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See supplementary material ftp://ftp.aip.org/epaps/journ_chem_phys/E-JCPSA6-145-030643 for experimental data for (C60)N (N = 1-6) in combination with atomic Cs and small Csn clusters, as well as details on the DFT calculations performed in this work.Alkali metal atoms and small alkali clusters are classic heliophobes and when in contact with liquid helium they reside in a dimple on the surface. Here we show that alkalis can be induced to submerge into liquid helium when a highly polarizable co-solute, C60, is added to a helium nanodroplet. Evidence is presented that shows that all sodium clusters, and probably single Na atoms, enter the helium droplet in the presence of C60. Even clusters of cesium, an extreme heliophobe, dissolve in liquid helium when C60 is added. The sole exception is atomic Cs, which remains at the surface.This work was given financial support by the Austrian Science Fund (FWF) via Grant Nos. I978 and P26635. A.W.H. thanks Marti Pi for helpful discussions at the MOLIM WG3 meeting in Bratislava, Slovakia, supported by the COST Action No. CM1405 “Molecules in Motion.”Peer-reviewedPublisher Versio

Communication: Dopant-induced solvation of alkalis in liquid helium nanodroplets