Effects of disorder on polaritonic and dark states in a cavity using the disordered Tavis-Cummings model

TL;DR

This paper analyzes how disorder affects polaritonic and dark states in a cavity using a disordered Tavis-Cummings model, revealing their stability, spectral shifts, and the influence of lifetimes and disorder types.

Contribution

It provides analytical solutions for disordered molecular ensembles in cavities, detailing the stability of polaritonic states and effects of various disorder sources on spectral properties.

Findings

Polaritonic states are stable against disorder.

Disorder increases the gap between polaritonic states on resonance.

Dark states become 'grey' with increasing disorder.

Abstract

We consider molecules confined to a microcavity whose dimensions are such that an excitation of the molecule is nearly resonant with a cavity mode. We investigate the situation where the excitation energies of the molecules are randomly distributed with a mean value of $\epsilon_a$ and variance $\sigma$. For this case, we find a solution that approaches the exact result for large values of the number density $\mathscr{N}$ of the molecules. We find the conditions for the existence of the polaritonic states, as well as expressions for their energies. The polaritonic states are quite stable against disorder. Analytical results are verified by comparison with simulations. When $\epsilon_a$ is equal to that of the cavity state $\epsilon_c$ (on resonance) the gap between the two polaritonic states is found to increase with disorder, the increase being equal to $2 \frac{\sigma^2}{\sqrt{\mathscr{N}}|\tilde{V}|}$ where $\tilde{V}$ is the coupling of a molecular excitation to the cavity state. An analytic expression is found for the disorder induced width of the polaritonic peak. We results for various densities of states, and the absorption spectrum. The dark states that exist in the case $\sigma=0$ turn "grey" in presence of disorder with their contribution to the absorption increasing with $\sigma$. We analyze the effect of including lifetimes of the cavity and molecular states and find that in the strong coupling regime, the width of the polaritonic peaks is dominated by the lifetime effect and that disorder plays almost no role, if the Rabi splitting is sufficiently large. We also consider the case where there is (a) orientational disorder as well as (b) spatial variation of the cavity field and find that they effectively amount to a renormlisation of the coupling.