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

Excitonic Coherent Emission Process in Semiconductors

Takashi Kuroda

Published Dec 26, 1994• 0 citations
Publisher

Abstract

Coherent emission process of excitons in a layered compound GaSe, and in ZnSe/ZnSo.isSeo.s2 multiple quantum wells has been directly observed for the first time, by means of two independent newly-developed methods; time-resolved Brewster-angle reflectance (TRBR) spectroscopy and time-resolved four-wave-mixing (TRFWM) spectroscopy. In TRBR measurement, we have succeeded in observing a distinct free-induction-decay of coherently-driven polarization, with an oscillatory behavior due to finely split exciton levels. An analysis on the basis of a s imple model provides key information on the dynamical phase relaxation process. The result of the TRFWM measurement gives the comprehensive treatment of two dephasing processes; destructive interference due to static inhomogeneous broadening, and dynamical homogeneous phase relaxation. An analysis of TRFWM intensity enables one to exactly determine the homogeneous phase relaxation time. Finally, we show that a comparison between the coherent emission signal measured by TRBR or TRFWM, and third-order nonlinear correlation profile observed by time integrated FWM measurement enables one to make distinction between which of quantum - or classical interference effect causes the beat feature seen in the coherent emission signal.

DOI
10.11501/3098906

Related papers

Ultrafast coherent dynamics of excitons of higher-order subbands in semiconductor quantum wells

S. Arlt, U. Siegner, François Morier-Genoud +1 more

The coherent emission from excitons corresponding to different subband transitions in a 500 Åbroad GaAs/AlGaAs quantum well is studied by spectrally resolved transient four-wave mixing (FWM). For the simultaneous excitation of several subband transitions, the dephasing times of the lowest exciton and higher- order exciton transitions are determined from the width of the resonances in the FWM spectrum. The decay of the spectrally integrated FWM signal as a function of the time delay between the excitation laser pulses does not reflect the dephasing times but is determined by the laser pulse width for multi-subband excitation. This is indicative of quantum interference between exciton and continuum transitions. Many-body Coulomb effects have to be included in a theoretical treatment of these experimental observations.

Radiative Processes and Dephasing in Semiconductors•Jan 1, 1998•0 citations

DEPHASING OF EXCITONS AND PHASE COHERENT PHOTOREFRACTIVITY IN ZnSe QUANTUM WELLS

Suvranta K. Tripathy

Spectrally resolved and time-integrated degenerate four-wave mixing (FWM) experiments with ultra-short pulses have been used to investigate the relaxation times and coherent interactions of excitons in the Boltzmann and in the quantum kinetic regime in ZnSe single quantum wells.Three-pulse FWM experiments using 100 fs pulses in a 10 nm thick ZnSe/ZnMgSe single quantum well reveal nearly equal zero-density dephasing rates for coherences between + σ and - σ heavy-and/or light-hole exciton states as compared to the dephasing rate of the interband coherence between these states and the ground state.The measurements also demonstrate that exciton-exciton scattering destroys the phase coherence between heavy-and light-hole excitons about three times more effectively than the coherence between + σ and + σ heavy-hole excitons.The different coherent nonlinear signals obtained in a three-beam FWM experiment are explained and reproduced by numerical calculations of the optical Bloch equations for a ten-level model including excitation induced dephasing (EID).Two-beam FWM experiments using 30 fs pulses on a 10 nm ZnSe quantum well reveal marked quantum beats and a pronounced non-exponential decay for delay times smaller ~500 fs.The pronounced peak at pulse overlap is attributed to rapid destructive interference of the created polarization and to spin dependent quantum kinetic effects caused by the transient formation of an electron-hole (eh) pair grating.The three-beam FWM trace shows a bi-exponential decay which is attributed to a nonlinear polarization that is caused by the interaction of polarization 3 k with both an exciton grating and an eh-pair grating.Model calculations using the OBEs of a two level system that includes ∑ -+

