Different perspectives on the exact factorization for photon-electron-nuclear systems

TL;DR

This paper uses the exact factorization approach to analyze the dynamics of photon-electron-nuclear systems, especially in strong coupling regimes like molecular polaritons, and evaluates the foundations of existing simulation techniques.

Contribution

It applies the exact factorization framework to photon-electron-nuclear systems and critically assesses the performance of nonadiabatic molecular dynamics methods in this context.

Findings

Analyzes the foundations of nonadiabatic molecular dynamics in photon-electron-nuclear systems.

Assesses the performance of these techniques on model studies.

Provides insights into the dynamics of molecular polaritons.

Abstract

We employ the exact factorization of a multi-component wavefunction to analyze the dynamics of interacting photons, electrons and nuclei. We consider physical situations emerging in the regime of strong coupling between light excitations and molecular - electronic excitations, giving rise to the so-called molecular polaritons. Nonadiabatic molecular dynamics techniques, routinely used in the field of chemical physics, have been often employed to simulate photophysical and photochemical phenomena in the presence of molecular polaritons. In this work, we analyze the foundations of these techniques in the eye of the exact factorization and we assess their performance on illustrative model studies.