Multidimensional Coherent Spectroscopy of Molecular Polaritons : Langevin Approach

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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Original languageEnglish
Article number103001
Journal / PublicationPhysical Review Letters
Volume130
Issue number10
Online published10 Mar 2023
Publication statusPublished - 10 Mar 2023

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Abstract

We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. Using the Heisenberg-Langevin equation, an analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations. We identify clear signatures of the polariton-polaron interaction from multidimensional projections of the signal, e.g., pathways and timescales. Cooperative dynamics of cavity polaritons against intramolecular vibrations is revealed, along with a crosstalk between long-range coherence and vibronic coupling that may lead to localization effects. Our results further characterize the polaritonic coherence and the population transfer that is slower. © 2023 American Physical Society.

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Citation Format(s)

Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach. / Zhang, Zhedong; Nie, Xiaoyu; Lei, Dangyuan et al.
In: Physical Review Letters, Vol. 130, No. 10, 103001, 10.03.2023.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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