Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Journal of the Optical Society of America B

Picosecond phase coherence and orientational relaxation of Wannier excitons in GaAs

Lothar Schultheis, J. Kühl, A. Honold, C. W. Tu

Published Jun 9, 1986• 0 citations
OpenAlex

Abstract

The energy levels of Wannier excitons in a thin (≈200-nm) semiconductor layer are quantized because of confinement and are characterized by the wave vector parallel to the layer k║. In contrast to bulk semiconductors, polariton effects which strongly modify the excitonic dispersion curve leading to polariton transport phenomena in a coherent optical experiment are not expected.1 Thus, in an optically thin semiconductor layer, purely excitonic coherence properties can be studied.

Related papers

Picosecond dephasing and energy relaxation of excitons in semiconductors

Yasuaki Masumoto

Picosecond relaxation processes of excitons, including dephasing processes, are systematically studied in CuCl, CdSe and GaAs/AlAs MQW (multi-quantum well structures) by observing time-resolved induced absorption, luminescence and non-degenerate four-wave mixing. By studying the transient induced absorption from the exciton (polariton) state to the excitonic molecule state, time-resolved energy distribution of excitons in CuCl is determined (Fig.1).1) Another technique, i.e. time-resolved luminescence measurement, is applied to excitons in CdSe and GaAs/AlAs MQW (Figs.2 and 3).2,3) By analyzing the above-mentioned experiments the distribution of excitons in the two-dimensional energy-time coordinates is successfully determined. Thus, energy relaxation processes of excitons are clearly visualized. Prior to energy relaxation, coherently generated excitons are considered to be dephased. Phase relaxation of excitons in CuCl is directly measured for the first time in the picosecond time domain by means of time-resolved non-degenerate four-wave mixing (Fig.4).4) These new techniques will be demonstrated and the dephasing as well as energy relaxation mechanism of excitons and excitonic polaritons will be discussed. In the above experiments characteristics of a picosecond tunable optical parametric oscillator pumped by a mode-locked Nd3+:YAG laser as well as a picosecond tunable dye laser synchronously pumped by a mode-locked ion laser are complementarily utilized.

International Conference on Ultrafast Phenomena•Jan 1, 1984•0 citations

Picosecond Dynamics in Optically ExcitedSemiconductors: Exciton Dephasing,Ionization Equilibrium and Pauli Blocking

Rocharj Mondal

Excitons, the bound states of an electron and a hole, in semiconductors are interesting objects and they continue to attract attention of researchers from all over the world. Despite intense research on exciton physics over last three-four decades, many interesting phenomena related to the dynamics and the nonlinear optical properties of excitons in semiconductors and their nanostructures in the coherent and incoherent regimes are still to be explored. This thesis presents our effort to study the nonlinear optical properties as well as the exciton dynamics in coherent and incoherent regime in semiconductor nanostructures including GaAs quantum wells (QWs) and InAs quantum dots (QDs). We have set up several time-resolved and steady-state optical spectroscopic measurement techniques in our laboratory to carry out our study on excitons dynamics in semiconductor QWs and QDs. We work out a clear and detailed theory of the pump-probe signal taking account of all aspect of the measurement, namely, the lock-in detection, spectral selection by the monochromator and time-integration at the slow photodetector. We have used the formalism of optical Bloch equations conventionally used to analyse wave mixing experiments. Our analysis puts the pump-probe technique on the same footing as the wave mixing experiments. We show that pumpprobe experiments can be used to study both coherent and incoherent dynamics. We also present a clear physical picture of the measured signal using the Lorentz harmonic oscillator model. We report the investigation of the coherent exciton dephasing dynamics using pumpprobe reflectivity measurement in GaAs QWs for resonant excitation. Two GaAs/AlGaAs QWs with well thicknesses 8 nm and 17.5 nm are used. We found a strong dependence of the dephasing rate of the excitons with increasing exciton density due to exciton-exciton scattering. We found that the exciton dephasing rate of 8 nm QWs at low excitation density and at low lattice temperature is larger than the corresponding dephasing rate of the 17.5 nm QWs, possibly due to larger effect of inhomogeneous broadening. We also report that the dephasing rates for both QWs are linear with the sample temperature below the 30 K. We report the study of ionization equilibrium between the exciton and the electronhole plasma population in the temperature and pressure (excitation density) phase space. Non-resonant excitation of semiconductor creates a nonequilibrium state of electron-hole plasma. We investigate this ionization equilibrium using steady state photoluminescence and time-resolved excitation correlation PL measurements. We present a clear phase diagram (in temperature and carrier density phase space) of this ionization process.A clear density-dependent increase in the ionization ratio is observed and its connection with the Mott transition is discussed. Semiconductor nanocrystals and QDs are another important area of research, mainly due to their huge potential for device application. We present a simple model which combines carrier loss kinetics, detailed balance principle in thermodynamic equilibrium and Pauli exclusion principle to quantitatively explain the observed behaviour of the experimental data.

