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

Optica

Single-scan acquisition of multiple multidimensional spectra

Travis M. Autry, Galan Moody, James M. Fräser, Corey McDonald, Richard P. Mirin, Kevin L. Silverman

Published May 29, 2019• 34 citations
Publisher

Abstract

Multidimensional coherent spectroscopy is a powerful tool for understanding the ultrafast dynamics of complex quantum systems. To fully characterize the nonlinear optical response of a system, multiple pulse sequences must be recorded and quantitatively compared. We present a new single-scan method that enables rapid and parallel acquisition of all unique pulse sequences corresponding to first- and third-order degenerate wave-mixing processes. Signals are recorded with shot-noise limited detection, enabling acquisition times of ~2 minutes with ~100 zs phase stability and ~8 orders of dynamic range, in a collinear geometry, on a single-pixel detector. We demonstrate this method using quantum well excitons, and quantitative analysis reveals new insights into the bosonic nature of excitons. This scheme may enable rapid and scalable analysis of unique chemical signatures, metrology of optical susceptibilities, nonperturbative coherent control, and the implementation of quantum information protocols using multidimensional spectroscopy.

DOI
10.1364/optica.6.000735

Related papers

Optical three-dimensional coherent spectroscopy

Hebin Li, Alan D. Bristow, Mark E. Siemens +2 more

Optical multidimensional coherent spectroscopy is a powerful tool for studying structure and dynamics in complex systems, such as semiconductors. In optical two-dimensional coherent spectroscopy (2DCS), where the spectrum is presented in a two-dimensional (2D) plane with two frequency axes, an important advantage is the ability to isolate quantum pathways by unfolding a one-dimensional spectrum onto a 2D plane. For many systems, however, the quantum pathways are only partially separated in a 2D spectrum. In order to completely isolate the quantum pathways, we extend 2DCS into a third dimension to generate three-dimensional (3D) spectra in which the spectrum is further unfolded. A 3D spectrum provides complete and well-isolated information of the third-order optical response of the system. The information can be used to fully characterize the quantum pathways and to determine the system’s Hamiltonian. Quantitative knowledge of the Hamiltonian enables prediction and control of quantum processes. For instance, such information is essential for deterministic control and improved performance of coherent control schemes.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Mar 7, 2014•22 citations

Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

Gaël Nardin

Abstract Multidimensional coherent optical spectroscopy (MDCS) is an elegant and versatile tool to measure the ultrafast nonlinear optical response of materials. Of particular interest for semiconductor nanostructures, MDCS enables the separation of homogeneous and inhomogeneous linewidths, reveals the nature of coupling between resonances, and is able to identify the signatures of many-body interactions. As an extension of transient four-wave mixing (FWM) experiments, MDCS can be implemented in various geometries, in which different strategies can be used to isolate the FWM signal and measure its phase. I review and compare different practical implementations of MDCS experiments adapted to the study of semiconductor materials. The power of MDCS is illustrated by discussing experimental results obtained on semiconductor nanostructures such as quantum dots, quantum wells, microcavities, and layered semiconductors.

Semiconductor Science and Technology•Nov 16, 2015•14 citations

Optical analogue of 2D heteronuclear double-quantum NMR

Jonathan Owen Tollerud, Jeffrey A. Davis

Heteronuclear multi-quantum spectroscopy is a powerful part of the NMR toolbox, commonly used to identify specific sequences of atoms in complex pulse sequences designed to determine the structure of complex molecules, including proteins. Optical coherent multidimensional spectroscopy (CMDS) is analogous to multidimensional NMR and many of the techniques of NMR have been adapted for application in the optical regime. This has been highly successful, with CMDS being used to understand energy transfer in photosynthesis and many body effects in semiconductor nanostructures amongst many other scientific breakthroughs. Experimental challenges have, however, prevented the translation of heteronuclear multi-quantum NMR to the optical regime, where capabilities to isolate signals in otherwise congested spectra, reduce acquisition times and enable more incisive probes of multi-particle correlations and complex electronic systems would have great benefit. Here we utilise a diffraction based pulseshaper to impose the two key avenues of selectivity required for the analogue of heteronuclear multi-quantum spectrocopy, - control of the individual pulse spectra, and control of the order and timing of interactions - while maintaining phase-locked excitation pulses. We utilise this approach to isolate the 2-quantum signal from a mixed two exciton state in a semiconductor coupled quantum well. The removal of other overlapping peaks allows analysis of the relevant peak shape and thus details of interactions with the environment and other carriers. An alternative pulse ordering also identifies a 2-quantum state associated only with a GaAs defect, the signature of which would otherwise be confused with other interaction induced effects. The experimental approach described here provides access to crucial details of excitonic interactions, which are important in a range of material systems

