A1 Journal article (refereed)
Non-Hermitian molecular dynamics simulations of exciton–polaritons in lossy cavities (2024)

Sokolovskii, I., & Groenhof, G. (2024). Non-Hermitian molecular dynamics simulations of exciton–polaritons in lossy cavities. Journal of Chemical Physics, 160(9), Article 092501. https://doi.org/10.1063/5.0188613

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Publication details

All authors or editors: Sokolovskii, Ilia; Groenhof, Gerrit

Journal or series: Journal of Chemical Physics

ISSN: 0021-9606

eISSN: 1089-7690

Publication year: 2024

Publication date: 01/03/2024

Volume: 160

Issue number: 9

Article number: 092501

Publisher: AIP Publishing

Publication country: United States

Publication language: English

DOI: https://doi.org/10.1063/5.0188613

Publication open access: Not open

Publication channel open access: 

Web address of parallel published publication (pre-print): https://arxiv.org/abs/2311.13453

Abstract

The observation that materials can change their properties when placed inside or near an optical resonator has sparked a fervid interest in understanding the effects of strong light–matter coupling on molecular dynamics, and several approaches have been proposed to extend the methods of computational chemistry into this regime. Whereas the majority of these approaches have focused on modeling a single molecule coupled to a single cavity mode, changes to chemistry have so far only been observed experimentally when very many molecules are coupled collectively to multiple modes with short lifetimes. While atomistic simulations of many molecules coupled to multiple cavity modes have been performed with semi-classical molecular dynamics, an explicit description of cavity losses has so far been restricted to simulations in which only a very few molecular degrees of freedom were considered. Here, we have implemented an effective non-Hermitian Hamiltonian to explicitly treat cavity losses in large-scale semi-classical molecular dynamics simulations of organic polaritons and used it to perform both mean-field and surface hopping simulations of polariton relaxation, propagation, and energy transfer.

Keywords: molecular dynamics; quasiparticles; polaritons; potential energy; computational chemistry; photochemistry

Free keywords: molecular dynamics; atomistic simulations; computational chemistry; diabatic states; potential energy surfaces; quantum mechanical/molecular mechanical calculations; surface hopping; nanoplasmonics; quasiparticle; photochemistry

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