Superexchange via Cluster States: Calculations of Spin-Phonon Coupling Constants for CuGeO3

Abstract

Calculations for spin-phonon coupling constants in CuGeO3 are presented, applying fourth order superexchange perturbation theory to an extended Hubbard model. In our treatment, the intermediate oxygen ligand states are described by band-like cluster states, due to the presence of significant O(p)-O(p) hopping. We also include the effect of the Ge ions on the O ligand states. We find a considerable q-dependence of the spin-phonon coupling. For the pi-modes involved in the spin-Peierls transition, our results of the coupling constants are in fair agreement with the work of Werner, Gros, and Braden. Yet some discrepancies remain, especially concerning the coupling to the vibrations, which modulate the O(2)-O(2)-Ge angle delta. Our studies of the pressure dependence of the magnetic coupling constants J_1 and J_2 suggest, that relatively large non-linear effects are present, even at small pressure values, probably due to the existence of a `soft', van-der-Waals-type bond direction in CuGeO3.