1. Ultrafast relaxation of photoexcited superfluid He nanodroplets.
- Author
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Mudrich, M, LaForge, A, Ciavardini, A, OKeeffe, P, Callegari, C, Coreno, M, Demidovich, A, Devetta, M, Fraia, M, Drabbels, M, Finetti, P, Gessner, Oliver, Grazioli, C, Hernando, A, Neumark, Daniel, Ovcharenko, Y, Piseri, P, Plekan, O, Prince, K, Richter, R, Ziemkiewicz, M, Möller, T, Eloranta, J, Pi, M, Barranco, M, and Stienkemeier, F
- Abstract
The relaxation of photoexcited nanosystems is a fundamental process of light-matter interaction. Depending on the couplings of the internal degrees of freedom, relaxation can be ultrafast, converting electronic energy in a few fs, or slow, if the energy is trapped in a metastable state that decouples from its environment. Here, we study helium nanodroplets excited resonantly by femtosecond extreme-ultraviolet (XUV) pulses from a seeded free-electron laser. Despite their superfluid nature, we find that helium nanodroplets in the lowest electronically excited states undergo ultrafast relaxation. By comparing experimental photoelectron spectra with time-dependent density functional theory simulations, we unravel the full relaxation pathway: Following an ultrafast interband transition, a void nanometer-sized bubble forms around the localized excitation (He[Formula: see text]) within 1 ps. Subsequently, the bubble collapses and releases metastable He[Formula: see text] at the droplet surface. This study highlights the high level of detail achievable in probing the photodynamics of nanosystems using tunable XUV pulses.
- Published
- 2020