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Updated: Aug 5, 2025

Experimental Methods for Spin- and Angle-Resolved Photoemission Spectroscopy Combined with Polarization-Variable Laser
Published on: June 28, 2018
Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach
Zhedong Zhang1,2, Xiaoyu Nie3, Dangyuan Lei4
1Department of Physics, City University of Hong Kong, Kowloon, Hong Kong SAR.
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.
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