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Photoluminescence-excitation spectra of a doped single quantum wire near metal-insulator crossover Toshiyuki 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. We measured photoluminescence-excitation spectra at 5K on an n-type modulation-doped single quantum wire with a gate to tune electron densities. We found drastic transfer of oscillator strength from excitons to trions. At higher electron densities, double absorption peaks corresponding to the band edge and the Fermi edge are observed. These anomalies show bound-state formation and carrier population in inverse-square-root density of states inherent to one-dimensional systems. Optical spectroscopy of doped quantum structures have provided intriguing subjects in fundamental physics, such as the Burstein-Moss shift between photoluminescence (PL) and absorption reflecting Fermi electron distribution and Pauli exclusion principle, the trion state formed as a bound state of two electrons and a hole, metal-insulator crossover, Fermiedge singularity and other many-body effects [1]. In particular, effects of low dimensionality in these phenomena have attracted strong interests, and intensive research has been made in two-dimensional (2D) quantum wells [2]. In 1D quantum wires, there have been several reports predicting or finding novel 1D features induced by the inverse-square-root density of state (DOS), singular 1D Coulomb interactions, and 1D collective excitation effects [3]. However, the difficulty in fabrication of high-quality quantum wires has prevented us from a detailed study on 1D system, since the band bottom singularity can be easily smoothed by sample disorders. In addition, the small volumes of quantum wire make it difficult to measure the absorption or excitation spectra that directly reflect the oscillator strength. Therefore, many of the subjects of fundamental interests are still left open, and most of the earlier predictions and findings need experimental verification or further confirmation. Recently, we improved the quality of T-shaped GaAs quantum wires, and measured photoluminescence excitation (PLE) spectra of nondoped multiple quantum wires with high spectral resolutions [4]. We observed the pronounced OS concentration into the lowest bound state, as well as the reduction of the absorption at the continuum state, i.e., the 1D DOS divergence does not appear at the continuum absorption edge. We interpreted this feature as a result of Coulomb interaction between an electron and a hole, which is consistent of the earlier theoretical predictions [5]. On another front, we also fabricated a high-quality n-type modulation doped quantum wire with a gate to tune the density of one-dimensional electron gas. In the previous paper, we demonstrated the evolution of PL spectra during metal-insulator crossover where a trion PL peak evolves to a broad PL peak due to bandto-band transition [6]. In this letter, we report on the PL and PLE spectra at various electron densities (ne) in an n-type doped single quantum wire with a gate. The PLE spectra show a drastic OS transfer from excitons to trions with increasing ne from zero, which can be interpreted as a nature of 1D system where the OS concentrates into the lowest bound state. At higher ne, we observed the metal-insulator crossover where the trion peak evolves to the typical single absorption onset of the band-toband transition. In this crossover region, we found a double absorption peak structure corresponding to Fermi edge at low temperature and inverse-square-root divergence of 1D DOS at band edge. The sample structure of n-type doped GaAs quantum wire is illustrated in the inset of Fig.1. The Tshaped quantum wire is formed at the cross sectional area of 14nm Al0.07Ga0.93As - Al0.33Ga0.67As quantum well (stem well) and 6 nm GaAs - Al0.45Ga0.55As quantum well (arm well). The modulation doping of Si at the spacer distance of 100nm from the stem well results in the formation of 2D electron gas with the density of 1x10^11cm-2 