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

Two-dimensional spectroscopy of semiconductor quantum wells

Hebin Li, Bachana Lomsadze, Galan Moody, Christopher L. Smallwood, Steven T. Cundiff

Published Feb 28, 2023• 0 citations
Publisher

Abstract

Abstract Two-dimensional coherent spectroscopy of semiconductor quantum wells is discussed in this chapter. The chapter starts with an introduction of semiconductor optics. The signatures of many-body interaction and correlation are revealed as spectral features in 2D spectra including one-, double-, and multi-quantum 2D spectra. Two-dimensional coherent spectroscopy can also be used to study the coupling in coupled quantum wells and exciton-polaritons in microcavities.

DOI
10.1093/oso/9780192843869.003.0007

Related papers

Two-dimensional coherent spectroscopy of excitons, biexcitons and exciton-polaritons

Alan D. Bristow

Semiconductors systems exhibiting excitonic properties are discussed in terms of their coherent response, which is extracted using two-dimensional coherent spectroscopy. This control method allows for separation of quantum pathways that comprise the optical response, such as interactions between excitons, their dephasing rates, the effects of many-body interactions and the role of structure on the microscopic electronic environment. Additional controls, such as polarization can be used to further distinguish biexcitons and suppress many-body interactions. These result are compared and contrasted with those from a semiconductor microcavity where the excitons form polaritonic modes due to normal-mode splitting. Rephrasing spectra map the detuning dependence of the exciton-polariton branches. Increasing the detuning shifts all features to higher energy and the expected anti-crossing is observed. An isolated biexciton is seen only at negative detuning, separated by a binding energy. For positive detuning, the spectral weight of the off-diagonal features swap, as the lower polariton branch and biexciton come into resonance. This indicates that the off-diagonal features are sensitive to the interactions of the exciton-polaritons and other resonances in the system.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Oct 3, 2016•1 citation

Two-dimensional optical spectroscopy of excitons in semiconductor quantum wells: Liouville-space pathway analysis

Lijun Yang, Igor V. Schweigert, Steven T. Cundiff +1 more

We demonstrate how dynamic correlations of heavy-hole and light-hole excitons in semiconductor quantum wells may be investigated by two-dimensional correlation spectroscopy. The coherent response to three femtosecond optical pulses is predicted to yield cross (off-diagonal) peaks that contain direct signatures of many-body two-exciton correlations. Signals generated at various phase-matching directions are compared.

arXiv:cond-mat/0701424•Physical Review B•Mar 2, 2007•65 citations

Advances in multi-dimensional coherent spectroscopy of semiconductor nanostructures

Galan Moody, Steven T. Cundiff

Multi-dimensional coherent spectroscopy (MDCS) has become an extremely versatile and sensitive technique for elucidating the structure, composition, and dynamics of condensed matter, atomic, and molecular systems. The appeal of MDCS lies in its ability to resolve both individual-emitter and ensemble-averaged dynamics of optically created excitations in disordered systems. When applied to semiconductors, MDCS enables unambiguous separation of homogeneous and inhomogeneous contributions to the optical linewidth, pinpoints the nature of coupling between resonances, and reveals signatures of many-body interactions. In this review, we discuss the implementation of MDCS to measure the nonlinear optical response of excitonic transitions in semiconductor nanostructures. Capabilities of the technique are illustrated with recent experimental studies that advance our understanding of optical decoherence and dissipation, energy transfer, and many-body phenomena in quantum dots and quantum wells, semiconductor microcavities, layered semiconductors, and photovoltaic materials.

Advances in Physics X•May 4, 2017•66 citations

Probing many particle correlations in semiconductor quantum wells using double-quantum-coherence signal

Lijun Yang, Shaul Mukamel

Multidimensional analysis of coherent signals is commonly used in nuclear magnetic resonance to study correlations among spins. These techniques were recently extended to the femtosecond regime and applied to chemical, biological and semiconductor systems. In this work, we apply a two-dimensional correlation spectroscopy technique which employs double-quantum-coherence to investigate many-body effects in a semiconductor quantum well. The signal is detected along the direction k(1)+ k(2)- k(3), where k(1), k(2) and k(3) are the pulse wave vectors in chronological order. We show that this signal is particularly sensitive to many-body correlations which are missed by time-dependent Hartree-Fock approximation. The correlation energy of two-exciton can be probed with a very high resolution arising from a two-dimensional correlation spectrum, where two-exciton couplings spread the cross peaks along both axes of the 2D spectrum to create a characteristic highly resolved pattern. This level of detail is not available from conventional one-dimensional four-wave mixing or other two-dimensional correlation spectroscopy signals such as the photo echo (-k(1)+ k(2)+ k(3)).

