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Physical review. B, Condensed matter

Theory of femtosecond photon-echo decay in semiconductors

S. V. Gantsevich, V. L. Gurevich, Д. А. Паршин, Д. А. Паршин

Published Nov 15, 1995• 2 citations
Publisher

Abstract

We investigate a mechanism responsible for the observed very short times of the photon-echo decay (of the order of a few femtoseconds) in semiconductors. It is associated with the loss of phase memory as a result of the interaction of the interband mixed state with an unscreened random Coulomb potential of the photocarriers and/or charged impurities. A time characteristic of a system of interacting electrons is found. This is the time of phase breaking ${\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}$, which we calculate within the eikonal approximation using diagrammatic techniques. ${\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}$ is shown to be typically much shorter than both the time of electron-electron collisions and the period of plasma oscillations. We demonstrate that the screening of Coulomb potential cannot be built up during this time. ${\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}$ is proportional to ${\mathit{n}}^{\mathrm{\ensuremath{-}}1/\mathit{d}}$ (where n is the carrier concentration and d the dimensionality of a system), which is consistent with the experimental results. The derived law of echo decay of the form exp[-(\ensuremath{\tau}/${\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}$${)}^{\mathit{d}}$] agrees with the results of numerical simulation, although it does not agree with the existing results of physical experiment. We believe that such a disagreement is of a fundamental nature and manifests a basic need for further experimental and theoretical work.

DOI
10.1103/physrevb.52.14006

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We investigate a mechanism responsible for the observed very short times of the photon-echo decay (of the order of a few femtoseconds) in semiconductors. It is associated with the loss of phase memory as a result of the interaction of the interband mixed state with an unscreened random Coulomb potential of the photocarriers and/or charged impurities. A time characteristic of a system of interacting electrons is found. This is the time of phase breaking \ensuremathτcphi{\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}\ensuremathτcphi​, which we calculate within the eikonal approximation using diagrammatic techniques. \ensuremathτcphi{\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}\ensuremathτcphi​ is shown to be typically much shorter than both the time of electron-electron collisions and the period of plasma oscillations. We demonstrate that the screening of Coulomb potential cannot be built up during this time. \ensuremathτcphi{\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}\ensuremathτcphi​ is proportional to n\ensuremath−1/d{\mathit{n}}^{\mathrm{\ensuremath{-}}1/\mathit{d}}n\ensuremath−1/d (where n is the carrier concentration and d the dimensionality of a system), which is consistent with the experimental results. The derived law of echo decay of the form exp[-(\ensuremath{\tau}/{\mathrm{\ensuremath{\tau}}}_{\mathit{c}\mathit{p}\mathit{h}\mathit{i}}$${)}^{\mathit{d}}] agrees with the results of numerical simulation, although it does not agree with the existing results of physical experiment. We believe that such a disagreement is of a fundamental nature and manifests a basic need for further experimental and theoretical work.
The availability of femtosecond pulses in the optical-frequency regime allows the study of coherent effects in the interaction between semiconductors and light. Because the properties of the exciting pulses become important ingredients in spectroscopy, the theoretical analysis must treat the complete time dependence of the system. For this purpose we use the semiconductor Bloch equations (SBE),1-3 which are the coupled equations of motion for the interband polarization and the electron and hole populations for an interacting electron-hole system in the random-phase approximation. The equations describe the electron-hole Coulomb attraction leading to excitonic features; they contain phasespace filling and band-gap renormalization effects, as well as the dipole interaction with the applied light field.
We report the first observation of femtosecond photon echoes from the band-to-band transitions in a bulk semiconductor. The time decay of the echo, found to vary from 3.5 to 11 fs, has allowed us to determine the polarization dephasing rate in GaAs. This rate was found to depend on the carrier density in the experimental range covered, 1.5\ifmmode\times\else\texttimes\fi{}1017{10}^{17}1017 to 7\ifmmode\times\else\texttimes\fi{}1018{10}^{18}1018 ${\mathrm{cm}}^{\ensuremath{-}3}$, indicating the dominance of carrier-carrier scattering as the principal dephasing mechanism. The observed functional dependence of the dephasing rate on the carrier density has yielded previously unavailable information on Coulomb screening in a nonequilibrium carrier distribution.
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​.
The phase relaxation of optically excited electronic states can be studied in fourwave mixing experiments where three excitation pulses at t = 0, t =t21, and t = T, respectively, interact via the third-order polarization of the medium to generate a nonlinear signal whose intensity depends on the dephasing time T2. For inhomogeneously broadened optical transitions the signal will be emitted as a time delayed photon echo pulse at t = T + t21 provided the pulse duration is short compared with T2. The echo amplitude decays as exp(−4t21/T2).1
We report femtosecond photon echo and four-wave mixing measurements performed on GaAs/AlGaAs heterostructure at room temperature. In femtosecond photon echo experiment the dephasing time was obtained, found to vary between 40 and 55 fs depending on carrier density. The dependence showed a power-law behavior T 2 ∝ N -0.22 , which indicates that major phase coherence loss is due to screened Coulomb electron-electron interaction. Transient grating experiments yielded the electron diffusion coefficient value of 200 cm 2 /s and electron relaxation time equal to 3 ns.