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Register a new userQuantum interference oscillations of the superparamagnetic blocking in an Fe8 molecular nanomagnet
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We show that the dynamic magnetic susceptibility and the superparamagnetic blocking temperature of an Fe8 single molecule magnet oscillate as a function of the magnetic field Hx applied along its hard magnetic axis. These oscillations are associated with quantum interferences, tuned by Hx, between different spin tunneling paths linking two excited magnetic states. The oscillation period is determined by the quantum mixing between the ground S=10 and excited multiplets. These experiments enable us to quantify such mixing. We find that the weight of excited multiplets in the magnetic ground state of Fe8 amounts to approximately 11.6%.
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Time-dependent specific heat experiments on the molecular nanomagnet Fe8 and the isotopic enriched analogue 57Fe8 are presented. The inclusion of the 57Fe nuclear spins leads to a huge enhancement of the specific heat below 1 K, ascribed to a strong increase in the spin-lattice relaxation rate Gamma arising from incoherent, nuclear-spin-mediated magnetic quantum tunneling in the ground-doublet. Since Gamma is found comparable to the expected tunneling rate, the latter process has to be inelastic. A model for the coupling of the tunneling levels to the lattice is presented. Under transverse field, a crossover from nuclear-spin-mediated to phonon-induced tunneling is observed.
Ramsey et al. [Nature Phys. 4, 277-281 (2008)] report the observation of quantum interference associated with tunnelling trajectories between states of different total spin length in a dimeric molecular nanomagnet. They argue that the interference is a consequence of the unique characteristics of a molecular Mn12 wheel, which behaves as a molecular dimer with weak ferromagnetic exchange coupling. We show here that the data published by Ramsey et al. are not consistent and unfortunately mostly wrong. We show further that the Landau-Zener (LZ) formula, which links the tunnel probability with the tunnel splitting, can only be applied in a well-defined experimental region, which lays outside the region accessed by Ramsey and colleagues. Only a lower-limit estimate of the tunnel splitting can be obtained, showing that the observed transition cannot be explained with the dimer model. We also present other shortcomings of the paper questioning the dimer model, and that the alignment of the magnetic field is crucial for observing quantum interference.
A Mn30 molecular cluster is established to be the largest single-molecule magnet (SMM) discovered to date. Magnetization versus field measurements show coercive fields of about 0.5 T at low temperatures. Magnetization decay experiments reveal an Arrhenius behavior and temperature-independent relaxation below 0.2 K diagnostic of quantum tunneling of magnetization through the anisotropy barrier.The quantum hole digging method is used to establish resonant quantum tunneling. These results demonstrate that large molecular nanomagnets,having a volume of 15 nm^3, with dimensions approaching the mesoscale can still exhibit the quantum physics of the microscale.
We present here an exact version of our response (dated April 27) to Wernsdorfers correspondence submitted to Nature Physics on March 31, 2008. After consultation with a referee, Nature Physics chose not publish any part of this exchange. We would therefore like to point out that our original study has now been considered favorably by four separate referees chosen by Nature Physics. Unfortunately, Wernsdorfer subsequently posted two further variations of his correspondence on this archive (arXiv:0804.1246v1 and arXiv:0804.1246v2). We note that aspects of the most recent posting (dated after submission of our response) contradict the version submitted to Nature Physics. However, none of the revisions add weight to Wernsdorfers original correspondence.
We report observation of coherent quantum oscilations in spin-10 Fe8 molecular clusters. The powder of magnetically oriented Fe8 crystallites was placed inside a resonator, in a dc magnetic field perpendicular to the magnetization axis. The field dependence of the ac-susceptibility was measured up to 5 T, at 680 MHz, down to 25 mK. Two peaks in the imaginary part of the susceptibility have been detected, whose positions coincide, without any fitting parameters, with the predicted two peaks corresponding to the quantum splitting of the ground state in the magnetic field parallel and perpendicular to the hard magnetization axis.
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