•Sep 1, 2015•0 citations

Sub-relaxation and sub-dephasing dynamics of light-induced polarization in semiconductors.

B. Fluegel

Using laser pulses of duration comparable to semiconductor relaxation and dephasing times, the coherent phenomena common to two-level systems have been demonstrated in II-VI and III-V semiconductors. These light-matter interactions are characterized by electrons and holes in their initially excited states and/or a macroscopic polarization that persists after the excitation. A nonthermal carrier distribution was observed in bulk CdSe, demonstrating the extremely fast energy relaxation possible when carrier-LO-phonon scattering is included. Quantum-confined CdSe microcrystallites were then employed to limit the available decay avenues. The one and two-pair transitions were characterized, and using spectral hole-burning, energy relaxation was shown to be substantially slower than in bulk. Dipole dephasing remained very rapid. Persistent macroscopic polarization was demonstrated in semiconductors through pump and probe experiments conducted on time scales faster than the inverse linewidth of the exciton. In the first set of experiments, it was found that the exciton optical Stark shift deviates from that predicted by a steady-state theory. The shift is smaller than expected and lasts longer than the pump pulse. Both effects are explained by free evolution of the exciton's polarization. Transient exciton bleaching is observed and shown to be a result of adiabatic following. In a second study of coherent polarization, spectral oscillations at negative delay times were studied. Oscillations were measured in a wide variety of semiconductors, temporally preceding several different pump-probe phenomena. By comparison with a semiclassical theory, it was shown that spectral oscillations in the spectral region of the exciton are evidence of persistent exciton polarization. Oscillations in the band are due to four wave mixing of the pump and probe beams.

•Jan 1, 1992•0 citations

Ultrafast and large nonlinear optical response of excitons weakly confined in a semiconductor thin film

Toshiro Isu, Koichi Akiyama, Nobuyuki Tomita +3 more

We observe ultrafast and large nonlinear optical responses of a semiconductor thin film where excitons are weakly confined and their center-of-mass motion is quantized. The observed degenerate four-wave mixing (DFWM) signal of a GaAs double-hetero-structure layer exhibits an anomalous thickness-dependence, and is much enhanced at the thickness of 110nm. The decay time of the response is the order of ps, which depends on the thickness of the layer and on the number of the layer. These phenomena are elucidated by the theory of the nonlocal interaction between excitonic states and the light beyond the long wavelength approximation regime. The enhancement at the thickness is due to the size-resonant enhancement of the internal field with a nano-scale spatial structure, where the second quantized level of the exciton center-of-mass motion mainly contributes to the large response at the thickness. We, furthermore, demonstrate ultrafast response in a reflective type nonlinear polarization rotation switch with the 110nm thick three double-hetero. The signal intensity of 20% for the reflective pulse was obtained at a pump intensity of 10nJ/cm2, and the decay time is 1.5ps at low temperatures. These results provide a novel design of a semiconductor structure in order to obtain both large and ultrafast nonlinear response that is suitable for device application.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Jun 2, 2003•1 citation

Dynamics of Below-Gap Photoexcitation in GaAs Quantum Wells

Jane E. Zucker, A. VonLehmen, D. S. Chemla +1 more

We have identified several physical processes by which below-gap photons can modify excitonic absorption in GaAs quantum wells.1-3 These different phenomena can be distinguished by their temporal response times, which range from tens of nanoseconds to less than one picosecond. Our experiments also show that the relative contributions of these mechanisms to below-gap optical modulation of exciton absorption depend strongly on temperature as well as on the wavelength of the below-gap modulating beam. The size of the modulation indicates that a new class of absorptive and dispersive devices for optical signal processing is possible in which signals propagate in the transparent region of the crystal and experience negligible attenuation. In order to successfully interpret and calculate the magnitude of these exciting new effects, we show that it is necessary to take into account the special properties of two-dimensional excitons in semiconductor quantum wells.