•Jan 1, 2006•0 citations

Measuring Excitonic Coherence in Nanostructures: Time-Resolved Speckle Analysis versus Four-Wave Mixing

W. Langbein, J. M. Hvam

The excitonic coherence in semiconductor quantum wells is measured by time-resolved speckle analysis and four-wave mixing. It is found that in the case of single GaAs quantum wells, the results of both methods are in agreement, and can be understood in the framework of an inhomogeneously broadened distribution of localized excitons which are subject to phonon-scattering and radiative recombination. The speckle analysis gives the additional distinction between recombination and pure dephasing processes. In multiple quantum wells, the radiative coupling between the quantum wells leads to a pronounced change of the observed dynamics. In the secondary emission, a strong coherent component with an oscillating time-structure is observed for small scattering angles. This is attributed to the beating of the radiative eigenstates of the stacked structure.

physica status solidi (a)•Mar 1, 2000•7 citations

Exciton free induction in II-VI thin films observed by transient Brewster-angle reflectance spectroscopy

Takashi Kuroda, Kuon Inoue, Ikuo Suemune +2 more

The coherent emission process at excitonic resonance was first investigated in short-period ZnSe/ZnSxSe1-x (x equals 0.18) superlattices with one period of 50 A/50 A and 19 A/19 A by observing a temporal profile with subpicosecond time resolution, of reflected pulses in the Brewster-angle configuration. As a result, an almost background-free signal with nonresonant contribution reduced greatly, was observed reflecting free induction decay (FID) of coherently driven exciton polarization. In particular, a beat signal of FID was clearly observed for the first time, which arises from interference effect between a few split spectral lines of the relevant exciton. Further, it was confirmed that the decay spread of FID becomes faster as the power density of incident pulse was increased for the SL sample with a thicker well. The results may be explained qualitatively by a simple model with the knowledge of the exciton structure as well as a preliminary data of the phase relaxation time obtained by four- wave-mixing measurement. The present results have provided a basis for that the transient Brewster-angle reflection spectroscopy serves as a powerful tool for exploring coherent interaction of exciton with light.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Feb 9, 1995•1 citation

Excitation-Induced Phase Shifts of Heavy and Light Hole Quantum Beats in Multiple Quantum Wells

Wei E. I. Sha, A. E. Paul, Shekhar Patkar +1 more

In recent years, transient four-wave mixing (FWM) techniques have been used to investigate the dephasing times of non-equilibrium carriers in semiconductor heterostructures by monitoring the decay of the macroscopic polarization. Initially, this decay was measured by temporally-integrating the scattered FWM signal as a function of time delay between two (or more) pump pulses. More recently, the macroscopic polarization decay has been measured by time-resolving the FWM signal by cross correlating it with an ultrashort laser pulse via frequency up-conversion in a nonlinear crystal. When excitons with slightly different energies are excited, oscillations (or beats) have been observed both in the time-integrated FWM signal and in the time-resolved FWM signal. Such beats have been observed, for example, between light- and heavy-hole excitons and between excitons in wells of different widths. Both the spectral behavior1 of the time-integrated FWM signal and the temporal behavior2 of the time-resolved signal have been shown to allow the distinction between the polarization interference associated with two independent oscillators and the quantum beats associated with two coupled oscillators which share a common level. In addition, it has been demonstrated3 that the quantum beats produced by incident pulses with parallel polarizations are exactly out of phase (by π) with the beats produced by orthogonally polarized pulses. In each case1-3, the period and phase of the beats and the polarization of FWM signal were explained by using a six-level model, which excluded many-body effects, to describe the J=1/2 conduction and J=3/2 valence states. Within the last few months, however, it has been shown that a complete description of the polarization selection rules for the FWM signal requires excitation-induced dephasing4 or disorder-induced coupling of the σ + and σ – excitonic transitions5.