in the stem well. By applying DC gate voltage (Vg) to the gate layer on the top of arm well relative to 2D electron gas in the stem well, we can tune the electron concentrations in 1D wire and also in 2D arm well. The detailed conformation of this sample is shown in ref. [6]. In our micro-PL and PLE measurements, the excitation light from a continuous wave Titaniumsapphire laser was polarized to (001) direction, which was perpendicular to the wire axis, and was focused into a 1 m spot by a 0.5 numerical aperture objective lens on the top (110) surface of the sample. The emission to the direction of (001) was detected by a 0.5 numerical aperture objective lens via a polarizer of (-110) direction so as to cut the intense laser scattering. (1.566eV) and broad peak at higher energy (1.570eV). At Vg=0.7V, we observe a broad absorption onset (FE) that has long tail at low-energy side. The absorption of the arm well is so large that we cannot remove its low-energy tail at 1.580eV. In the PL spectra at low ne (0-0.15V), we observed sharp excitonic emission at the energy of both X and X-. As ne increases, X- evolves into the broad PL peak whose low energy shoulder (BE) shows red-shift. We have demonstrated the evolution of PL spectra in a previous paper [6]. In order to give a rough assignment of the spectral structure at high ne, we make a theoretical calculation of free particle approximation, neglecting the manybody interaction. We take into account joint density of state (Dj), Fermi distribution for electrons (fe) and holes (fh), and Lorenzian convolution with phenomenological broadening (L). Using these terms on the effective mass approximation, the emission (I) and absorption (A) spectra are given by following equations. I D1j D f e e f h h L E g d A D1j D 1 f e e L E g d where FIG. 1 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 density. Note we have checked that this experimental setup does not change the lineshape of optical spectra shown in this paper, but significantly reduces the background noise of PLE spectra. Fig.1 (a) shows the normalized PL (dotted lines) and PLE (solid lines) spectra at various gate voltages (Vg) measured on 1D quantum wire at 5K. At first, we demonstrate the evolution of PLE spectra with increasing ne. At Vg=0V, where ne is very low, we observe a sharp absorption peak at 1.569eV (X) with FWHM of 0.9meV, which is assigned as neutral excitons. The splitting of X peak is probably due to the inhomogeneous monolayer fluctuations of the stem well. As ne increases with applying gate voltage, X moves to higher energy showing drastic quenching. Instead, a new absorption peak (X-) appears at almost 2meV below X, which we assigned as negatively charged excitons (trions). At Vg=0.2V, X becomes undetectable, and asymmetric X- peak completely dominates the PLE spectrum. At much higher Vg, a new broad peak appears from the high-energy tail of X-, which results in a characteristic double peak structure (0.35V) of sharp onset at the lowest energy e , h are the kinetic energy of electrons and holes, respectively, and e h (1 me / mh ) e . We assumed the band gap energy (Eg) as a constant, and calculated the spectra as a function of photon energy ( ). Fig.1 (b) shows the normalized emission (dotted lines) and absorption spectra (solid lines) calculated for 1D system at various electron density with the parameter of =0.2meV, me=0.067m0, and mh=0.105m0, and Te=Th=8K. The electron density was calculated by following relation. ne De1D e f e e d e 1 2me 2 1 e f e e d e While the emission peak stays at band edge (the energy of Eg), the absorption spectra show dramatic evolution from the sharp peak at band edge at low ne (5.2x104) to the broad onset at Fermi edge of 8K at high ne (5.8x105). The good agreements between measured PLE and calculated absorption spectra lead us to the following conclusion: First, the FE onset observed at high ne (0.7V) corresponds to the absorption at Fermi edge at low temperature (5K). Next, the low energy shoulder of PL peak (BE) at high ne, which