Stochastic Metholodgy Shows Molecular Interactions Protect 2D Polaritons

TL;DR

This paper introduces stochastic simulation techniques to study 2D molecular aggregate polaritons, revealing how intermolecular coupling preserves polariton states amidst disorder, advancing understanding of light-matter interactions.

Contribution

The paper presents a novel stochastic computational method for simulating large molecular aggregate polaritons, highlighting the protective role of intermolecular coupling against disorder.

Findings

Intermolecular coupling preserves polariton formation despite disorder.

Dark molecular states remain delocalized due to aggregate Hamiltonian.

New stochastic simulation approach enables large-scale polariton studies.

Abstract

We introduce stochastic techniques that enable the simulations of polaritons resulting from placing giant 2D molecular aggregate crystals with $10^8$ interacting excitonic dyes in realistic multi-mode cavities. We show that the intermolecular coupling protects the formation of polariton states in the face of strong molecular disorder due to persistent delocalization of the dark molecular states. This demonstrates the nontrivial role of internal aggregate Hamiltonian in polariton properties, and the new computational method opens horizons for stochastic simulations of related systems.