Jahn-Teller effect versus Hund's rule coupling in C60N-

Abstract

We propose variational states for the ground state and the low-energy collective rotator excitations in negatively charged C N− 60 ions (N = 1 . . . 5). The approach includes the linear electron-phonon coupling and the Coulomb interaction on the same level. The electron-phonon coupling is treated within the effective mode approximation (EMA) which yields the linear t1u ⊗Hg Jahn-Teller problem whereas the Coulomb interaction gives rise to Hund's rule coupling for N = 2, 3, 4. The Hamiltonian has accidental SO(3) symmetry which allows an elegant formulation in terms of angular momenta. Trial states are constructed from coherent states and using projection operators onto angular momentum subspaces which results in good variational states for the complete parameter range. The evaluation of the corresponding energies is to a large extent analytical. We use the approach for a detailed analysis of the competition between Jahn-Teller effect and Hund's rule coupling, which determines the spin state for N = 2, 3, 4. We calculate the low-spin/high-spin gap for N = 2, 3, 4 as a function of the Hund's rule coupling constant J. We find that the experimentally measured gaps suggest a coupling constant in the range J = 60 − 80 meV. Using a finite value for J, we recalculate the ground state energies of the C N− 60 ions and find that the Jahn-Teller energy gain is partly counterbalanced by the Hund's rule coupling. In particular, the ground state energies for N = 2, 3, 4 are almost equal.