Strong coupling electron-photon dynamics: a real-time investigation of energy redistribution in molecular polaritons

TL;DR

This paper presents a real-time quantum electrodynamics coupled cluster model to visualize and analyze electron-photon dynamics and energy redistribution in molecular polaritons, revealing different time scales and mechanisms involved.

Contribution

It introduces a novel RT-QED-CC method capable of simulating electron-photon interactions with high accuracy, including multiple laser pulses and correlation effects.

Findings

Electrons and photons exhibit different time scales under strong coupling.

Dark states significantly influence energy transfer processes.

The method enables detailed simulation of nonlinear optical phenomena.

Abstract

We analyze the real-time electron-photon dynamics in long-range polariton-mediated energy transfer using a real-time quantum electrodynamics coupled cluster (RT-QED-CC) model, which allows for spatial and temporal visualization of transport processes. We compute the time evolution of photonic and molecular observables, such as the dipole moment and the photon coordinate, following the excitation of the system induced by short laser pulses. Our simulation highlights the different time scales of electrons and photons under light-matter strong coupling, the role of dark states, and the differences with the electronic (F\"orster and Dexter) energy exchange mechanisms. The developed method can simulate multiple high-intensity laser pulses while explicitly retaining electronic and electron-photon correlation and is thus suited for nonlinear optics and transient absorption spectroscopies of molecular polaritons.