Quantum dynamics simulation of exciton-polariton transport

Abstract

Abstract Strong coupling between excitons and confined modes of light presents a promising pathway to tunable and enhanced energy transport in organic materials. By forming hybrid light-matter quasiparticles, exciton-polaritons, electronic excitations can traverse long distances at high velocities through ballistic flow. However, transport behavior of exciton-polaritons varies strongly across experiments, spanning both diffusive and ballistic transport regimes. Which properties of the material and light-modes govern the transport behavior of polaritons remains an open question. Through full-quantum dynamical simulations we reveal a strong dependence of polariton transport on vibronic interactions and static disorder within molecules in both ideal and lossy cavities. Specifically, we show that intramolecular vibrations mediate relaxation processes that alter polariton composition, lifetime and velocity on ultrafast timescales. Analysis of the propagating wavepacket in position and momentum space provides mechanistic insight into the robustness of ballistic flow of exciton-polaritons found experimentally under cryogenic conditions.