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

TL;DR

This paper develops a variational approach to study the competition between Jahn-Teller distortions and Hund's rule coupling in negatively charged C60 ions, providing insights into their ground states and spin configurations.

Contribution

It introduces a unified variational framework that includes electron-phonon and Coulomb interactions, enabling detailed analysis of spin states in C60N- ions.

Findings

The low-spin/high-spin gap depends on Hund's coupling J.

Experimental gaps suggest J=60-80meV.

Jahn-Teller energy gain is partly offset by Hund's coupling.

Abstract

We propose variational states for the ground state and the low-energy collective rotator excitations in negatively charged C60N- 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 t_{1u} x H_g 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=60-80meV. Using a finite value for J, we recalculate the ground state energies of the C60N- 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.