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Introduction to multidimensional coherent spectroscopy

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

Published Feb 28, 2023• 0 citations
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Abstract

Abstract An introduction to multidimensional coherent spectroscopy (MDCS) is provided in this chapter. We start out by introducing MDCS in qualitative terms, as an extension of transient absorption spectroscopy. We proceed to discuss the meaning and utility of coherent spectroscopy more generally. We go on to discuss the specifics of MDCS as a specific form of coherent spectroscopy. Pulse sequences involved in generating MDCS plots are introduced. Finally, we discuss density matrix perturbation theory and double-sided Feynman diagrams, and the role of this formalism in simulating and interpreting MDCS.

DOI
10.1093/oso/9780192843869.003.0002

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Laser & Photonics Review•Dec 1, 2018•7 citations
Abstract An introduction to multidimensional coherent spectroscopy (MDCS) is provided in this chapter. We start out by introducing MDCS in qualitative terms, as an extension of transient absorption spectroscopy. We proceed to discuss the meaning and utility of coherent spectroscopy more generally. We go on to discuss the specifics of MDCS as a specific form of coherent spectroscopy. Pulse sequences involved in generating MDCS plots are introduced. Finally, we discuss density matrix perturbation theory and double-sided Feynman diagrams, and the role of this formalism in simulating and interpreting MDCS.
Abstract Interpretation of multi-dimensional coherent spectra is presented in this chapter. Results are presented with the Bloch model. We begin by discussing the characteristic features of an MDCS rephasing plot corresponding to a two-level system. We then discuss the characteristics of inhomogeneous ensembles of two-level systems. We go on to discuss the origins of cross-peaks in MDCS, and then some of the signatures in MDCS that arise as a result of many-body effects. Double-quantum spectra, zero-quantum spectra, three-dimensional spectra, and nonrephasing single-quantum spectra are discussed. Finally, we discuss the impact that finite pulse effects can have on a multidimensional spectrum.
Multidimensional coherent spectroscopy (MDCS) has been established in quantum chemistry as a powerful tool for studying the nonlinear response and nonequilibrium dynamics of molecular systems. More recently, the technique has also been applied to correlated electron materials, where the interplay of localized and itinerant states makes the interpretation of the spectra more challenging. Here we use the Keldysh contour representation of effective models and nonequilibrium dynamical mean field theory to systematically study the MDCS signals of prototypical correlated lattice systems. By analyzing the current induced by sequences of ultrashort laser pulses we demonstrate the usefulness of MDCS as a diagnostic tool for excitation pathways and coherent processes in correlated solids. We also show that this technique allows to extract detailed information on the nature and evolution of photo-excited nonequilibrium states.
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.
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.
In article number 1800171, Christopher L. Smallwood and Steven T. Cundiff introduce a multidimensional coherent spectroscopy (MDCS) probe of the dynamics of excitons in an asymmetric In0.05Ga0.95As/GaAs double quantum well. Spectral information here is plotted as a correlation between the frequency of a first-order optical excitation interaction (ωτ) and a third-order emission interaction (ωt) at various intermediate-state mixing times (T), providing a window into a semiconductor's inhomogeneity, many-body interactions, and coherent coupling dynamics at femtosecond timescales. Image credit: Brad Baxley, Part to Whole.