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arXiv · 2303.04844

Observation of Nuclear-wavepacket Interference in Ultrafast Inter-atomic Energy Transfer

Meng Han·Jacqueline Fedyk·Jia-Bao Ji·Victor Despré·Alexander I. Kuleff·Hans Jakob Wörner
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Abstract

We report the experimental observation of quantum interference in the nuclear wave-packet dynamics driving ultrafast excitation-energy transfer in argon dimers below the threshold of interatomic Coulombic decay (ICD). Using time-resolved photoion-photoion coincidence spectroscopy and quantum dynamics simulations, we reveal that the electronic relaxation dynamics of the inner-valence $3s$ hole on one atom leading to a $4s$ or $4p$ excitation on the other one is influenced by nuclear quantum dynamics in the initial state, giving rise to a deep, periodic modulation on the kinetic-energy-release (KER) spectra of the coincident Ar$^+$-Ar$^+$ ion pairs. Moreover, the time-resolved KER spectra show characteristic fingerprints of quantum interference effects during the energy-transfer process. Our findings pave the way to elucidating quantum-interference effects in ultrafast charge- and energy-transfer dynamics in more complex systems.

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Meng Han, Jacqueline Fedyk, Jia-Bao Ji, Victor Despré, Alexander I. Kuleff, Hans Jakob Wörner. 2023-03-08. Observation of Nuclear-wavepacket Interference in Ultrafast Inter-atomic Energy Transfer. https://doi.org/10.1103/physrevlett.130.253202

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