Unprecedented Prediction of a B 160 Cluster Stuffed by Dual-Icosahedron B 12 .

Serving as the premise to understand bulk allotropes, boron clusters have been intriguing experimentalists and theoreticians to study their geometries and chemical bonding. Here, we designed a complete core-shell B 160 cluster stuffed by two B 12 cores, which is energetically preferable over the bilayer structure of the same size. The unprecedented peanutlike structure with C i symmetry has superior stability and exhibits superatomic electronic configuration and spherical aromaticity. Our theoretical work not only proposed the core-shell structure of dual icosahedrons for the first time but also indicated the multi-B 12 core-shell structural pattern in boron particles, bridging to boron crystalline structures.