Journal Article PUBDB-2024-06652

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Direct observation of time-dependent coherent chiral tunneling dynamics

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2025
APS College Park, Md.

Physical review letters 134(12), 123403 () [10.1103/PhysRevLett.134.123403]
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Abstract: Superpositions of handed molecular states give rise to achiral eigenstates, delocalized across a double-well potential via tunneling. In principle, a coherent superposition of these stationary eigenstates could dynamically relocalize the molecules into chiral states, which has only been demonstrated 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, using enantiomeric excess as the observable. We also demonstrate precise phase control of this coherence via phase modulation during pump excitation. Our results offer foundational evidence for the superposition principle in chiral tunneling systems, with implications for advancing quantum control in these system.

Classification:

Contributing Institute(s):
  1. Spectroscopy of molecular processes (FS-SMP)
  2. FS-CFEL-3 (CFEL-DESYT)
  3. CFEL-Theory (FS-CFEL-3)
Research Program(s):
  1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
  2. SFB 1319 B02 - Enantiomerenunterscheidung, Trennung und Präzisionsuntersuchungen mittels zugeschnittener Mikrowellenfelder (B02) (389894861) (389894861)
  3. DFG project G:(GEPRIS)328961117 - SFB 1319: Extremes Licht zur Analyse und Kontrolle molekularer Chiralität (ELCH) (328961117) (328961117)
Experiment(s):
  1. No specific instrument

Appears in the scientific report 2025
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 Record created 2024-11-08, last modified 2025-07-22