Strong light-matter interaction effects on molecular ensembles

TL;DR

This study models the effects of strong light-matter coupling in a photonic wire on molecular ensembles, revealing how cavity tuning influences spectral and transport properties, which is crucial for controlling chemical processes.

Contribution

We develop a detailed simulation approach for hybrid light-matter excitations in a photonic wire coupled with molecular ensembles, highlighting effects missed by single-mode theories.

Findings

Stronger changes occur when the cavity is redshifted and disorder is weak.

Higher-dimensional cavities likely exhibit similar trends.

Single cavity-mode theories do not capture these effects.

Abstract

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.