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Multidimensional coherent spectroscopy of atomic ensembles

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

Published Feb 28, 2023• 0 citations
Publisher

Abstract

Abstract Multidimensional coherent spectroscopy (MDCS) of atomic ensembles is discussed in this chapter. Atomic vapors such as potassium and rubidium atomic vapors are used a model system for demonstrating MDCS. The technique of MDCS can also be used to probe many-body dipole-dipole interaction and correlation in atoms by using double-quantum 2D spectroscopy. Multi-quantum 2D spectroscopy can detect many-body correlations associated with coherent states of multiple atoms in atoms.

DOI
10.1093/oso/9780192843869.003.0005

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Abstract Multidimensional coherent spectroscopy (MDCS) of atomic ensembles is discussed in this chapter. Atomic vapors such as potassium and rubidium atomic vapors are used a model system for demonstrating MDCS. The technique of MDCS can also be used to probe many-body dipole-dipole interaction and correlation in atoms by using double-quantum 2D spectroscopy. Multi-quantum 2D spectroscopy can detect many-body correlations associated with coherent states of multiple atoms in atoms.
Many-body interactions and correlations in atomic ensembles are fundamental in understanding many-body effects such as collective and emergent phenomena and also play an important role in various atom-based applications. Optical two-dimensional coherent spectroscopy (2DCS) provides a powerful tool to measure many-body interactions and correlations. Here, we present the study of many-body dipole-dipole interactions and correlations in potassium and rubidium atomic vapors by using double-quantum and multi-quantum 2DCS. The results show that double-quantum 2DCS provides sensitive and background-free detection of weak dipole-dipole interaction between atoms with a mean separation up to about 16 μm, and multi-quantum 2DCS can excite and detect multi-atom states (Dicke states) with up to eight correlated atoms. The technique of optical 2DCS can provide a new approach to study many-body physics in atomic ensembles and can be potentially implemented to measure many-body effects in cold atoms and other atomic/molecular systems.
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.
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.