Ultrafast relaxation of photoexcited superfluid He nanodroplets

Mudrich, M.; LaForge, A. C.; Ciavardini, A.; O’Keeffe, P.; Callegari, C.; Coreno, M.; Demidovich, A.; Devetta, M.; Fraia, M. Di; Drabbels, M.; Finetti, P.; Gessner, O.; Grazioli, C.; Hernando, A.; Neumark, D. M.; Ovcharenko, Y.; Piseri, P.; Plekan, O.; Prince, K. C.; Richter, R.; Ziemkiewicz, M. P.; Möller, T.; Eloranta, J.; Pi, M.; Barranco, M.; Stienkemeier, F.

doi:10.1038/s41467-019-13681-6

Title: Ultrafast relaxation of photoexcited superfluid He nanodroplets

Journal Article · 07 January 2020 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-13681-6 · OSTI ID:1599845

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Aarhus Univ. (Denmark)
Univ. of Freiburg, Freiburg im Breisgau (Germany); Univ. of Connecticut, Storrs, CT (United States)
Central European Research Infrastructure Consortium (CERIC–ERIC), Trieste (Italy); Italian National Research Council (CNR), Monterotondo Scalo (Italy)
Italian National Research Council (CNR), Monterotondo Scalo (Italy)
Elettra Sincrotrone Trieste (Italy)
Italian National Research Council (CNR), Trieste (Italy); Univ. degli Studi, Milan (Italy)
Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne (Switzerland)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Italian National Research Council (CNR), Trieste (Italy)
Kido Dynamics, Lausanne (Switzerland); Inst. de Fisica Interdisciplinar y Sistemas Complejos, Palma de Mallorca (Spain)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
European X-Ray Free-Electron Laser Facility (XFEL), Schenefeld (Germany); Inst. für Optik und Atomare Physik, Berlin (Germany)
Univ. degli Studi, Milan (Italy)
Inst. für Optik und Atomare Physik, Berlin (Germany)
California State Univ., Northridge, CA (United States)
Univ. de Barcelona (Spain)
Univ. de Barcelona (Spain); Univ. Paul Sabatier-Toulouse (France)
Univ. of Freiburg, Freiburg im Breisgau (Germany)

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*) within 1 ps. Subsequently, the bubble collapses and releases metastable He* at the droplet surface. This study highlights the high level of detail achievable in probing the photodynamics of nanosystems using tunable XUV pulses.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; Deutsche Forschungsgemeinschaft; National Science Foundation (NSF); Carl-Zeiss-Stiftung; Swiss National Science Foundation

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1599845

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Vibrational relaxation and dephasing of Rb2 attached to helium nanodroplets Grüner, Barbara; Schlesinger, Martin; Heister, Philipp arXiv https://doi.org/10.48550/arxiv.1011.0924	text	January 2010
Laser-induced rotation of iodine molecules in He-nanodroplets: revivals and breaking-free Shepperson, Benjamin; Søndergaard, Anders A.; Christiansen, Lars arXiv https://doi.org/10.48550/arxiv.1702.01977	text	January 2017
Femtosecond photoexcitation dynamics inside a quantum solvent Thaler, Bernhard; Ranftl, Sascha; Heim, Pascal arXiv https://doi.org/10.48550/arxiv.1804.04497	text	January 2018
Quantum dynamics of Rb atoms desorbing off the surface of He nanodroplets Dozmorov, N. V.; von Vangerow, J.; Fordyce, J. A. M. arXiv https://doi.org/10.48550/arxiv.1809.04846	text	January 2018

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Molecular sunscreen: water protects pyrrole from radiation damage Johny, Melby; Schouder, Constant A.; Al-Refaie, Ahmed arXiv https://doi.org/10.48550/arxiv.2010.00453	preprint	January 2020

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