Quantum dynamics simulation of exciton-polariton transport

TL;DR

This paper uses full-quantum dynamical simulations to explore how vibronic interactions influence exciton-polariton transport, revealing mechanisms that affect their velocity, lifetime, and transport regime in organic materials.

Contribution

It demonstrates the critical role of intramolecular vibrations in governing polariton transport properties and provides mechanistic insights into ballistic flow behavior.

Findings

Vibronic interactions significantly affect polariton relaxation and transport.

Intramolecular vibrations mediate ultrafast changes in polariton composition.

Ballistic transport robustness is linked to vibrational effects under cryogenic conditions.

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 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.