Direct observation of time-dependent coherent chiral tunneling dynamics

TL;DR

This study experimentally observes and controls the time-dependent coherent tunneling between chiral states in molecules using microwave spectroscopy, revealing periodic dynamics and phase control of chiral superpositions.

Contribution

First experimental demonstration of real-time, phase-controlled coherent chiral tunneling dynamics in molecules using microwave six-wave mixing spectroscopy.

Findings

Periodic time evolution of chiral wavepackets observed

Phase modulation enables precise control of chiral coherence

Field-free conditions allow natural tunneling dynamics

Abstract

Superpositions of handed molecular states give rise to achiral eigenstates, delocalized across a double-well potential via tunneling. A coherent superposition of these energy eigenstates could dynamically relocalize the molecules into chiral states, which has only been addressed theoretically. Here, we present a microwave six-wave mixing pump-probe study to create and probe coherent chiral tunneling dynamics in a rotational state. Through a time-resolved scheme, we uncover the periodic time evolution of the induced chiral wavepacket under field-free conditions. Moreover, we demonstrate precise phase control of this coherence via phase modulation during pump excitation.