•Jul 15, 2016•1 citation

Single-Shot Fourier-Slice Dual-Comb Spectroscopy

Bachana Lomsadze, Skyler C. Weight, Peyton Clark

Multidimensional coherent spectroscopy is a powerful method for studying materials’ optical properties. It also has potential to be used for chemical sensing applications as it allows the measurements of samples’ energy level structures as well as couplings between the excited states resonances. This coupling information is the key to identify whether or not the sample contains a mixture of analytes. Coupling information is not easily accessible using one-dimensional linear or non-linear methods, necessitating more complex multidimensional experimental techniques. However, multidimensional techniques require bulky apparatus, complex stabilization schemes, and/or long acquisition times that prevent them from being used outside the lab. Here we propose and demonstrate a new and simple approach that enables the measurements of the main absorption lines as well as the couplings between the excited states resonances extremely fast (tens to hundreds of$\mu \text{s}$) without measuring the full multidimensional spectra. This approach is based on the Fourier-slice theorem and was inspired by frequency comb technology, particularly dual-comb spectroscopy. Our approach uses free-running lasers and co-linear geometry, and with the development of compact lasers this approach can become field-deployable for sensing applications. We demonstrate the concept on rubidium vapor.

IEEE Photonics Technology Letters•Oct 18, 2023•3 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

Automated multidimensional coherent optical spectroscopy with multiple phase-related femtosecond pulses

Marc M. Wefers, Hitoshi Kawashima, Keith Adam Nelson

Multidimensional spectroscopy with femtosecond phase-related pulse sequences, in which the relative delays and optical phases of pulses are scanned during spectroscopic observation, is demonstrated on electronic transitions in atomic potassium vapor. The pulse sequences were constructed using emerging femtosecond pulse-shaping techniques that allow for automated generation of complex ultrafast waveforms. Sequences of two and three pulses with specified optical phase relationships and interpulse delays were used to prepare specified coherent states.

