One-dimensional band-edge absorption in a 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 an n-type modulation-doped T-shaped single quantum wire with a gate to tune electron densities. With non-degenerate 1D electron gas, band-edge absorption exhibits a sharp band-edge-divergence of 1D density of states (DOS). 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 1D-electron-gas filling. Optical spectroscopy of 1D electron gas formed in ntype doped semiconductor quantum wires has been a subject of exciting challenges in the past two decades [1-11]. Theories have pointed out some interesting phenomena inherent in 1D electron gas, such as appearance/disappearance of band-edge 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 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 clarify such fundamental properties by optical spectroscopy, we need to measure both emission and absorption spectra at various temperatures and electron densities. This is because emission and absorption in doped systems selectively occur for occupied and unoccupied conduction-band states, respectively. 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 temperature-dependent absorption spectra of 1D electron systems at various electron densities. To investigate this unexplored subject, we developed a measurement system of resonant photoluminescence-excitation (PLE) spectra, which allows us to get clear lineshapes of absorption spectra 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. The sample structure of an n-type doped GaAs quantum wire is illustrated in Fig. 1. A single T-shaped quantum wire was formed at the cross-sectional area of 14nm-thick Al0.07Ga0.93As/Al0.33Ga0.67As quantum well (stem well) and 6 nm-thick GaAs/Al0.45Ga0.55As quantum well (arm well). Delta doping of Si at a distance of 100 nm from the stem well induced 2D electron gas with a density of 1 x 10 11 cm-2 in the stem well. By applying DC gate voltage (V g) 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]polarization direction to cut intense laser scattering. Normalized PLE spectra at various temperatures in the presence of dense 1D electron gas are shown by solid curves in Fig. 2 (a). The gate voltage was fixed to 0.7V, which corresponds to the electron density of FIG. 1 Schematic view of n-type doped T-shaped quantum wire sample. FIG. 2 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. about 6 x 105 cm –1 in the quantum wire. At low temperature (5K), we observed a single absorption onset 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 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 at 50K. We assigned this peak to the band-edge (BE) singularity induced by the inverse square root 1D-DOS divergence. Dotted curves in Fig. 2 (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. We 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 red shift 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. We calculated optical spectra with a free-particle model. 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 many-body Coulomb interactions. Figure 2 (b) shows normalized 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. 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. 2 (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 these freeparticle-model calculations. 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. 3 (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. 2 (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. 4 (a). At Vg = 0.4V, band-edge absorption onset appeared at low-energy side (1.566eV). At Vg = 0.35V, this lowenergy onset increased its intensity, and 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 peak, and formed a single asymmetrical absorption peak structure at V g = 0.2V. This asymmetrical peak became a symmetrical peak (X-) at Vg = 0.15V, which is 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 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 fullwidth-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. 4 (a), we plot peak energies of X- (solid triangles) and X (solid circles). Dotted curves in Fig. 3 (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 Fig. 4 (a) The position of peaks and (b) estimated electron density and corresponding Fermi energy are plotted as a function of gate voltage. FIG. 3 ormalized 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. observed broad PL peak which shifts to higher energy with decreasing electron density, which represents the band-gap-renormalization shift. The energies of the PL peak at BE are plotted by solid squares in Fig. 4 (a). At 0-0.15V, PL spectra also show sharp peaks of trions (X ) and excitons (X). The Stokes shift between the PL and PLE peaks of excitons was less than 0.2meV. Figure 3 (b) shows calculated normalized emission (dotted curves) and absorption (solid curves) spectra with the free-particle model assuming various electron densities (ne) and parameters of Te (=Th) = 8K, = 0.4 meV. 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. 