English

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

Atomic and Molecular Clusters 2023-07-05 v1 Chemical Physics

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 3s3s hole on one atom leading to a 4s4s or 4p4p 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.

Keywords

Cite

@article{arxiv.2303.04844,
  title  = {Observation of Nuclear-wavepacket Interference in Ultrafast Inter-atomic Energy Transfer},
  author = {Meng Han and Jacqueline Fedyk and Jia-Bao Ji and Victor Despré and Alexander I. Kuleff and Hans Jakob Wörner},
  journal= {arXiv preprint arXiv:2303.04844},
  year   = {2023}
}

Comments

5 pages, 4 figures