Radiative Emission of Polaritons Controlled by Light-Induced Geometric Phase

TL;DR

This paper demonstrates that the ultrafast radiative emission of molecular polaritons can be controlled by the geometric phase induced by light-induced conical intersections, offering new insights into polariton emission dynamics.

Contribution

It introduces a method to compute polariton emission signals by incorporating a geometric phase into the Born-Oppenheimer approximation.

Findings

Radiative emission is controlled by the geometric phase from LICIs.

The approach enhances understanding of polariton emission processes.

The method allows for more accurate modeling of polariton dynamics.

Abstract

Polaritons - hybrid light-matter states formed in cavity - strongly change the properties of the underlying matter. In optical or plasmonic nanocavities, polaritons decay by radiative emission of the cavity, which is accessible experimentally. Due to the interaction of a molecule with the quantized radiation field, polaritons exhibit light-induced conical intersections (LICIs) which dramatically influence the nuclear dynamics of molecular polaritons. We show that ultrafast radiative emission from the lower polariton is controlled by the geometric phase imposed by the LICI. This finding provides insight into the process of emission and, furthermore, allows one to compute these signals by augmenting the Born-Oppenheimer approximation for polaritons with a geometric phase term.