Hund’s rule magnetism in C <InlineEquation ID="Equ1"> <EquationSource Format="TEX">$\mathsf{_{60}}$</EquationSource> </InlineEquation> ions?

We investigate the occurrence of Hund’s rule magnetism in C<InlineEquation ID="Equ2"> <EquationSource Format="TEX">$_{60}^{n\pm}$</EquationSource> </InlineEquation> molecular ions, by computing the ground-state spin for all charge states n from -3 to +5. The two competing interactions, electron-vibration (e-v, including Jahn Teller, favoring low spin) and electron-electron (e-e, including Hund-rule exchange, favoring high spin), are accounted for based on previously computed ab initio coupling parameters. Treating the ion coordinates as classical, we first calculate and classify the static Jahn-Teller distorted states for all n, inclusive of both e-v and e-e effects. We then correct the adiabatic result by including the zero-point energy lowering associated with softening of vibrations at the adiabatic Jahn-Teller minima. Our overall result is that while, like in previous investigations, low-spin states prevail in negative ions, Hund’s rule high spin dominates all positive C<Subscript>60</Subscript> <Superscript> n+</Superscript> ions. This suggests also that Hund-rule magnetism could arise in fullerene cation-based solid state compounds, particularly those involving C<Subscript>60</Subscript> <Superscript>2+</Superscript>. Copyright Springer-Verlag Berlin/Heidelberg 2003