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. C_3v 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.