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Interatomic Coulombic decay (ICD) processes play a crucial role in weaklybound complexes exposed to intense or high-energy radiation. Using large heliumnanodroplets, we demonstrate that ICD is efficient even when the droplets areirradiated by weak synchrotron radiation at relatively low photon energies.Below the ionization threshold, resonant excitation of multiple centersefficiently induces resonant ICD as previously observed for intense pulses [A.C. LaForge et al., PRX 11, 021011 (2021)]. More surprisingly, we observe ICDeven above the ionization threshold due to recombination of photoelectrons andions into excited states which subsequently decay by ICD. This demonstrates theimportance of secondary processes, in particular electron scattering andrecombination, in inducing ICD in extended condensed phase systems. Inaddition, we show that ICD can serve as a diagnostic tool for monitoring therelaxation dynamics of highly-excited and ionized weakly-bound nanosystems.

Spectroscopically resolved resonant interatomic Coulombic decay in photoexcited large He nanodroplets