International Conference on Ultrafast Phenomena•Jan 1, 1994•0 citations

Coherent exciton dynamics : time-resolved polarimetry

Arthur L. Smirl

The studies described in this chapter convince the reader that time-resolved polarimetry is an extremely sensitive way to study many body effects. The vectorial dynamics contain useful information about many-body effects, quantum interference and optical anisotropies that would be difficult to obtain in any other way. The chapter begins with a brief review of some of the four-wave-mixing (FWM) techniques that have been most commonly used to measure the coherent emission from multiple quantum wells (MQWs). The ellipticity and the fraction of unpolarised light are both significantly smaller for the negative delay. These features provide additional tests for any proposed model that purports to describe coherent excitonic dynamics in MQWs. The chapter discusses the treatment of excitons in semiconductors as two-level systems, and follows with a detailed review of the solutions to the density matrix equations for two independent two-level systems, with an emphasis on the vectorial nature of the FWM emission from such systems.

CRC Press eBooks•Dec 5, 2020•0 citations
Coherent emission process of excitons in a layered compound GaSe, and in ZnSe/ZnSo.isSeo.s2 multiple quantum wells has been directly observed for the first time, by means of two independent newly-developed methods; time-resolved Brewster-angle reflectance (TRBR) spectroscopy and time-resolved four-wave-mixing (TRFWM) spectroscopy. In TRBR measurement, we have succeeded in observing a distinct free-induction-decay of coherently-driven polarization, with an oscillatory behavior due to finely split exciton levels. An analysis on the basis of a s imple model provides key information on the dynamical phase relaxation process. The result of the TRFWM measurement gives the comprehensive treatment of two dephasing processes; destructive interference due to static inhomogeneous broadening, and dynamical homogeneous phase relaxation. An analysis of TRFWM intensity enables one to exactly determine the homogeneous phase relaxation time. Finally, we show that a comparison between the coherent emission signal measured by TRBR or TRFWM, and third-order nonlinear correlation profile observed by time integrated FWM measurement enables one to make distinction between which of quantum - or classical interference effect causes the beat feature seen in the coherent emission signal.
The coherent emission from excitons corresponding to different subband transitions in a 500 Åbroad GaAs/AlGaAs quantum well is studied by spectrally resolved transient four-wave mixing (FWM). For the simultaneous excitation of several subband transitions, the dephasing times of the lowest exciton and higher- order exciton transitions are determined from the width of the resonances in the FWM spectrum. The decay of the spectrally integrated FWM signal as a function of the time delay between the excitation laser pulses does not reflect the dephasing times but is determined by the laser pulse width for multi-subband excitation. This is indicative of quantum interference between exciton and continuum transitions. Many-body Coulomb effects have to be included in a theoretical treatment of these experimental observations.
Spectrally resolved and time-integrated degenerate four-wave mixing (FWM) experiments with ultra-short pulses have been used to investigate the relaxation times and coherent interactions of excitons in the Boltzmann and in the quantum kinetic regime in ZnSe single quantum wells.Three-pulse FWM experiments using 100 fs pulses in a 10 nm thick ZnSe/ZnMgSe single quantum well reveal nearly equal zero-density dephasing rates for coherences between + σ and - σ heavy-and/or light-hole exciton states as compared to the dephasing rate of the interband coherence between these states and the ground state.The measurements also demonstrate that exciton-exciton scattering destroys the phase coherence between heavy-and light-hole excitons about three times more effectively than the coherence between + σ and + σ heavy-hole excitons.The different coherent nonlinear signals obtained in a three-beam FWM experiment are explained and reproduced by numerical calculations of the optical Bloch equations for a ten-level model including excitation induced dephasing (EID).Two-beam FWM experiments using 30 fs pulses on a 10 nm ZnSe quantum well reveal marked quantum beats and a pronounced non-exponential decay for delay times smaller ~500 fs.The pronounced peak at pulse overlap is attributed to rapid destructive interference of the created polarization and to spin dependent quantum kinetic effects caused by the transient formation of an electron-hole (eh) pair grating.The three-beam FWM trace shows a bi-exponential decay which is attributed to a nonlinear polarization that is caused by the interaction of polarization 3 k with both an exciton grating and an eh-pair grating.Model calculations using the OBEs of a two level system that includes ∑ -+
