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Interpretation of multidimensional coherent spectra

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

Published Feb 28, 2023• 0 citations
Publisher

Abstract

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.

DOI
10.1093/oso/9780192843869.003.0003

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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.
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.
Double-quantum two-dimensional (2D) coherent spectroscopy (MDCS) is a powerful optical method that is used to study the optical properties of atomic and complex molecular systems and semiconductor materials. Double-quantum 2D spectra and particularly the peak line shapes on the spectra can also provide information about many-body interactions. We model 2D spectra by solving the optical Bloch equations and show the effects of correlation between coupled resonances, which also explains the discrepancies between the experimental results reported by multiple groups.
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.
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.