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Feb 11, 2010•1 citation

Two-Dimensional Correlation Spectroscopy of Two-Exciton Resonances in Semiconductor Quantum Wells

Lijun Yang, Shaul Mukamel

We propose a three-pulse coherent ultrafast optical technique that is particularly sensitive to two-exciton correlations. Two Liouville-space pathways for the density matrix contribute to this signal which reveals double quantum coherences when displayed as a two-dimensional correlation plot. Two-exciton couplings spread the cross peaks along both axes, creating a characteristic highly resolved pattern. This level of detail is not available from conventional one-dimensional four-wave mixing or other two-dimensional correlation spectroscopy signals such as the photo echo, in which two-exciton couplings show up along a single axis and are highly congested.

arXiv:0712.2263•Physical Review Letters•Feb 4, 2008•88 citations

Optical Multidimensional Coherent Spectroscopy

Hebin Li, Bachana Lomsadze, Galan Moody +2 more

Abstract Optical multidimensional coherent spectroscopy provides information about the structure and excitation dynamics in a broad range of material systems. This book focuses on systems of interest in physics, including atomic vapors, semiconductor nanostructures and two-dimensional materials. An introduction to ultrafast spectroscopy and the fundamental concepts of multidimensional coherent spectroscopy applies to all material systems. Relevant experimental implementations, including phase-stabilized crossed-beams, frequency-tagged fully-collinear, three-dimensional and frequency-comb based methods. The use of the method to study atomic vapors, semiconductor quantum wells, semiconductor quantum dots and two-dimensional materials are described in separate chapters. The final chapters survey the use of the method in some other areas and speculate on future directions.

•Feb 28, 2023•36 citations
Abstract Two-dimensional coherent spectroscopy of semiconductor quantum wells is discussed in this chapter. The chapter starts with an introduction of semiconductor optics. The signatures of many-body interaction and correlation are revealed as spectral features in 2D spectra including one-, double-, and multi-quantum 2D spectra. Two-dimensional coherent spectroscopy can also be used to study the coupling in coupled quantum wells and exciton-polaritons in microcavities.
Semiconductors systems exhibiting excitonic properties are discussed in terms of their coherent response, which is extracted using two-dimensional coherent spectroscopy. This control method allows for separation of quantum pathways that comprise the optical response, such as interactions between excitons, their dephasing rates, the effects of many-body interactions and the role of structure on the microscopic electronic environment. Additional controls, such as polarization can be used to further distinguish biexcitons and suppress many-body interactions. These result are compared and contrasted with those from a semiconductor microcavity where the excitons form polaritonic modes due to normal-mode splitting. Rephrasing spectra map the detuning dependence of the exciton-polariton branches. Increasing the detuning shifts all features to higher energy and the expected anti-crossing is observed. An isolated biexciton is seen only at negative detuning, separated by a binding energy. For positive detuning, the spectral weight of the off-diagonal features swap, as the lower polariton branch and biexciton come into resonance. This indicates that the off-diagonal features are sensitive to the interactions of the exciton-polaritons and other resonances in the system.
Multi-dimensional coherent spectroscopy (MDCS) has become an extremely versatile and sensitive technique for elucidating the structure, composition, and dynamics of condensed matter, atomic, and molecular systems. The appeal of MDCS lies in its ability to resolve both individual-emitter and ensemble-averaged dynamics of optically created excitations in disordered systems. When applied to semiconductors, MDCS enables unambiguous separation of homogeneous and inhomogeneous contributions to the optical linewidth, pinpoints the nature of coupling between resonances, and reveals signatures of many-body interactions. In this review, we discuss the implementation of MDCS to measure the nonlinear optical response of excitonic transitions in semiconductor nanostructures. Capabilities of the technique are illustrated with recent experimental studies that advance our understanding of optical decoherence and dissipation, energy transfer, and many-body phenomena in quantum dots and quantum wells, semiconductor microcavities, layered semiconductors, and photovoltaic materials.
Multidimensional analysis of coherent signals is commonly used in nuclear magnetic resonance to study correlations among spins. These techniques were recently extended to the femtosecond regime and applied to chemical, biological and semiconductor systems. In this work, we apply a two-dimensional correlation spectroscopy technique which employs double-quantum-coherence to investigate many-body effects in a semiconductor quantum well. The signal is detected along the direction k(1)+ k(2)- k(3), where k(1), k(2) and k(3) are the pulse wave vectors in chronological order. We show that this signal is particularly sensitive to many-body correlations which are missed by time-dependent Hartree-Fock approximation. The correlation energy of two-exciton can be probed with a very high resolution arising from a two-dimensional correlation spectrum, where two-exciton couplings spread the cross peaks along both axes of the 2D spectrum to create a characteristic highly resolved pattern. This level of detail is not available from conventional one-dimensional four-wave mixing or other two-dimensional correlation spectroscopy signals such as the photo echo (-k(1)+ k(2)+ k(3)).
We propose a three-pulse coherent ultrafast optical technique that is particularly sensitive to two-exciton correlations. Two Liouville-space pathways for the density matrix contribute to this signal which reveals double quantum coherences when displayed as a two-dimensional correlation plot. Two-exciton couplings spread the cross peaks along both axes, creating a characteristic highly resolved pattern. This level of detail is not available from conventional one-dimensional four-wave mixing or other two-dimensional correlation spectroscopy signals such as the photo echo, in which two-exciton couplings show up along a single axis and are highly congested.
Abstract Optical multidimensional coherent spectroscopy provides information about the structure and excitation dynamics in a broad range of material systems. This book focuses on systems of interest in physics, including atomic vapors, semiconductor nanostructures and two-dimensional materials. An introduction to ultrafast spectroscopy and the fundamental concepts of multidimensional coherent spectroscopy applies to all material systems. Relevant experimental implementations, including phase-stabilized crossed-beams, frequency-tagged fully-collinear, three-dimensional and frequency-comb based methods. The use of the method to study atomic vapors, semiconductor quantum wells, semiconductor quantum dots and two-dimensional materials are described in separate chapters. The final chapters survey the use of the method in some other areas and speculate on future directions.