Effect of defects on the line shape of electron paramagnetic resonance signals from the single-molecule magnet Mn12: A theoretical study

Abstract

We herein estimate the effect of lattice defects on the line shape of electron paramagnetic resonance (EPR) signals from a single crystal of the S = 10 single-molecule magnet Mn 12 with the external magnetic field along the crystal c axis. A second-order perturbation treatment of an effective single-spin Hamiltonian indicates that a small, random, static misorientation of the magnetic symmetry axes in a crystalline lattice can lead to asymmetric EPR peaks. Full spectra are simulated by calculating probability-distribution functions for the resonant fields, employing distributions in the tilt angle of the easy axis from the c axis, in the uniaxial anisotropy parameter, and in the gfactor. We discuss conditions under which the asymmetry in the EPR spectra becomes prominent. The direction and magnitude of the asymmetry provide information on the specific energy levels involved with the EPR transition, the EPR frequency, and the distribution in the tilt angle.

Effect of extra electrons on the exchange and magnetic anisotropy in the anionic single-molecule magnetMn12

“…It has been suggested that the distribution in internal transverse fields could arise from a distribution in the magnetic easy axes of individual molecules. 16,17 But the origin of the distribution in the magnetic easy axes remains unknown. In this regard, we consider, within DFT, the possibility that extra electrons when accepted by Mn 12 molecules, will exhibit a disorder-or defect-induced behavior that is observed in the experimental samples.…”