Tunneling with dissipation and decoherence for a large spin

We present rigorous solution of problems of tunneling with dissipation and decoherence for a spin of an atom or a molecule in an isotropic solid matrix. Our approach is based upon switching to a rotating coordinate system coupled to the local crystal field. We show that the spin of a molecule can be used in a qubit only if the molecule is strongly coupled with its atomic environment. This condition is a consequence of the conservation of the total angular momentum (spin + matrix), that has been largely ignored in previous studies of spin tunneling.Comment: 4 page

Detailed single crystal EPR lineshape measurements for the single molecule magnets Fe8Br and Mn12-ac

It is shown that our multi-high-frequency (40-200 GHz) resonant cavity technique yields distortion-free high field EPR spectra for single crystal samples of the uniaxial and biaxial spin S = 10 single molecule magnets (SMMs) [Mn12O12(CH3COO)16(H2O)4].2CH3COOH.4H2O and [Fe8O2(OH)12(tacn)6]Br8.9H2O. The observed lineshapes exhibit a pronounced dependence on temperature, magnetic field, and the spin quantum numbers (Ms values) associated with the levels involved in the transitions. Measurements at many frequencies allow us to separate various contributions to the EPR linewidths, including significant D-strain, g-strain and broadening due to the random dipolar fields of neighboring molecules. We also identify asymmetry in some of the EPR lineshapes for Fe8, and a previously unobserved fine structure to some of the EPR lines for both the Fe8 and Mn12 systems. These findings prove relevant to the mechanism of quantum tunneling of magnetization in these SMMs.Comment: Phys. Rev. B, accepted with minor revision