In this work, we study the spin dynamics of ${\mathrm{Mn}}_{12}$-acetate molecules in the regime of thermally assisted tunneling. In particular, we describe the system in the presence of a strong transverse magnetic field. Similar to recent experiments, the relaxation time/rate is found to display a series of resonances; their Lorentzian shape is found to stem from the tunneling. The dynamic susceptibility $\chi \left(\omega \right)$ is calculated starting from the microscopic Hamiltonian and the resonant structure manifests itself also in $\chi \left(\omega \right).\mathrm{}$ Similar to recent results reported on another molecular magnet, ${\mathrm{Fe}}_8,$ we find oscillations of the relaxation rate as a function of the transverse magnetic field when the field is directed along a hard axis of the molecules. This phenomenon is attributed to the interference of the geometrical or Berry phase. We propose susceptibility experiments to be carried out for strong transverse magnetic fields to study these oscillations and for a better resolution of the sharp satellite peaks in the relaxation rates.

• Received 8 May 2000

DOI:https://doi.org/10.1103/PhysRevB.62.15026