4 8me (b) as blank squares and blank circles, respectively. The calculated absorption spectra for ne = 1 – 5.9 x 105 cm-1 show good agreements with the experimental PLE spectra at Vg > 0.2V. In particular, the characteristic double peak structures of the band-edge and the Fermi-edge absorptions at Vg = 0.35-0.4 V are almost completely reproduced by the calculations. The sharp band-edge absorption originates from 1D-DOS divergence, and it appears in the PLE spectra when the 1D electron gas is not degenerate at low density. We have already demonstrated, in Fig. 2 (a), the appearance of band-edge divergence in the PLE spectra at high temperature (50K). These results confirm our insistence that the divergence of 1D DOS appears in the PLE spectra in the presence of non-degenerated electron gas at low density, or at high temperature. On the contrary, the sharp symmetrical absorption peaks of trions and excitons observed at V g = 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. In 1D systems, this excitonic effect becomes strong due to its large quantum confinement [someya]. However, it has not been fully understood how the 1D excitonic effect is weakened by screening or phase-space-filling effects caused by the 1D electron gas. Our experiments provided a quantitative value of the electron density where the excitonic effects have to be taken into account. The value was ne < 1 x 105 cm-1, which corresponds to the Fermi energy of Ef < 0.15 meV and mean distances between carriers of rs < 8aB, where aB (=12.7 nm) is the Bohr radius of bulk GaAs. Above this density, the PLE spectra exhibited free-particle behavior. Let us now discuss the 1D many body effects that appear in PL and PLE spectra at high electron densities. As we have mentioned, the pioneering works have pointed out interesting many-body effects, such as the FES effects [4-9] and the BGR effects [10,11]. The FES theory [4-7] predicts a sharp FES peak, or a power-law singularity, at low-energy (high-energy) shoulder of absorption (emission) spectra. This effect results from multiple scattering processes involving electrons near the Fermi level. The BGR theory [*] predicts an energy shift of band-edge emission peak with increasing the electron density, which results from the electronic correlation effects. In our experiments, as shown in Fig. 3 (a), or Fig. 4 (a), the BGR effect was observed as the red shifts of the band-edge PL peak (BE) with increasing electron density. However, the FES effect in the PLE spectra was surprisingly small. No sharp peak, or no power-law singularity, was observed at the Fermi edge of the PLE spectra. We should notice that the inhomogeneous broadening is small (0.9 meV) and the temperature is low (5-8 K), which are favorable conditions for strong FES effects. Even under these conditions, the FES effect was found to be weak. This indicates that the strength of FES effects are governed by not only dimensions and temperatures, but also other factors. As pointed out by pioneering works [4,5,12], we guess the carrier localization and the existence of empty higher subband are necessary for strong FES effects. In this sense, the free particle behavior without FES effect could be the essential character inherent to 1D electron gas formed in the high quality 1D limit quantum wires. We want to focus here on the carrier localization effect, which is also one of the interesting topics for 1D electron systems [*]. Generally speaking, the effect of localization is strong when the carrier density is small, because of its weak screening effect. Even in the presence of dense electron gas, the localization of valence holes needs to be taken into account. In fact, our experimental results of PL spectra at high density (Vg > 0.5V) shows inhomogeneous structures, such as the appearance of multiple peak structures at higher energy tail of BE, as shown in our previous paper [10]. We guess this indicates that a part of valence holes are localized to the inhomogeneous potential fluctuations. This is consistent to the theoretical prediction that hole localization causes the strong FES effects in PL spectra [4,5]. On the contrary, the lineshape of PLE structures at high density, such as band-edge and Fermi-edge peaks, have no dependence on the position of the wire. These facts indicate that a small amount of hole localization modifies the PL, but not PLE. The present work is the first convincing observation of the 1D DOS divergence, and also provides new findings for optical response of 1D electron gas. We want to notice that these findings were provided as a result of following experimental progresses. First of all, the high-quality sample fabrication method [13] cannot be omitted. Without this, the sharp 1D DOS peak, and also sharp excitonic peaks, would be broadened. The development of resonant PLE measurement system is also important. This enables us to observe the lineshape of band-edge absorption peaks of a single quantum wire. In addition, n-type doping is one of the important factors for the observation of 1D DOS. In the case of non-doped wire [14,15], the continuum onset exhibited a step-functional lineshape due to the small Sommerfeld factor [16,17], even though it’s quality is as good as our doped samples. Thanks to these experimental improvements, we confirmed our progress to the fabrication of ideal 1D electron gas formed in the semiconductor quantum wire. 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. The 1D excitonic effects were found to be suppressed by the electron gas at the density of 1 x 105 cm-1, so that the PLE spectra above this density exhibited free-particle behavior without many-body modifications. Compared to PL spectra, the PLE spectra were less modified by the small amount of localization of valence holes. These new findings confirm our progress to the fabrications of ideal 1D electron gas formed in the semiconductor quantum wire. 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. 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