] J. M. Calleja et al., Solid State Commun. 79, 911 (1991); Surf. Sci. 263, 346 (1992). [9] M. Fritze et al., Phys. Rev. B 48, 4960 (1993). [10] H. Akiyama et al., Solid State Commun. 122, 169 (2002). [11] R. Rinaldi et al., Phys. Rev. B 59, 2230 (1999). [12] D. Y. Oberli et al., Physica E 11, 224 (2001). [13] M. Yoshita et al., Jpn. J. Appl. Phys. 40, L252 (2001). [14] H. Itoh et al., App. Phys. Lett. 83, 2043 (2003). [15] H. Akiyama et al., App. Phys. Lett. 82, 379 (2003). [16] T. Ogawa et al., Phys. Rev. B 43, 14325 (1991); 44, 8138 (1991). [17] F. Rossi et al., Phys. Rev. Lett. 76, 3642 (1996).