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.

14 pages, 4 figures in the main text and 27 pages, 12 figures, and 4 tables in the Supplementary Material

References in corpus (3)

• Enantiomer-Specific State Transfer of Chiral Molecules
• Complete Controllability Despite Degeneracy: Quantum Control of Enantiomer-Specific State Transfer in Chiral Molecules
• State-specific Enrichment of Chiral Conformers with Microwave Spectroscopy

Cited by in corpus (2)

• Chiral Electron Momentum Distribution upon Strong-Field Ionization of Atoms
• Fast chiral resolution with optimal control