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Register a new userResonant Tunneling in Truly Axial Symmetry Mn12 Single-Molecule Magnets: Sharp Crossover between Thermally Assisted and Pure Quantum Tunneling
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Added by
Wolfgang Wernsdorfer
Publication date
2005
fields
Physics
and research's language is
English
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Magnetization measurements of a truly axial symmetry Mn12-tBuAc molecular nanomagnet with a spin ground state of S = 10 show resonance tunneling. This compound has the same magnetic anisotropy as Mn12-Ac but the molecules are better isolated and the crystals have less disorder and a higher symmetry. Hysteresis loop measurements at several temperatures reveal a well-resolved step fine-structure which is due to level crossings of excited states. All step positions can be modeled by a simple spin Hamiltonian. The crossover between thermally assisted and pure quantum tunneling can be investigated with unprecedented detail.
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We present a detailed study of the influence of various interactions on the spin quantum tunneling in a Mn12 wheel molecule. The effects of single-ion and exchange (spin-orbit) anisotropy are first considered, followed by an analysis of the roles played by secondary influences, e.g. disorder, dipolar and hyperfine fields, and magnetoacoustic interactions. Special attention is paid to the role of the antisymmetric Dzyaloshinski-Moriya (DM) interaction. This is done within the framework of a 12-spin microscopic model, and also using simplified dimer and tetramer approximations in which the electronic spins are grouped in 2 or 4 blocks, respectively. If the molecule is inversion symmetric, the DM interaction between the dimer halves must be zero. In an inversion symmetric tetramer, two independent DM vectors are allowed, but no new tunneling transitions are generated by the DM interaction. Experiments on the Mn12 wheel can only be explained if the molecular inversion symmetry is broken, and we explore this in detail using both models, focussing on the asymmetric disposition and rounding of Berry phase minima associated with quantum interference between states of opposite parity. A remarkable behavior exists for the `Berry phase zeroes as a function of the directions of the internal DM vectors and the external transverse field. A rather drastic breaking of the molecular inversion-symmetry is required to explain the experiments; in the tetramer model this requires a reorientation of the DM vectors on one half of the molecule by nearly 180 degrees. This cannot be attributed to sample disorder. These results are of general interest for the quantum dynamics of tunneling spins, and lead to some interesting experimental predictions.
The low temperature spin dynamics of a Fe8 Single-Molecule Magnet was studied under circularly polarized electromagnetic radiation allowing us to establish clearly photon-assisted tunneling. This effect, while linear at low power, becomes highly non-linear above a relatively low power threshold. This non-linearity is attributed to the nature of the coupling of the sample to the thermostat.These results are of great importance if such systems are to be used as quantum computers.
Based on the dielectric continuum model, we calculated the phonon assisted tunneling (PAT) current of general double barrier resonant tunneling structures (DBRTSs) including both symmetric and antisymmetric ones. The results indicate that the four higher frequency interface phonon modes (especially the one which peaks at either interface of the emitter barrier) dominate the PAT processes, which increase the valley current and decrease the PVR of the DBRTSs. We show that an asymmetric structure can lead to improved performance.
Single-molecule magnets facilitate the study of quantum tunneling of magnetization at the mesoscopic level. The spin-parity effect is among the fundamental predictions that have yet to be clearly observed. It is predicted that quantum tunneling is suppressed at zero transverse field if the total spin of the magnetic system is half-integer (Kramers degeneracy) but is allowed in integer spin systems. The Landau-Zener method is used to measure the tunnel splitting as a function of transverse field. Spin-parity dependent tunneling is established by comparing the transverse field dependence of the tunnel splitting of integer and half-integer spin systems.
Magnetization measurements of a molecular clusters Mn12 with a spin ground state of S = 10 show resonance tunneling at avoided energy level crossings. The observed oscillations of the tunnel probability as a function of the magnetic field applied along the hard anisotropy axis are due to topological quantum phase interference of two tunnel paths of opposite windings. Mn12 is therefore the second molecular clusters presenting quantum phase interference.
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