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Stochastic methodology shows molecular interactions protect two-dimensional polaritons

Nadine C. Bradbury1, Raphael F. Ribeiro2, Justin R. Caram1,*, and Daniel Neuhauser1,†

  • *Contact author: jcaram@chem.ucla.edu
  • †Contact author: dxn@ucla.edu

Phys. Rev. B 109, L241303 – Published 12 June, 2024

DOI: https://doi.org/10.1103/PhysRevB.109.L241303

Abstract

We introduce stochastic techniques that enable the simulations of polaritons resulting from placing giant two-dimensional molecular aggregate crystals with 108 interacting excitonic dyes in realistic multimode 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.

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