High frequency EPR on dilute solutions of the single molecule magnet Ni4_4

Dilute frozen solutions of the single molecule magnet Ni$_4$ (S=4) have been studied using high frequency D-band (130 GHz) EPR. Despite the random orientation of the molecules, well defined EPR absorption peaks are observed, due to the strong variation of the splittings between the different spin-states on magnetic field. Temperature dependent studies above 4 K and comparison with simulations enable identification of the spin transitions and determination of the Hamiltonian parameters. The latter are found to be close to those of Ni$_4$ single crystals. No echo was detected from Ni$_4$ in pulsed experiments, which sets an upper bound of about 50 ns on the spin coherence time.Comment: 4 pages, 3 figures, accepted for publication in Journal of Applied Physics (52nd MMM conference proceedings

Measurement of Magnetization Dynamics in Single-Molecule Magnets Induced by Pulsed Millimeter-Wave Radiation

We describe an experiment aimed at measuring the spin dynamics of the Fe8 single-molecule magnet in the presence of pulsed microwave radiation. In earlier work, heating was observed after a 0.2-ms pulse of intense radiation, indicating that the spin system and the lattice were out of thermal equilibrium at millisecond time scale [Bal et al., Europhys. Lett. 71, 110 (2005)]. In the current work, an inductive pick-up loop is used to probe the photon-induced magnetization dynamics between only two levels of the spin system at much shorter time scales (from ns to us). The relaxation time for the magnetization, induced by a pulse of radiation, is found to be on the order of 10 us.Comment: 3 RevTeX pages, including 3 eps figures. The paper will appear in the Journal of Applied Physics as MMM'05 conference proceeding

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

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.Comment: 11 pages including 2 figure