Two-dimensional Infrared Spectroscopy of vibrational polaritons of molecules in an optical cavity

TL;DR

This paper explores how vibrational polaritons formed by molecules in an optical cavity can be controlled and probed using two-dimensional infrared spectroscopy, revealing insights into molecular vibrational states.

Contribution

It demonstrates control over vibrational polariton states via cavity coupling strength and introduces a time domain 2DIR technique for probing these states.

Findings

Control of single and double vibrational polariton manifolds.

Application of Double Quantum Coherence (DQC) spectroscopy.

Insights into amide-I and amide-II vibrational modes.

Abstract

Strong coupling of molecular vibrations to an infrared cavity mode affects their nature by creating dressed polariton states. We show how the single and double vibrational polariton manifolds may be controlled by varying the cavity coupling strength, and probed by a time domain 2DIR technique, Double Quantum Coherence (DQC). Applications are made to the amide-I ($CO$) and amide-II ($CN$) bond vibrations of $N-methylacetamide$ (NMA).