evolves smoothly from X- peak, corresponds to band edge. Finally, the double peak observed at the crossover region (0.35V) corresponds to the coexistence of absorption at band edge and Fermi edge. We believe this is the first observation of the characteristic double peak feature corresponding 1D DOS singularity and Fermi edge. Note that these interpretations have been confirmed by the measurement of temperature dependence of optical spectra. In that experiment, we found that, as the temperature increases, FE onset loses its amplitude FIG. 2 (a) The position of peaks, (b) X - X- energy gap and Fermi energy, and (c) PLE maximum intensity measured for 1D wire are plotted as a function of gate voltage. The same plots for 2D arm well are shown in (d), (e) and (f). and the absorption at band edge appears, i.e., BursteinMoss shift disappears. The temperature dependence of PLE spectra will be reported elsewhere. The calculation we made in this paper neglects the all kinds of many-body effects. This is why it cannot reproduce the sharp excitonic absorption peaks due to bound states (X, X-) observed at low ne. By the same reason, the theoretical emission spectra at high ne are inconsistent with the experimental PL spectra where we observed significant red shift of low energy shoulder (BE) and broadening with increasing ne. The red shift of BE shoulder with 2meV from the position of X- peak corresponds to the shrinkage of band gap energy due to the many-body effect known as Band Gap Renormalization [7]. The origin of the increase of half-width-of-half-maximum of PL peak from 0.5meV (at 0.2V) to 2meV (at 0.7V) is currently not understood. We should notice that the sharp emission peak of calculated spectrum in Fig.1 (b) results from the small value of (0.2meV), which is chosen to reproduce the double absorption peak structure at Vg=0.35V markedly. Quantitative plots of experimental results for 1D system are presented in the left side of Fig.2. The bottom figure (a) gives the main PLE peak energy of X (solid circles), X- (solid triangles), FE (solid squares), and the PL energy of BE shoulder (blank squares) as a function of gate voltage. Fig.2 (b) plots the energy separation X-X- (solid inverse-triangles) and Fermi energy (blank inverse-triangles) estimated FIG. 3 Normalized experimental (a) and theoretical (b) spectra of PL (dotted line) and PLE (solid line) for 2D arm well at various electron density. by the calculation from the corresponding electron density shown in Fig.1 (b) using the following relation. 2 2 ne 2 Ef 8me We also plot the PLE maximum ratio of X (solid circles), X- (solid triangles) and FE (solid squares) in Fig.2 (c). With these results for 1D system in mind, we will now take a look at the results for 2D system. Since 2D electron gas is formed in the arm well (one of the quantum well composing T-shaped quantum wire), we can measure the optical spectra of 2D system by changing the position of sample as illustrated in the inset of Fig.3. Figure 3 (a) shows normalized PL (dotted lines) and PLE (solid lines) spectra measured for 2D electron system in the arm well, and (b) shows the theoretical calculation of the free particle approximation with step-functional 2D DOS. In the same way as 1D system, we plot, in the right side of Fig.2, (d) the peak energy of PL and PLE, (e) the X,X- splitting and Fermi energy, and (f) ratio of PLE maximum value as a function of gate voltage. From the PLE spectra measured for 2D system, we found following: First, there are always two absorption peaks in the presence of 2D electron gas (at Vg=0.30.8V): the peak which evolves from X and that from X-. As ne increases, the OS transfers gradually from X to X-, and the splitting of X and X- increases nonlinearly from 1.5meV to 8meV. Second, the evolution from X- to FE occurs smoothly by single peak with increasing ne. FE shows typical asymmetrical peak line shape that is not consistent of the free-particle calculation shown in the top line of Fig.3 (b). These results for 2D system, especially the asymmetrical peak