Topical Meeting on Picosecond Electronics and Optoelectronics•Jan 1, 1987•0 citations

Coherent control of a semiconductor qubit in the strong coupling regime: Impact of energy and phase relaxation mechanisms

Alexandre Enderlin, M. Ravaro, V. Voliotis +2 more

We report on coherent control of the fundamental exciton state in a single quantum dot by means of two phase-locked picosecond laser pulses. By analyzing the experiments performed in the Rabi regime and comparing them to numerical simulations, we show that we can address the exciton coherence and get an insight into the involved dephasing processes. The total decoherence time ${T}_{2}$ (170 ps) is comparable to the effective exciton lifetime ${T}_{1}$ (200 ps), although not reaching the upper theoretical limit of $2{T}_{1}$. We conclude that energy relaxation and pure dephasing processes due to virtual scattering with phonons both contribute on an equal footing to the loss of coherence in this kind of monolayer-step-induced GaAs quantum dots.

Physical Review B•Aug 4, 2009•9 citations
The energy levels of Wannier excitons in a thin (≈200-nm) semiconductor layer are quantized because of confinement and are characterized by the wave vector parallel to the layer k║. In contrast to bulk semiconductors, polariton effects which strongly modify the excitonic dispersion curve leading to polariton transport phenomena in a coherent optical experiment are not expected.1 Thus, in an optically thin semiconductor layer, purely excitonic coherence properties can be studied.
Picosecond relaxation processes of excitons, including dephasing processes, are systematically studied in CuCl, CdSe and GaAs/AlAs MQW (multi-quantum well structures) by observing time-resolved induced absorption, luminescence and non-degenerate four-wave mixing. By studying the transient induced absorption from the exciton (polariton) state to the excitonic molecule state, time-resolved energy distribution of excitons in CuCl is determined (Fig.1).1) Another technique, i.e. time-resolved luminescence measurement, is applied to excitons in CdSe and GaAs/AlAs MQW (Figs.2 and 3).2,3) By analyzing the above-mentioned experiments the distribution of excitons in the two-dimensional energy-time coordinates is successfully determined. Thus, energy relaxation processes of excitons are clearly visualized. Prior to energy relaxation, coherently generated excitons are considered to be dephased. Phase relaxation of excitons in CuCl is directly measured for the first time in the picosecond time domain by means of time-resolved non-degenerate four-wave mixing (Fig.4).4) These new techniques will be demonstrated and the dephasing as well as energy relaxation mechanism of excitons and excitonic polaritons will be discussed. In the above experiments characteristics of a picosecond tunable optical parametric oscillator pumped by a mode-locked Nd3+:YAG laser as well as a picosecond tunable dye laser synchronously pumped by a mode-locked ion laser are complementarily utilized.
Excitons, the bound states of an electron and a hole, in semiconductors are interesting objects and they continue to attract attention of researchers from all over the world. Despite intense research on exciton physics over last three-four decades, many interesting phenomena related to the dynamics and the nonlinear optical properties of excitons in semiconductors and their nanostructures in the coherent and incoherent regimes are still to be explored. This thesis presents our effort to study the nonlinear optical properties as well as the exciton dynamics in coherent and incoherent regime in semiconductor nanostructures including GaAs quantum wells (QWs) and InAs quantum dots (QDs). We have set up several time-resolved and steady-state optical spectroscopic measurement techniques in our laboratory to carry out our study on excitons dynamics in semiconductor QWs and QDs. We work out a clear and detailed theory of the pump-probe signal taking account of all aspect of the measurement, namely, the lock-in detection, spectral selection by the monochromator and time-integration at the slow photodetector. We have used the formalism of optical Bloch equations conventionally used to analyse wave mixing experiments. Our analysis puts the pump-probe technique on the same footing as the wave mixing experiments. We show that pumpprobe experiments can be used to study both coherent and incoherent dynamics. We also present a clear physical picture of the measured signal using the Lorentz harmonic oscillator model. We report the investigation of the coherent exciton dephasing dynamics using pumpprobe reflectivity measurement in GaAs QWs for resonant excitation. Two GaAs/AlGaAs QWs with well thicknesses 8 nm and 17.5 nm are used. We found a strong dependence of the dephasing rate of the excitons with increasing exciton density due to exciton-exciton scattering. We found that the exciton dephasing rate of 8 nm QWs at low excitation density and at low lattice temperature is larger than the corresponding dephasing rate of the 17.5 nm QWs, possibly due to larger effect of inhomogeneous broadening. We also report that the dephasing rates for both QWs are linear with the sample temperature below the 30 K. We report the study of ionization equilibrium between the exciton and the electronhole plasma population in the temperature and pressure (excitation density) phase space. Non-resonant excitation of semiconductor creates a nonequilibrium state of electron-hole plasma. We investigate this ionization equilibrium using steady state photoluminescence and time-resolved excitation correlation PL measurements. We present a clear phase diagram (in temperature and carrier density phase space) of this ionization process.A clear density-dependent increase in the ionization ratio is observed and its connection with the Mott transition is discussed. Semiconductor nanocrystals and QDs are another important area of research, mainly due to their huge potential for device application. We present a simple model which combines carrier loss kinetics, detailed balance principle in thermodynamic equilibrium and Pauli exclusion principle to quantitatively explain the observed behaviour of the experimental data.
