Quantum coherence is a fundamental mechanism driving ultrafast molecular reaction dynamics, playing a decisive role in processes such as light-induced ultrafast vision molecular isomerization and dissociation. However, due to the complexity of highly excited states in polyatomic molecules and interference from decoherence processes, directly observing vibrational quantum coherence signals from excited states has long been a major experimental challenge. This study, using time-resolved photoelectron spectroscopy, clearly resolves quantum beat signals resulting from interference between different vibrational states during the ultrafast predissociation dynamics of excited SF6 molecules. By combining high-precision calculations of the excited state potential energy surface and quantum dynamics simulations, the vibrational levels involved in the quantum coherence process are identified, and the lifetimes of the predissociating vibrational states are quantitatively analyzed. This work opens new avenues for understanding the role of quantum coherence in complex photo-induced ultrafast chemical reactions and ultimately for achieving active control over them.

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The research paper, published on Mar 23, 2026 in the journal Cyborg and Bionic Systems.