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arXiv · 2210.13366

Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach

Zhedong Zhang·Xiaoyu Nie·Dangyuan Lei·Shaul Mukame
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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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Zhedong Zhang, Xiaoyu Nie, Dangyuan Lei, Shaul Mukame. 2022-10-24. Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach. https://doi.org/10.1103/physrevlett.130.103001

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