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Abstract
The relaxation of photoexcited nanosystems is a fundamental process of light-matter interaction. This study investigates helium nanodroplets excited resonantly by femtosecond extreme-ultraviolet (XUV) pulses. Despite their superfluid nature, ultrafast relaxation is observed in the lowest electronically excited states. Photoelectron spectra, compared with time-dependent density functional theory (TD-DFT) simulations, reveal a three-step relaxation pathway involving an ultrafast interband transition, bubble formation around the excitation, and bubble collapse releasing metastable He* at the droplet surface. The high detail achievable in probing nanosystem photodynamics using tunable XUV pulses is highlighted.
Publisher
Nature Communications
Published On
Jan 01, 2020
Authors
M. Mudrich, A.C. LaForge, A. Ciavardini, P. O’Keeffe, C. Callegari, M. Coreno, A. Demidovich, M. Devetta, M. Di Fraia, M. Drabbels, P. Finetti, O. Gessner, C. Grazioli, A. Hernando, D.M. Neumark, Y. Ovcharenko, P. Piseri, O. Plekan, K.C. Prince, R. Richter, M.P. Ziemkiewicz, T. Möller, J. Eloranta, M. Pi, M. Barranco
Tags
helium nanodroplets
photoexcitation
ultrafast relaxation
extreme-ultraviolet pulses
nanosystem photodynamics
time-dependent density functional theory
bubble formation
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