Lattice Distortion Mediated Paramagnetic Relaxation in High-Spin High-Symmetry Molecular Magnets

Field-dependent maxima in the relaxation rate of the magnetic molecules Mn12-Ac and Fe8-tacn have commonly been ascribed to some resonant tunneling phenomenon. We argue instead that the relaxation can be understood as purely due to phonons. The rate maxima arise because of a Jahn-Tellerlike distortion caused by the coupling of lattice phonons to degenerate Zeeman levels of the molecule at the top of the barrier. The binding energy of the distorted intermediate states lowers the barrier height and increases the relaxation rate. A nonperturbative calculation of this effect is carried out for a model system. An approximate result for the field variation near a maximum is found to agree reasonably with experiment. 76.30.-v, 76.20.+q, 75.80.+q, 75.60.Ej Typeset using REVTEX