Ab Initio Linear-Response Approach to Vibro-Polaritons in the Cavity Born-Oppenheimer Approximation.

ABSTRACT: Recent years have seen significant developments in the study of strong light-matter coupling including the control of chemical reactions by altering the vibrational normal modes of molecules. In the vibrational strong coupling regime, the normal modes of the system become hybrid modes which mix nuclear, electronic, and photonic degrees of freedom. First-principles methods capable of treating light and matter degrees of freedom on the same level of theory are an important tool in understanding such systems. In this work, we develop and apply a generalized force constant matrix approach to the study of mixed vibration-photon (vibro-polariton) states of molecules based on the cavity Born-Oppenheimer approximation and quantum-electrodynamical density-functional theory. With this method, vibro-

SUBMITTER: Bonini J 

PROVIDER: S-EPMC9097282 | biostudies-literature | 2022 May

REPOSITORIES: biostudies-literature