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Register a new userTuning of the magnetic properties of the high spin molecular cluster Fe8
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The synthesis, crystal structure and magnetic characterization of a high spin cluster comprising eight iron ions, are presented in this contribution. The cluster has formula [(tacn)6Fe8O2(OH)12Br4.3(ClO4)3.7]6H2O, (Fe8PCL) where tacn is the organic ligand 1,4,7-triazacyclononane. It can be considered a derivative of Fe8Br8, a cluster whose low temperature dynamics of the magnetization has been deeply investigated, where four of the bromide ions have been replaced by perchlorate anions. The structure of the central core of the two molecules, [Fe8O(OH)12(tacn)6]8+, is essentially the same, but Fe8PCL has a higher symmetry (Fe8Br8 crystallizes in the acentric P1 space group, while Fe8PCL crystallizes in the P21/c space group, monoclinic). The magnetic properties of Fe8PCL suggest it is very similar to Fe8Br having a S=10 ground state as well. The zero field splitting parameters were accurately determined by HF-EPR measurements. The two clusters have similar axial anisotropy but Fe8PCL has a larger transverse anisotropy. Ac susceptibility measurements revealed the cluster behaves like a superparamagnetic particle. However, due to the occurrence of large terms in the transverse anisotropy, the temperature dependence of the relaxation time can not be reproduced by a simple Arrhenius law. As observed in Fe8Br8, below 350 mK the relaxation time becomes temperature independent, indicating that a pure tunneling regime is attained. The comparison of the tunneling rate in the two clusters shows that in the perchlorate derivative the relaxation process is 35 times faster. The observed ratio of the tunneling rates is in reasonable agreement with that calculated from the tunneling splitting, i.e. the energy difference between the two almost degenerate lowest levels Ms = +/-10, in the two clusters.
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We report measurements on magnetization reversal in the Fe$_8$ molecular magnet using fast pulsed magnetic fields of 1.5 kT/s and in the temperature range of 0.6-4.1 K. We observe and analyze the temperature dependence of the reversal process, which involves in some cases several resonances. Our experiments allow observation of resonant quantum tunneling of magnetization up to a temperature of $sim$ 4 K. We also observe shifts of the resonance fields in temperature that suggest the emergence of a thermal instability---a combination of spin reversal and self-heating that may result in a magnetic deflagration process. The results are mainly understood in the framework of thermally-activated quantum tunneling transitions in combination with emergence of a thermal instability.
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%.
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.
Antiferromagnetic spin rings represent prototypical realizations of highly correlated, low-dimensional systems. Here we theoretically show how the introduction of magnetic defects by controlled chemical substitutions results in a strong spatial modulation of spin-pair entanglement within each ring. Entanglement between local degrees of freedom (individual spins) and collective ones (total ring spins) are shown to coexist in exchange-coupled ring dimers, as can be deduced from general symmetry arguments. We verify the persistence of these features at finite temperatures, and discuss them in terms of experimentally accessible observables.
We show that CdMnTe self-assembled quantum dots can be formed by depositing a submonolayer of Mn ions over a ZnTe surface prior to deposition of the CdTe dot layer. Single dot emission lines and strongly polarized quantum dot photoluminescence in an applied magnetic field confirm the presence of Mn in individual quantum dots. The width of PL lines of the single CdMnTe dots is 3 meV due to magnetic moment fluctuations of the Mn ions. After rapid thermal annealing, the emission lines of individual magnetic quantum dots narrow significantly to 0.25 meV showing that effect of magnetic fluctuations is strongly reduced most probably due to an increase in the average quantum dot size. These results suggest a way to tune the spin properties of magnetic quantum dots.
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