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Register a new userResonant Spin Tunneling in Randomly Oriented Nanospheres of Mn$_{12}$ Acetate
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We report measurements and theoretical analysis of resonant spin tunneling in randomly oriented nanospheres of a molecular magnet. Amorphous nanospheres of Mn$_{12}$ acetate have been fabricated and characterized by chemical, infrared, TEM, X-ray, and magnetic methods. Magnetic measurements have revealed sharp tunneling peaks in the field derivative of the magnetization that occur at the typical resonant field values for Mn$_{12}$ acetate. Theoretical analysis is provided that explains these observations. We argue that resonant spin tunneling in a molecular magnet can be established in a powder sample, without the need for a single crystal and without aligning the easy magnetization axes of the molecules. This is confirmed by re-analyzing the old data on a powdered sample of non-oriented micron-size crystals of Mn$_{12}$ acetate. Our findings can greatly simplify the selection of candidates for quantum spin tunneling among newly synthesized molecular magnets.
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We report synthesis, structural characterization, and magnetic measurements of amorphous Mn$_{12}$-acetate ribbons with a triclinic short-range crystal order not previously seen in experiment. The ribbons exhibit the same structure of Mn$_{12}$ molecules and the same positions of tunneling resonances on the magnetic field as a conventional tetragonal Mn$_{12}$-acetate crystal. However, the width of the zero-field resonance is by at least one order of magnitude smaller, indicating very small inhomoge- neous broadening due to dipolar and nuclear fields. Possible origins of this effect are discussed.
In magnetic fields applied parallel to the anisotropy axis, the magnetization of Mn$_{12}$ has been measured in response to a field that is swept back and forth across the resonances corresponding to steps $N=4,5,...9$. The fraction of molecules remaining in the metastable well after each sweep through the resonance is inconsistent with expectations for an ensemble of identical molecules. The data are consistent instead with the presence of a broad distribution of tunnel splittings. A very good fit is obtained for a Gaussian distribution of the second-order anisotropy tunneling parameter $X_E=-ln(mid Emid/2D)$. We show that dipolar shuffling is a negligible effect which cannot explain our data.
Local time-resolved measurements of fast reversal of the magnetization of single crystals of Mn12-acetate indicate that the magnetization avalanche spreads as a narrow interface that propagates through the crystal at a constant velocity that is roughly two orders of magnitude smaller than the speed of sound. We argue that this phenomenon is closely analogous to the propagation of a flame front (deflagration) through a flammable chemical substance.
We report measurements of the magnetic susceptibility of single crystals of Mn$_{12}$-acetate-MeOH, a new high-symmetry variant of the original single molecule magnet Mn$_{12}$-acetate. A comparison of these data to theory and to data for the Mn$_{12}$ acetate material shows that Mn$_{12}$-acetate-MeOH is a realization of a transverse-field Ising ferromagnet in contrast to the original Mn$_{12}$ acetate material, in which solvent disorder leads to effects attributed to random field Ising ferromagnetism.
In magnetic fields applied parallel to the anisotropy axis, the relaxation of the magnetization of Mn$_{12}$ measured for different sweep rates is shown to collapse onto a single scaled curve. The form of the scaling implies that the dominant symmetry-breaking process that gives rise to tunneling is a locally varying second-order anisotropy, forbidden by tetragonal symmetry in the perfect crystal, which gives rise to a broad distribution of tunnel splittings in a real crystal of Mn$_{12}$-acetate. Different forms applied to even and odd-numbered steps provide a distinction between even step resonances (associated with crystal anisotropy) and odd resonances (which require a transverse component of magnetic field).
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