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Kulichenko, Maksim; Fedik, Nikita; Boldyrev, Alexander; Muñoz‐Castro, Alvaro
Chemistry : a European journal, February 17, 2020, Letnik: 26, Številka: 10Journal Article
Structural characterization of the discrete Sn@Cu12@Sn2012− cluster exposed a fascinating architecture composed of three concentric structural layers in which an endohedral Sn atom is enclosed in a Cu12 icosahedron, which in turn is embedded in an Sn20 dodecahedron. Herein, the possibility of sustaining aromatic behavior for this prototypical multilayered species was evaluated, in order to extend this concept to more complex clusters on the basis of magnetic response and bonding analysis by the AdNDP approach. This revealed characteristic features of spherical aromatics, given by the ability to sustain the shielding cone property, similar to archetypal aromatics. The favorable bonding pattern in the Sn@Cu12@Sn2012− cluster fulfills the 2(N+1)2 Hirsch rule for aromaticity; thus, the cluster could be regarded as a first member of aromatic multilayered structures. The set of four 13c–2e aromatic bonds that was identified in the internal SnCu12 structure results in spherical aromatic character of this multilayered cluster. This insight builds a bridge between the traditional concept of Hückel's aromaticity and the aromaticity of complex and stable 3D systems that may be explored on the basis of magnetic response and bonding analysis. It also may open a way to novel findings in bottled clusters displaying aromatic behavior in multilayer structures, which are of great interest for inorganic nano‐ and material sciences due to their unprecedented stability. Russian doll aromatic: The Sn@Cu12@Sn2012− cluster, in which an endohedral Sn atom is enclosed in a Cu12 icosahedron, which in turn is embedded in an Sn20 dodecahedron, was shown by theoretical calculations to exhibit spherical aromaticity. Its shielding cone, which remains parallel to applied fields aligned in different orientations, resembles that of the classical planar aromatic compound benzene (see figure).
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