  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 a
single-molecule magnet at low temperatures, displaying hysteresis and
exceptionally fast magnetization tunneling. We show that this behavior is
related to a 4th-order transverse crystal-field interaction, which produces a
significant tunnel-splitting (~10 MHz) of the ground state of this S = 4
system. 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 the
individual NiII sites, as determined for the x = 0.02 crystals.