Using laser pulses of duration comparable to semiconductor relaxation and dephasing times, the coherent phenomena common to two-level systems have been demonstrated in II-VI and III-V semiconductors. These light-matter interactions are characterized by electrons and holes in their initially excited states and/or a macroscopic polarization that persists after the excitation. A nonthermal carrier distribution was observed in bulk CdSe, demonstrating the extremely fast energy relaxation possible when carrier-LO-phonon scattering is included. Quantum-confined CdSe microcrystallites were then employed to limit the available decay avenues. The one and two-pair transitions were characterized, and using spectral hole-burning, energy relaxation was shown to be substantially slower than in bulk. Dipole dephasing remained very rapid. Persistent macroscopic polarization was demonstrated in semiconductors through pump and probe experiments conducted on time scales faster than the inverse linewidth of the exciton. In the first set of experiments, it was found that the exciton optical Stark shift deviates from that predicted by a steady-state theory. The shift is smaller than expected and lasts longer than the pump pulse. Both effects are explained by free evolution of the exciton's polarization. Transient exciton bleaching is observed and shown to be a result of adiabatic following. In a second study of coherent polarization, spectral oscillations at negative delay times were studied. Oscillations were measured in a wide variety of semiconductors, temporally preceding several different pump-probe phenomena. By comparison with a semiclassical theory, it was shown that spectral oscillations in the spectral region of the exciton are evidence of persistent exciton polarization. Oscillations in the band are due to four wave mixing of the pump and probe beams.
We observe ultrafast and large nonlinear optical responses of a semiconductor thin film where excitons are weakly confined and their center-of-mass motion is quantized. The observed degenerate four-wave mixing (DFWM) signal of a GaAs double-hetero-structure layer exhibits an anomalous thickness-dependence, and is much enhanced at the thickness of 110nm. The decay time of the response is the order of ps, which depends on the thickness of the layer and on the number of the layer. These phenomena are elucidated by the theory of the nonlocal interaction between excitonic states and the light beyond the long wavelength approximation regime. The enhancement at the thickness is due to the size-resonant enhancement of the internal field with a nano-scale spatial structure, where the second quantized level of the exciton center-of-mass motion mainly contributes to the large response at the thickness. We, furthermore, demonstrate ultrafast response in a reflective type nonlinear polarization rotation switch with the 110nm thick three double-hetero. The signal intensity of 20% for the reflective pulse was obtained at a pump intensity of 10nJ/cm2, and the decay time is 1.5ps at low temperatures. These results provide a novel design of a semiconductor structure in order to obtain both large and ultrafast nonlinear response that is suitable for device application.
We have identified several physical processes by which below-gap photons can modify excitonic absorption in GaAs quantum wells.1-3 These different phenomena can be distinguished by their temporal response times, which range from tens of nanoseconds to less than one picosecond. Our experiments also show that the relative contributions of these mechanisms to below-gap optical modulation of exciton absorption depend strongly on temperature as well as on the wavelength of the below-gap modulating beam. The size of the modulation indicates that a new class of absorptive and dispersive devices for optical signal processing is possible in which signals propagate in the transparent region of the crystal and experience negligible attenuation. In order to successfully interpret and calculate the magnitude of these exciting new effects, we show that it is necessary to take into account the special properties of two-dimensional excitons in semiconductor quantum wells.
We report on coherent control of the fundamental exciton state in a single quantum dot by means of two phase-locked picosecond laser pulses. By analyzing the experiments performed in the Rabi regime and comparing them to numerical simulations, we show that we can address the exciton coherence and get an insight into the involved dephasing processes. The total decoherence time T2{T}_{2}T2​ (170 ps) is comparable to the effective exciton lifetime T1{T}_{1}T1​ (200 ps), although not reaching the upper theoretical limit of 2T12{T}_{1}2T1​. We conclude that energy relaxation and pure dephasing processes due to virtual scattering with phonons both contribute on an equal footing to the loss of coherence in this kind of monolayer-step-induced GaAs quantum dots.