at FE, remind us the many-body enhancements known as Fermi edge singularity. Indeed, the observed evolution of optical structures is analogous to the numerical calculation including FES effect and also electronic spin effect [8]. The fact that these FES theories appear to agree with the measured optical properties of 2D electron system has been verified by several experiments by other groups [9]. In 1D system, however, the evolution of PLE spectra shows a slightly different story. Now, let us discuss the difference between results of 1D system and those of 2D system, focusing on the PLE spectra. The sharp excitonic peaks (X, X-) observed at low ne for both 1D and 2D system show interesting differences of dimensionality. In 1D system, we observe drastic OS transfer from X to X- with increasing ne, and X- completely dominates the PLE spectrum at 0.2V. In 2D system, on the contrary, X peak is still detectable at high ne, and there are no ranges of ne where X- completely dominates the spectrum. This difference is observed for the first time and provides us an answer to the fundamental question ”How are the bound states formed in the presence of 1D (2D) electron gas? ” as discussed below. In theoretical terms, the exciton has to be orthogonal to all the lower-lying three-particle states [10]. As ne increases, the available unoccupied states for the exciton formation decrease due to phase-space filling. This occurs significantly in 1D system, because the amount of DOS at large wave number is small due to the inverse-square-root divergence feature. Thus, X of 1D system loses its intensity drastically with increasing ne compared to that of 2D system. In other words, the enhancement of OS of trion state in 1D system can be interpreted as the OS concentration into the lowest ground state resulted from 1D DOS singularity. The crossover region from X- to FE reflects the difference of DOS more directly. In 1D system, we observe a characteristic double peak structure corresponding band bottom singularity and Fermi edge. In 2D system, the evolution from X- to FE occurs smoothly by single peak with increasing ne, which is consistent with the fact that band bottom of the stepfunctional 2D DOS does not have such a sharp singularity as 1D case. It is surprising that we succeed to observe the divergence feature of 1D DOS so clearly in the optical spectrum. To our knowledge, the 1D DOS singularity has not been observed directly in experiments so far, because this anomaly could disappear due to the inhomogeneous broadening, and also due to the Coulomb interaction between electron and hole [5]. Indeed, because of the Coulomb-induced origin, the PLE spectrum measured for non-doped quantum wires of high quality shows a reduction of the absorption at the continuum state, i.e., the Sommerfeld factor is less than 1 in 1D system [4]. We guess that the screening effect of Coulomb interaction due to the doped electron gas plays an important role for the observation of 1D DOS without Coulomb-induced modification. Equally striking is that Fermi edge enhancement due to many-body effects in 1D system seems weaker than that in 2D system. In other words, the PLE spectra of 1D system at high ne show good agreement with the free-particle calculation, while those of 2D system are not consistent. This result contrasts with the widely used interpretation that the FES effect should become significant in 1D system due to larger many-body interaction induced by 1D confinement and also due to smaller hole recoil effects [11]. It is currently unclear for us what causes the weak FES effect in 1D system. We need further investigations. In summary, we measured the PL and PLE spectra on an n-type doped single quantum wire with a gate to tune the electron density. We observed drastic OS transfer from excitons to trions with increasing ne, which results from 1D character that OS concentrates into the lowest bound state. Furthermore, we found characteristic double peak structure near metalinsulator crossover. We interpret this double peak corresponds to the coexistence of Fermi edge and the inverse-square-root divergence of 1D DOS at the band edge, and confirm this conclusion by the comparison with free-particle calculation and also with the results for 2D system. This work was partly supported by a Grant-in-Aid from the Ministry of Education, Culture, Sports, Science, and Technology, Japan. [1]未定 [2]未定 [3]未定 [4] Akiyama et al. App. Phys. Lett. 82, 379 (2003), Itoh et al. App. Phys. Lett. 83, 2043 (2003). [5] Ogawa et al. Phys. Rev. B 43, 14325 (1991), Rossi et al. Phys. Rev. Lett. 76, 3642 (1996). [6] Akiyama et al. Solid State Commun. 