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

Abstract

We analyze the real-time electron-photon dynamics in long- and short-range energy transfer using a real-time quantum electrodynamics coupled cluster 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 simulations show that intermolecular interactions and light-matter strong coupling lead to modified electronic polarization compared to the undressed molecules. 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.