Simulating anharmonic vibrational polaritons beyond the long wavelength approximation

TL;DR

This paper develops a theoretical framework to simulate anharmonic vibrational polaritons beyond the long-wavelength approximation, incorporating localized light-matter interactions and anharmonic effects.

Contribution

It introduces a simple, localized model for light-matter coupling and employs self-consistent phonon and vibrational DMFT to simulate spectra including anharmonicity.

Findings

Accurately simulates momentum-resolved vibrational-polariton spectra.

Demonstrates applicability to model systems.

Includes effects of anharmonicity in the spectra.

Abstract

In this work we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of light-matter interactions, where spatially localized cavity radiation modes couple to localized vibrations. Within this theoretical framework, we employ self-consistent phonon theory and vibrational dynamical mean-field theory to efficiently simulate momentum-resolved vibrational-polariton spectra, including effects of anharmonicity. Numerical simulations in model systems demonstrate the accuracy and applicability of our approach.