Tensor network simulation of non-Markovian dynamics in organic polaritons

TL;DR

This paper uses tensor network methods to simulate the complex non-Markovian dynamics of organic polaritons in optical cavities, revealing how vibrational and collective molecular effects influence photon emission across different coupling regimes.

Contribution

It introduces an exact tensor network approach to model non-Markovian vibronic dynamics in organic polaritons, capturing effects of collective motion and dark states.

Findings

Signatures of non-Markovian vibronic dynamics in emission spectra

Impact of collective molecular motion on polariton behavior

Differences between single and many-molecule systems

Abstract

We calculate the exact many-body time dynamics of polaritonic states supported by an optical cavity filled with organic molecules. Optical, vibrational and radiative processes are treated on an equal footing employing the Time-Dependent Variational Matrix Product States algorithm. We demonstrate signatures of non-Markovian vibronic dynamics and its fingerprints in the far-field photon emission spectrum at arbitrary light-matter interaction scales, ranging from the weak to the strong coupling regimes. We analyse both the single and many-molecule cases, showing the crucial role played by the collective motion of molecular nuclei and dark states in determining the polariton dynamics and the subsequent photon emission.