The Journal of Chemical Physics•Jun 8, 1995•33 citations
Multidimensional coherent spectroscopy is a powerful tool for understanding the ultrafast dynamics of complex quantum systems. To fully characterize the nonlinear optical response of a system, multiple pulse sequences must be recorded and quantitatively compared. We present a new single-scan method that enables rapid and parallel acquisition of all unique pulse sequences corresponding to first- and third-order degenerate wave-mixing processes. Signals are recorded with shot-noise limited detection, enabling acquisition times of ~2 minutes with ~100 zs phase stability and ~8 orders of dynamic range, in a collinear geometry, on a single-pixel detector. We demonstrate this method using quantum well excitons, and quantitative analysis reveals new insights into the bosonic nature of excitons. This scheme may enable rapid and scalable analysis of unique chemical signatures, metrology of optical susceptibilities, nonperturbative coherent control, and the implementation of quantum information protocols using multidimensional spectroscopy.
Optical multidimensional coherent spectroscopy is a powerful tool for studying structure and dynamics in complex systems, such as semiconductors. In optical two-dimensional coherent spectroscopy (2DCS), where the spectrum is presented in a two-dimensional (2D) plane with two frequency axes, an important advantage is the ability to isolate quantum pathways by unfolding a one-dimensional spectrum onto a 2D plane. For many systems, however, the quantum pathways are only partially separated in a 2D spectrum. In order to completely isolate the quantum pathways, we extend 2DCS into a third dimension to generate three-dimensional (3D) spectra in which the spectrum is further unfolded. A 3D spectrum provides complete and well-isolated information of the third-order optical response of the system. The information can be used to fully characterize the quantum pathways and to determine the system’s Hamiltonian. Quantitative knowledge of the Hamiltonian enables prediction and control of quantum processes. For instance, such information is essential for deterministic control and improved performance of coherent control schemes.
Abstract Multidimensional coherent optical spectroscopy (MDCS) is an elegant and versatile tool to measure the ultrafast nonlinear optical response of materials. Of particular interest for semiconductor nanostructures, MDCS enables the separation of homogeneous and inhomogeneous linewidths, reveals the nature of coupling between resonances, and is able to identify the signatures of many-body interactions. As an extension of transient four-wave mixing (FWM) experiments, MDCS can be implemented in various geometries, in which different strategies can be used to isolate the FWM signal and measure its phase. I review and compare different practical implementations of MDCS experiments adapted to the study of semiconductor materials. The power of MDCS is illustrated by discussing experimental results obtained on semiconductor nanostructures such as quantum dots, quantum wells, microcavities, and layered semiconductors.
Heteronuclear multi-quantum spectroscopy is a powerful part of the NMR toolbox, commonly used to identify specific sequences of atoms in complex pulse sequences designed to determine the structure of complex molecules, including proteins. Optical coherent multidimensional spectroscopy (CMDS) is analogous to multidimensional NMR and many of the techniques of NMR have been adapted for application in the optical regime. This has been highly successful, with CMDS being used to understand energy transfer in photosynthesis and many body effects in semiconductor nanostructures amongst many other scientific breakthroughs. Experimental challenges have, however, prevented the translation of heteronuclear multi-quantum NMR to the optical regime, where capabilities to isolate signals in otherwise congested spectra, reduce acquisition times and enable more incisive probes of multi-particle correlations and complex electronic systems would have great benefit. Here we utilise a diffraction based pulseshaper to impose the two key avenues of selectivity required for the analogue of heteronuclear multi-quantum spectrocopy, - control of the individual pulse spectra, and control of the order and timing of interactions - while maintaining phase-locked excitation pulses. We utilise this approach to isolate the 2-quantum signal from a mixed two exciton state in a semiconductor coupled quantum well. The removal of other overlapping peaks allows analysis of the relevant peak shape and thus details of interactions with the environment and other carriers. An alternative pulse ordering also identifies a 2-quantum state associated only with a GaAs defect, the signature of which would otherwise be confused with other interaction induced effects. The experimental approach described here provides access to crucial details of excitonic interactions, which are important in a range of material systems
Multidimensional coherent spectroscopy is a powerful method for studying materials’ optical properties. It also has potential to be used for chemical sensing applications as it allows the measurements of samples’ energy level structures as well as couplings between the excited states resonances. This coupling information is the key to identify whether or not the sample contains a mixture of analytes. Coupling information is not easily accessible using one-dimensional linear or non-linear methods, necessitating more complex multidimensional experimental techniques. However, multidimensional techniques require bulky apparatus, complex stabilization schemes, and/or long acquisition times that prevent them from being used outside the lab. Here we propose and demonstrate a new and simple approach that enables the measurements of the main absorption lines as well as the couplings between the excited states resonances extremely fast (tens to hundreds ofμs\mu \text{s}μs) without measuring the full multidimensional spectra. This approach is based on the Fourier-slice theorem and was inspired by frequency comb technology, particularly dual-comb spectroscopy. Our approach uses free-running lasers and co-linear geometry, and with the development of compact lasers this approach can become field-deployable for sensing applications. We demonstrate the concept on rubidium vapor.
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.
Multidimensional spectroscopy with femtosecond phase-related pulse sequences, in which the relative delays and optical phases of pulses are scanned during spectroscopic observation, is demonstrated on electronic transitions in atomic potassium vapor. The pulse sequences were constructed using emerging femtosecond pulse-shaping techniques that allow for automated generation of complex ultrafast waveforms. Sequences of two and three pulses with specified optical phase relationships and interpulse delays were used to prepare specified coherent states.