Multimode polariton effects on molecular energy transport and spectral fluctuations

Despite the potential paradigm breaking capability of microcavities to control chemical processes, the extent to which photonic devices change properties of molecular materials is still unclear, in part due to challenges in modeling hybrid light-matter excitations delocalized over many length scales. We overcome these challenges for a photonic wire under strong coupling with a molecular ensemble. Our simulations provide a detailed picture of the effect of photonic wires on spectral and transport properties of a disordered molecular material. We find stronger changes to the probed molecular observables when the cavity is redshifted relative to the molecules and energetic disorder is weak. These trends are expected to hold also in higher-dimensional cavities, but are not captured with theories that only include a single cavity-mode. Therefore, our results raise important issues for future experiments and model building focused on unraveling new ways to manipulate chemistry with optical cavities. Optical microcavities affect chemical processes via strong light-matter interactions, but the extent to which chemistry can be controlled with these materials remains unclear. Here, the author employs microscopic simulations of multimode photonic wire under strong coupling with a disordered molecular ensemble to investigate the influence of the cavity resonator on the local molecular density of states and excited-state diffusion.