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As opposed to purely molecular systems where electron dynamics proceed onlythrough intramolecular processes, weakly bound complexes such as He dropletsoffer an environment where local excitations can interact with neighbouringembedded molecules leading to new intermolecular relaxation mechanisms. Here,we report on a new decay mechanism leading to the double ionization of alkalidimers attached to He droplets by intermolecular energy transfer. From theelectron spectra, the process is similar to the well-known shake-off mechanismobserved in double Auger decay and single-photon double ionization, however, inthis case, the process is dominant, occurring with efficiencies equal to, orgreater than, single ionization by energy transfer. Although an alkali dimerattached to a He droplet is a model case, the decay mechanism is relevant forany system where the excitation energy of one constituent exceeds the doubleionization potential of another neighbouring molecule. The process is, inparticular, relevant for biological systems, where radicals and slow electronsare known to cause radiation damage

Highly efficient double ionization of mixed alkali dimers by intermolecular Coulombic decay