The excitonic coherence in semiconductor quantum wells is measured by time-resolved speckle analysis and four-wave mixing. It is found that in the case of single GaAs quantum wells, the results of both methods are in agreement, and can be understood in the framework of an inhomogeneously broadened distribution of localized excitons which are subject to phonon-scattering and radiative recombination. The speckle analysis gives the additional distinction between recombination and pure dephasing processes. In multiple quantum wells, the radiative coupling between the quantum wells leads to a pronounced change of the observed dynamics. In the secondary emission, a strong coherent component with an oscillating time-structure is observed for small scattering angles. This is attributed to the beating of the radiative eigenstates of the stacked structure.
The coherent emission process at excitonic resonance was first investigated in short-period ZnSe/ZnSxSe1-x (x equals 0.18) superlattices with one period of 50 A/50 A and 19 A/19 A by observing a temporal profile with subpicosecond time resolution, of reflected pulses in the Brewster-angle configuration. As a result, an almost background-free signal with nonresonant contribution reduced greatly, was observed reflecting free induction decay (FID) of coherently driven exciton polarization. In particular, a beat signal of FID was clearly observed for the first time, which arises from interference effect between a few split spectral lines of the relevant exciton. Further, it was confirmed that the decay spread of FID becomes faster as the power density of incident pulse was increased for the SL sample with a thicker well. The results may be explained qualitatively by a simple model with the knowledge of the exciton structure as well as a preliminary data of the phase relaxation time obtained by four- wave-mixing measurement. The present results have provided a basis for that the transient Brewster-angle reflection spectroscopy serves as a powerful tool for exploring coherent interaction of exciton with light.
In recent years, transient four-wave mixing (FWM) techniques have been used to investigate the dephasing times of non-equilibrium carriers in semiconductor heterostructures by monitoring the decay of the macroscopic polarization. Initially, this decay was measured by temporally-integrating the scattered FWM signal as a function of time delay between two (or more) pump pulses. More recently, the macroscopic polarization decay has been measured by time-resolving the FWM signal by cross correlating it with an ultrashort laser pulse via frequency up-conversion in a nonlinear crystal. When excitons with slightly different energies are excited, oscillations (or beats) have been observed both in the time-integrated FWM signal and in the time-resolved FWM signal. Such beats have been observed, for example, between light- and heavy-hole excitons and between excitons in wells of different widths. Both the spectral behavior1 of the time-integrated FWM signal and the temporal behavior2 of the time-resolved signal have been shown to allow the distinction between the polarization interference associated with two independent oscillators and the quantum beats associated with two coupled oscillators which share a common level. In addition, it has been demonstrated3 that the quantum beats produced by incident pulses with parallel polarizations are exactly out of phase (by π) with the beats produced by orthogonally polarized pulses. In each case1-3, the period and phase of the beats and the polarization of FWM signal were explained by using a six-level model, which excluded many-body effects, to describe the J=1/2 conduction and J=3/2 valence states. Within the last few months, however, it has been shown that a complete description of the polarization selection rules for the FWM signal requires excitation-induced dephasing4 or disorder-induced coupling of the σ + and σ – excitonic transitions5.
The studies described in this chapter convince the reader that time-resolved polarimetry is an extremely sensitive way to study many body effects. The vectorial dynamics contain useful information about many-body effects, quantum interference and optical anisotropies that would be difficult to obtain in any other way. The chapter begins with a brief review of some of the four-wave-mixing (FWM) techniques that have been most commonly used to measure the coherent emission from multiple quantum wells (MQWs). The ellipticity and the fraction of unpolarised light are both significantly smaller for the negative delay. These features provide additional tests for any proposed model that purports to describe coherent excitonic dynamics in MQWs. The chapter discusses the treatment of excitons in semiconductors as two-level systems, and follows with a detailed review of the solutions to the density matrix equations for two independent two-level systems, with an emphasis on the vectorial nature of the FWM emission from such systems.