Direct observation of time-dependent coherent chiral 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.