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

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.

arXiv comment5 pages, 4 figures

References in corpus (5)

• A new intermolecular mechanism to selectively drive photoinduced damages
• The role of metal ions in X-ray induced photochemistry
• Tracing ultrafast interatomic electronic decay processes in real time and space
• Observation of intermolecular Coulombic decay in liquid water
• Overcoming blockade in producing doubly-excited dimers by a single intense pulse and their decay

Cited by in corpus (2)

• Electronic-vibrational dynamics and coherence in x-ray transient absorption of N2+ induced by strong-field ionization
• Spectral Signatures of Vibronic Coupling in Trapped Cold Ionic Rydberg Systems