Observation of Multiple Ordered Solvation Shells in Doped Helium Droplets: The Case of HeNCa2+

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 HeNCa2+ 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 Mozartkugellike structures: He12Ca2+ with an icosahedron, the second at He32Ca2+ with a dodecahedron, the third at He44Ca2+ with a larger icosahedron, and finally for He74Ca2+, 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.

Automated summary

In this study, we have observed the largest ordered structure of helium atoms surrounding a monatomic impurity using a newly developed technique. The investigation of HeNCa2+ clusters formed in helium nanodroplets shows magic numbers at N = 12, 32, 44, and 74, indicating the presence of well-ordered shells surrounding the calcium dication. These shells exhibit Mozartkugellike structures and consist of different shapes such as an icosahedron, dodecahedron, and icosidodecahedron.