Machine Learning Framework for Modeling Exciton-Polaritons in Molecular Materials

Fuente: arXiv
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Autori principali: Li, Xinyang, Lubbers, Nicholas, Tretiak, Sergei, Barros, Kipton, Zhang, Yu
Natura: Preprint
Pubblicazione: 2023
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author Li, Xinyang
Lubbers, Nicholas
Tretiak, Sergei
Barros, Kipton
Zhang, Yu
author_facet Li, Xinyang
Lubbers, Nicholas
Tretiak, Sergei
Barros, Kipton
Zhang, Yu
contents A light-matter hybrid quasiparticle, called a polariton, is formed when molecules are strongly coupled to an optical cavity. Recent experiments have shown that polariton chemistry can manipulate chemical reactions. Polariton chemistry is a collective phenomenon and its effects increase with the number of molecules in a cavity. However, simulating an ensemble of molecules in the excited state coupled to a cavity mode is theoretically and computationally challenging. Recent advances in machine learning techniques have shown promising capabilities in modeling ground state chemical systems. This work presents a general protocol to predict excited-state properties, such as energies, transition dipoles, and non-adiabatic coupling vectors with the hierarchically interacting particle neural network. Machine learning predictions are then applied to compute potential energy surfaces and electronic spectra of a prototype azomethane molecule in the collective coupling scenario. These computational tools provide a much-needed framework to model and understand many molecules' emerging excited-state polariton chemistry.
format Preprint
id arxiv_https___arxiv_org_abs_2306_02523
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Machine Learning Framework for Modeling Exciton-Polaritons in Molecular Materials
Li, Xinyang
Lubbers, Nicholas
Tretiak, Sergei
Barros, Kipton
Zhang, Yu
Chemical Physics
A light-matter hybrid quasiparticle, called a polariton, is formed when molecules are strongly coupled to an optical cavity. Recent experiments have shown that polariton chemistry can manipulate chemical reactions. Polariton chemistry is a collective phenomenon and its effects increase with the number of molecules in a cavity. However, simulating an ensemble of molecules in the excited state coupled to a cavity mode is theoretically and computationally challenging. Recent advances in machine learning techniques have shown promising capabilities in modeling ground state chemical systems. This work presents a general protocol to predict excited-state properties, such as energies, transition dipoles, and non-adiabatic coupling vectors with the hierarchically interacting particle neural network. Machine learning predictions are then applied to compute potential energy surfaces and electronic spectra of a prototype azomethane molecule in the collective coupling scenario. These computational tools provide a much-needed framework to model and understand many molecules' emerging excited-state polariton chemistry.
title Machine Learning Framework for Modeling Exciton-Polaritons in Molecular Materials
topic Chemical Physics
url https://arxiv.org/abs/2306.02523