122, 169 (2002). [7]未定 [8] Hawrylak et al. Phys. Rev. B 44, 3821 (1991), Takagiwa et al. J. Phys. Chem. Solids 63, 1587 (2002). [9] Huard et al. Phys. Rev. Lett. 84, 187 (1999), Yusa et al. Phys. Rev. B 62, 15390 (2000), Kaur et al. Phys. Status Solidi B 178, 465 (2000). [10] Esser et al. Phys. Status Solidi B 227, 317 (2001) [11] Calleja et al. Solid State Commun. 79, 911 (1991) <以下、文献選びのためのメモ書き。> 関連の強い文献。 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 3 \\duke\temp\toshi_soft\pdf\Huard_PRL_84_187.pdf 4 \\duke\temp\toshi_soft\pdf\Yusa_PRB_62_15390.pdf 5 \\duke\temp\toshi_soft\pdf\Fritze_PRB_48_4960.pdf 7 \\duke\temp\toshi_soft\pdf\Hawrylak_PRB_44_3821.pdf 8 \\duke\temp\toshi_soft\pdf\Ogawa_PRL_68_3638.pdf 9 \\duke\temp\toshi_soft\pdf\Rodriguez_PRB_47_1506.pdf 10 \\duke\temp\toshi_soft\pdf\Ruckenstein_PRB_35_7551.pdf 11 \\duke\temp\toshi_soft\pdf\Akiyama_SSC_122_169.pdf 15 \\duke\temp\toshi_soft\pdf\Oberli_PhysicaE_11_224.pdf 17 \\duke\temp\toshi_soft\pdf\Takagiwa_JPCS_63_1587.pdf 18 \\duke\temp\toshi_soft\pdf\Kaur_PSSa_178_465.pdf 22 \\duke\temp\toshi_soft\pdf\Skolnick_PRL_58_2130.pdf 25 \\duke\temp\toshi_soft\pdf\Mueller_PRB_42_11189.pdf 27 \\duke\temp\toshi_soft\pdf\Melin_PRL_85_852.pdf 37 \\duke\temp\toshi_soft\pdf\Finkelstein_PRL_74_976.pdf 47 \\duke\temp\toshi_soft\pdf\Delalande_PRL_59_2690.pdf 50 \\duke\temp\toshi_soft\pdf\Ogawa_PRB_43_14325.pdf 51 \\duke\temp\toshi_soft\pdf\Ogawa_PRB_44_8138.pdf 54 \\duke\temp\toshi_soft\pdf\Rossi_PRL_76_3642.pdf 57 \\duke\temp\toshi_soft\pdf\DasSarma_PRL_84_2010.pdf 59 \\duke\temp\toshi_soft\pdf\Rinaldi_PRB_59_2230.pdf 69 \\duke\temp\toshi_soft\pdf\Akiyama_JPCM_10_3095.pdf 90 \\duke\temp\toshi_soft\pdf\Kalt_PRB_40_12017.pdf 145 \\duke\temp\toshi_soft\pdf\Akiyama_APL_82_379.pdf 159 \\duke\temp\toshi_soft\pdf\Itoh_APL_83_2043.pdf 203 \\duke\temp\toshi_soft\pdf\Stebe_PRB_58_9926.pdf 208 \\duke\temp\toshi_soft\pdf\Stebe_SAM_5_545.pdf 255 \\duke\temp\toshi_soft\pdf\Brown_PRB_56_3937.pdf 352 \\duke\temp\toshi_soft\pdf\Esser_PSSb_227_317.pdf 353 \\duke\temp\toshi_soft\pdf\Stopa_PRB_63_195312.pdf 354 \\duke\temp\toshi_soft\pdf\Combescot_SSC_128_273.pdf 357 \\duke\temp\toshi_soft\pdf\esser_PSSa_178_489.pdf 365 \\duke\temp\toshi_soft\pdf\Otterburg_PRB_71_033301.pdf 379 \\duke\temp\toshi_soft\pdf\Cox_PRB_69_235303.pdf 393 \\duke\temp\toshi_soft\pdf\Raraport_PSSb_227_419.pdf 396 \\duke\temp\toshi_soft\pdf\Brunhes_PRB_60_11568.pdf 415 \\duke\temp\toshi_soft\pdf\Tischler_PRB_66_081310.pdf ※ そのほか、重要な参考文献の内容 ① Trion は低次元系で束縛エネルギーが増加して、 顕著に観測されるものであり[Stebe208]、一次元 系の方がより観測されやすいという指摘もある [Combescot354]。 ② Trion を介した Metal-Insulator crossover は、低 次元電子系で顕著に観測されるものであることが 理論的に指摘されている[Stebe208, Combescot354, Takagiwa17, Esser352, hawrylak7]。実験的には、 量子井戸に形成される二次元電子系で観測されて いる[Huard3, Yusa4, Kaur18, Finkelstein37, cox379]。 ③ 多体効果の次元性の影響は興味深く、様々に議 論されている。特に trion 理論・FES 理論が注目 されている。 ・一次元の trion の理論 Esser352、 ・一次元の FES の理論 Ogawa8, Hawrylak13 ・二次元・三次元の trion の理論 Stebe203 ・一次元の trion の実験 akiyama11, otterburg365 ・ 一 次 元 の FES の 実 験 akiyama11, Oberli15, calleja12, Fritze5 次元性の影響を調べるに当たって、多体効果が 温度や正孔質量、higher subband に対して非常に 敏感である点は無視できない。これは実験的 [Melin27, Skolnick17, Brown255, Esser357]にも、理 論 的 [Hawrylak7, Ruckenstein10, Mueller25, Rodigues9]にも指摘されている点である。試料品 質や測定条件をできる限り同じにして 1D・2D を 測定することは重要であると考える。 ④ そのほか、 ・ Weak BGR in 1D electron system [Cingolani59, Stopa353] ・2D では X+X-の振動子強度が一定となる実験結 果[Cox379] ・X-の Line shape analysis :低エネルギー側に多 体効果が現れる[Esser352, Esser357] などとの関連も興味深い