Observation of Multiple Ordered Solvation Shells in Doped Helium Droplets: The Case of He(N)Ca(2+)

[Image: see text] In this Letter, we report the experimental detection of likely the largest ordered structure of helium atoms surrounding a monatomic impurity observed to date using a recently developed technique. The mass spectrometry investigation of He(N)Ca(2+) clusters, formed in multiply charged helium nanodroplets, reveals magic numbers at N = 12, 32, 44, and 74. Classical optimization and path integral Monte Carlo calculations suggest the existence of up to four shells surrounding the calcium dication which are closed with well-ordered Mozartkugel-like structures: He(12)Ca(2+) with an icosahedron, the second at He(32)Ca(2+) with a dodecahedron, the third at He(44)Ca(2+) with a larger icosahedron, and finally for He(74)Ca(2+), we find that the outermost He atoms form an icosidodecahedron which contains the other inner shells. We analyze the reasons for the formation of such ordered shells in order to guide the selection of possible candidates to exhibit a similar behavior.