Geometric-phase interference in a Mn_{12} single-molecule magnet with four-fold rotational symmetry

Abstract: We study the magnetic relaxation rate Gamma of the single-molecule magnet Mn_{12}-tBuAc as a function of magnetic field component H_T transverse to the molecule's easy axis. When the spin is near a magnetic quantum tunneling resonance, we find that Gamma increases abruptly at certain values of H_T. These increases are observed just beyond values of H_T at which a geometric-phase interference effect suppresses tunneling between two excited energy levels. The effect is washed out by rotating H_T away from the spin's hard axis, thereby suppressing the interference effect. Detailed numerical calculations of Gamma using the known spin Hamiltonian accurately reproduce the observed behavior. These results are the first experimental evidence for geometric-phase interference in a single-molecule magnet with true four-fold symmetry.