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Physical review. B, Condensed matter

Quantum-kinetic dephasing in resonantly excited semiconductor quantum wells

B. Mieck, H. Haug, Werner Hügel, M. F. Heinrich, Martin Wegener

Published Jul 15, 2000• 36 citations
Publisher

Abstract

We investigate resonant time-resolved four-wave mixing on GaAs quantum wells at $T=300\mathrm{K}$ and at elevated carrier densities using excitation with 11 fs optical pulses. The experiments are compared with non-Markovian quantum-kinetic calculations including carrier-carrier and carrier-LO-phonon scattering. A self-consistently determined two-time-dependent screened random-phase approximation Coulomb potential is used for the carrier-carrier scattering. In experiment and theory we find an unusual real-time response, which is far from an ideal photon echo. Surprisingly, we also find that the dependence of the decay time \ensuremath{\tau} of the four-wave-mixing signal versus the optically excited nonequilibrium electron-hole pair density ${n}_{\mathrm{eh}}$ is quantitatively similar to the corresponding behavior of bulk GaAs. Thus both data sets can be fitted by the same form ${\ensuremath{\tau}}^{\ensuremath{-}1}={\ensuremath{\tau}}_{0}^{\ensuremath{-}1}{+cn}_{\mathrm{eh}}^{1/3}.$ This is not consistent with previous experimental work in a more limited range of carrier densities, which determined different behavior for quasi-two-dimensional (2D) and 3D, i.e., exponents of 0.3 and $0.55\ifmmode\pm\else\textpm\fi{}0.04,$ respectively.

