From Aromatic to Antiaromatic: Charge-Induced Electronic Transformation and Unexpected Stability of B24Ni3.

The structural and electronic features of B24Ni3 were examined across multiple charge states, revealing a double-ring configuration with three Ni atoms encapsulated within the B24 framework. C3v symmetry is consistently favored, with the neutral and anionic species representing the global minima. Analyses of bond current strength and orbital interactions highlight the crucial role of the ψ(2 0 2) wave function in stabilizing the system through enhanced Ni-Ni and intraring B-B bonding. The transformation of ψ(2 0 2) into a ψ(3 3 1)-like character triggers rotational transitions, and the way these transitions are quenched becomes an intriguing story of this study. Born-Oppenheimer molecular dynamics simulations at 300-900 K and ΔG calculations confirm the high thermodynamic stability of both the neutral and anionic species. The neutral B24Ni3 is more stable overall, whereas the anion B24Ni3- exhibits rotational motion of the boron framework around the nickel atoms, highlighting its potential as an antiaromaticity antifriction bearing motor at high temperatures.