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A theory of the magnetic relaxation of a large spin (S=10) having a large uniaxial magnetocrystalline anisotropy is outlined. The theory explains magnetic relaxation observed in Mn12 acetate. The joint action of local fields and a fourth order distortion of the magnetocrystalline anisotropy is necessary to account for the tunneling that is observed, between the m=-4 and m=4 unperturbed states. Even in resonance, tunneling takes place mainly incoherently in Mn12 acetate. It proceeds through the lowest energy state doublet which is not blocked by longitudinal local fields. The relaxation rate Γ has been calculated using a master equation. The model gives magnetization hysteresis loops and ac magnetic susceptibility curves which are in quantitative agreement with experimental results. For temperatures below 0.5 K approximately, nonresonant tunneling from the ground state becomes the dominant relaxation mechanism. © 1998 American Institute of Physics.
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