DOI
10.1103/physrevb.62.2686

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We investigate resonant time-resolved four-wave mixing on GaAs quantum wells at T=300KT=300\mathrm{K}T=300K and at elevated carrier densities using excitation with 11 fs optical pulses. The experiments are compared with non-Markovian quantum-kinetic calculations including carrier-carrier and carrier-LO-phonon scattering. A self-consistently determined two-time-dependent screened random-phase approximation Coulomb potential is used for the carrier-carrier scattering. In experiment and theory we find an unusual real-time response, which is far from an ideal photon echo. Surprisingly, we also find that the dependence of the decay time \ensuremath{\tau} of the four-wave-mixing signal versus the optically excited nonequilibrium electron-hole pair density neh{n}_{\mathrm{eh}}neh​ is quantitatively similar to the corresponding behavior of bulk GaAs. Thus both data sets can be fitted by the same form \ensuremathτ\ensuremath−1=\ensuremathτ0\ensuremath−1+cneh1/3.{\ensuremath{\tau}}^{\ensuremath{-}1}={\ensuremath{\tau}}_{0}^{\ensuremath{-}1}{+cn}_{\mathrm{eh}}^{1/3}.\ensuremathτ\ensuremath−1=\ensuremathτ0\ensuremath−1​+cneh1/3​. This is not consistent with previous experimental work in a more limited range of carrier densities, which determined different behavior for quasi-two-dimensional (2D) and 3D, i.e., exponents of 0.3 and 0.55\ifmmode±\else\textpm\fi0.04,0.55\ifmmode\pm\else\textpm\fi{}0.04,0.55\ifmmode±\else\textpm\fi0.04, respectively.
We show that the coherent response of semiconductor band-to-band continuum transitions at room temperature, excited by 11 fs pulses at elevated carrier densities, deviates substantially from that expected for an ideal photon echo. A microscopic non-Markovian quantum kinetic theory of both electron-electron and electron-LO-phonon scattering reproduces these unusual experimental observations qualitatively and, furthermore, the famous scaling of the decay time $\ensuremath{\tau}$ with carrier density neh{n}_{\mathrm{eh}}neh​ according to ${\ensuremath{\tau}}^{\ensuremath{-}1}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}{\ensuremath{\tau}}_{0}^{\ensuremath{-}1}{+cn}_{\mathrm{eh}}^{1/3}$ quantitatively. $\ensuremath{\tau}$, however, cannot be associated with a single unique phase relaxation time T2{T}_{2}T2​.
We have studied the coherent emission from bulk semiconductors by spectrally resolved and spectrally integrated four-wave mixing (FWM) with broadband 16-fs pulses in the carrier density range from $1\ifmmode\times\else\texttimes\fi{}{10}^{16}{\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$ to $6\ifmmode\times\else\texttimes\fi{}{10}^{17}{\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}.$ In GaAs, only continuum transitions are excited, while both excitonic and continuum transitions are excited in Al0.06Ga0.94As.{\mathrm{Al}}_{0.06}{\mathrm{Ga}}_{0.94}\mathrm{As}.Al0.06​Ga0.94​As. The decay of the FWM signal for positive time delays unambiguously reflects the dephasing of the continuum, irrespective of the excitation of excitonic transitions. We find identical ultrafast sub-20-fs decay times of the coherent emission from continuum transitions in GaAs and Al0.06Ga0.94As,{\mathrm{Al}}_{0.06}{\mathrm{Ga}}_{0.94}\mathrm{As},Al0.06​Ga0.94​As, independent of the excess excitation energy. These decay times depend only weakly on the carrier density for densities below ${10}^{17}{\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}.$ The continuum dephasing is analyzed considering carrier-carrier and carrier-LO-phonon scattering in a relaxation rate approach. The excitonic transitions in Al0.06Ga0.94As{\mathrm{Al}}_{0.06}{\mathrm{Ga}}_{0.94}\mathrm{As}Al0.06​Ga0.94​As dominate the FWM signal at negative time delays.
Summary form only given. We performed a comprehensive four-wave-mixing (FWM) study of the optical dephasing in bulk GaAs and AlGaAs with broadband 16-fs laser pulses. In contrast to previous work, spectral resolution has allowed us to unambiguously relate the decay of the coherent emission to either continuum or excitonic transitions. We have extended earlier measurements of continuum dephasing to one order of magnitude lower carrier densities. We find much shorter dephasing times and a much weaker density dependence of the dephasing than expected from the extrapolation of the high-density results. Our data indicate that a quantum kinetics model for both Coulomb and LO-phonon scattering is required to describe continuum dephasing on the 10-fs time scale at lower densities.
We report a strong (300:1) excitonic resonance in time-resolved (100 fs) four-wave mixing in GaAs quantum wells as a function of the incident photon energy and show that it results from the large difference in the dephasing rates of excitons and free carriers. We conclude that excitons dominate even when they make up only a small fraction of the excited states. These results, in conjuction with new results in exciton-phonon scattering, provide new insights into previous studies performed with spectrally broad ultrashort pulses.
Oscillations of the transient four-wave-mixing signal with a period of about 100fs100\mathrm{fs}100fs are observed in bulk GaAs using 14 fs pulses tuned to the exciton resonance at low temperatures. The measurements are explained in terms of the non-Markovian quantum kinetics for electron-hole pairs due to LO-phonon scattering. It is shown that the observed oscillations are evidence for memory effects. The experiments provide a first test of the central ideas of quantum kinetics, in which the effects of quantum coherence and of dissipation are intrinsically connected.
We investigate the temporal evolution of the instantaneous frequency of ultrashort-pulse four-wave mixing in GaAs/Gax{\mathrm{Ga}}_{\mathit{x}}Gax​${\mathrm{Al}}_{1\mathrm{\ensuremath{-}}\mathit{x}}$As quantum-well structures. We find that the coherent light emitted by excitons exhibits a complex phase behavior which depends critically on the density of excitons and the central frequency of the exciting pulses. Depending on the excitation conditions, we observe nonlinear shifts of the instantaneous frequency within one ultrashort pulsed emission or quantum beats. In the latter case we determine that the beat \ensuremath{\pi}-phase shift is very fast, only 40% above the fundamental quantum limit. We also present elaborate numerical simulations of the experiments based on a six-band generalization of the semiconductor Bloch equations. This formalism takes into account Coulomb many-body interactions and Pauli exclusion. It reproduces the salient features of the experimental data. It fails to account for important details revealed by the very sensitive phase measurements. The discrepancies can be traced back to two approximations in the theory: the statical treatment of screening, and the Lorentzian description of dephasing. In both cases, this indicates the need for theoretical refinements requiring a microscopic description of Coulomb scattering and dephasing processes in a non-Markovian theory.