Electron Dynamics of Open Molecular Systems in Photonic Cavities

Coupling molecular excitations to the quantized modes of a photonic cavity results in hybrid light-matter quasiparticles known as polaritons. The burgeoning field of polaritonic chemistry promises non-destructive routes to molecular quantum control and improved quantum devices via the modification of excited state electronic structure and ultrafast dynamics. Critical to the realization of these technologies is an understanding of excited state lifetimes and photonic loss due to coupling of the cavity-molecule system to its surroundings. Here we describe a theoretical method for modeling open cavity-coupled molecular systems and detail its application to small molecules in the strong coupling regime, revealing the impact of energetic loss on the dynamics of molecules in photonic cavities.