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We present high-frequency angle-dependent EPR data for crystals of[NixZn1-x(hmp)(t-BuEtOH)Cl]4 (x = 1 and 0.02). The x = 1 complex behaves as asingle-molecule magnet at low temperatures, displaying hysteresis andexceptionally fast magnetization tunneling. We show that this behavior isrelated to a 4th-order transverse crystal-field interaction, which produces asignificant tunnel-splitting (~10 MHz) of the ground state of this S = 4system. The magnitude of the 4th-order anisotropy, and the dominant axial term(D), can be related to the single-ion interactions (Di and Ei) at theindividual NiII sites, as determined for the x = 0.02 crystals.Comment: 11 pages including 2 figure

Origin of the fast magnetization tunneling in the single-molecule magnet [Ni(hmp)(t-BuEtOH)Cl]4