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 timedependent 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
Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics / Laforge, A. C.; Michiels, R.; Ovcharenko, Y.; Ngai, A.; Escartín, J. M.; Berrah, N.; Callegari, C.; Clark, A.; Coreno, M.; Cucini, R.; Di Fraia, M.; Drabbels, M.; Fasshauer, E.; Finetti, P.; Giannessi, L.; Grazioli, C.; Iablonskyi, D.; Langbehn, B.; Nishiyama, T.; Oliver, V.; Piseri, P.; Plekan, O.; Prince, K. C.; Rupp, D.; Stranges, S.; Ueda, K.; Sisourat, N.; Eloranta, J.; Pi, M.; Barranco, M.; Stienkemeier, F.; Möller, T.; Mudrich, M.. - In: PHYSICAL REVIEW. X. - ISSN 2160-3308. - 11:2(2021). [10.1103/PhysRevX.11.021011]
Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
Stranges, S.Membro del Collaboration Group
;
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 timedependent 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 oneI documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.