Floquet engineering of molecular dynamics via infrared coupling

TL;DR

This paper explores how periodic infrared driving and cavity coupling can be used to control and enhance molecular vibrational and electronic dynamics, leading to tailored optical responses and suppressed sidebands.

Contribution

It introduces a Floquet engineering approach to manipulate molecular vibrational and vibronic coherence using infrared fields and cavity modes, with a detailed theoretical framework.

Findings

Enhanced vibronic coherence observed

Controlled suppression of vibrational sidebands

Modified optical response of infrared-dressed molecules

Abstract

We discuss Floquet engineering of dissipative molecular systems through periodic driving of an infrared-active vibrational transition, either directly or via a cavity mode. Following a polaron quantum Langevin equations approach, we derive correlation functions and stationary quantities showing strongly modified optical response of the infrared-dressed molecule. The coherent excitation of molecular vibrational modes, in combination with the modulation of electronic degrees of freedom due to vibronic coupling can lead to both enhanced vibronic coherence as well as control over vibrational sideband amplitudes. The additional coupling to an infrared cavity allows for the controlled suppression of undesired sidebands, an effect stemming from the Purcell enhancement of vibrational relaxation rates.