Geometric-phase interference in a Mn12 single-molecule magnet with fourfold rotational symmetry

We study the magnetic relaxation rate Γ of the single-molecule magnet Mn(12)-tBuAc as a function of the 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 Γ 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 Γ 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 fourfold symmetry.