Machine Learning Framework for Modeling Exciton Polaritons in Molecular Materials

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 (ML) 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 nonadiabatic coupling vectors with the hierarchically interacting particle neural network. ML predictions are then applied to compute the 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.