Superfluid He nanodroplets resonantly excited by extreme ultraviolet (XUV) pulses can relax via interatomic coulombic decay (ICD), generally considered an ultrafast process. Here, we introduce a novel approach to probe the dynamics of ICD in He nanodroplets over timescales ranging from femtoseconds to nanoseconds. Our method relies on detecting XUV fluorescence emitted from the nanodroplets as they are driven into a nanoplasma by subsequent intense infrared pulses. Nanoplasma ignition is facilitated by tunnel ionization of XUV-excited He[Formula: see text] atoms attached to the droplets; it thus serves as a sensitive probe of their relaxation dynamics. The observed nanosecond-scale decay is attributed to ICD between pairs of He[Formula: see text] atoms undergoing roaming motion on the droplet surface, as supported by quantum-mechanical and classical model calculations.

Czech Technical University Prague FNSPE Prague 115 19 Czech Republic

Department of Physics and Astronomy Aarhus University Ny Munkegade 120 Aarhus C 8000 Denmark

ELI Beamlines facility The Extreme Light Infrastructure ERIC Za Radnicí 835 Dolní Břežany 253 41 Czech Republic

HUN REN Wigner Research Centre for Physics Budapest H 1121 Hungary

IKERBASQUE Basque Foundation for Science Bilbao 48011 Spain

Institute of Physics University of Kassel Kassel 34132 Germany

Kimika Fakultatea Euskal Herriko Unibertsitatea P K 1072 Donostia 20080 Spain

Laboratoire Collisions Agrégats Réactivité Université de Toulouse CNRS Toulouse 31062 France

Quantum Center of Excellence for Diamond and Emergent Materials School of Interdisciplinary Sciences and Department of Physics Indian Institute of Technology Madras Chennai 600036 India

Wildau Technical University of Applied Sciences Hochschulring 1 Wildau 15745 Germany

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