Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach

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.

6 pages, 2 figures

References in corpus (2)

• Coherent coupling of molecular resonators with a micro-cavity mode
• Quantum theory of collective strong coupling of molecular vibrations with a microcavity mode

Cited by in corpus (6)

• Polariton Localization and Dispersion Properties of Disordered Quantum Emitters in Multimode Microcavities
• Nonlinear semiclassical spectroscopy of ultrafast molecular polariton dynamics
• Coherent Nonlinear Optical Response for High-Intensity Excitation
• Photon-resolved Floquet theory approach to spectroscopic quantum sensing
• Nonlinear opto-vibronics in molecular systems
• Linear and nonlinear vibrational excitation driven by molecular polaritons