Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach

• URL: http://arxiv.org/abs/2210.13366v1
• Date: Mon, 24 Oct 2022 16:10:25 GMT
• Title: Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach
• Authors: Zhedong Zhang, Xiaoyu Nie, Dangyuan Lei and Shaul Mukame
• Abstract summary: We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. A quantum Langevin analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. A quantum Langevin 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 cross talk 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.

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