Interatomic processes play a crucial role in weakly bound complexes exposed to ionizing radiation; therefore, gaining a thorough understanding of their efficiency is of fundamental importance. Here, we directly measure the timescale of interatomic Coulombic decay (ICD) in resonantly excited helium nanodroplets using a high-resolution, tunable, extreme ultraviolet free-electron laser. Over an extensive range of droplet sizes and laser intensities, we discover the decay to be surprisingly fast, with decay times as short as 400 fs, nearly independent of the density of the excited states. Using a combination of time-dependent density functional theory and ab initio quantum chemistry calculations, we elucidate the mechanisms of this ultrafast decay process, where pairs of excited helium atoms in one droplet strongly attract each other and form merging void bubbles, which drastically accelerates ICD.

Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics

Coreno M;Cucini R;Di Fraia M;Finetti P;Grazioli C;
2021

Abstract

Interatomic processes play a crucial role in weakly bound complexes exposed to ionizing radiation; therefore, gaining a thorough understanding of their efficiency is of fundamental importance. Here, we directly measure the timescale of interatomic Coulombic decay (ICD) in resonantly excited helium nanodroplets using a high-resolution, tunable, extreme ultraviolet free-electron laser. Over an extensive range of droplet sizes and laser intensities, we discover the decay to be surprisingly fast, with decay times as short as 400 fs, nearly independent of the density of the excited states. Using a combination of time-dependent density functional theory and ab initio quantum chemistry calculations, we elucidate the mechanisms of this ultrafast decay process, where pairs of excited helium atoms in one droplet strongly attract each other and form merging void bubbles, which drastically accelerates ICD.
2021
Istituto di Struttura della Materia - ISM - Sede Roma Tor Vergata
Istituto Officina dei Materiali - IOM -
Istituto di Struttura della Materia - ISM - Sede Secondaria Trieste
Autoionization & Auger processes
Collective effects in clusters
Density functional theory
Diffusion & dynamics of clusters
Laser-cluster interaction
Single- and few-photon ionization & excitation
Ultrafast phenomena
Fluid Dynamics
Atomic
Molecular & Optical physics
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.14243/395656
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