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The quantum dynamics of atomic magnets, co-tunneling and dipolar-biased tunneling

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 Added by Romain Giraud
 Publication date 2003
  fields Physics
and research's language is English




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Multi-spins tunneling cross-relaxations in an ensemble of weakly-coupled Ho$^{3+}$ ions, mediated by weak anisotropic dipolar interactions, can be evidenced by ac-susceptibility measurements in a high temperature regime. Based on a four-body representation, including the rare-earth nuclear spin, two-ions tunneling mechanisms can be attributed to both dipolar-biased tunneling and co-tunneling processes. The co-reversal involving entangled pairs of magnetic moments is discussed with a particular emphasis, giving new evidences to elucidate the many-body quantum dynamics.



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We present a new family of exchange biased Single Molecule Magnets in which antiferromagnetic coupling between the two components results in quantum behaviour different from that of the individual SMMs. Our experimental observations and theoretical analysis suggest a means of tuning the quantum tunnelling of magnetization in SMMs. See also: W. Wernsdorfer, N. Aliaga-Alcalde, D. Hendrickson, G. Christou, Nature 416 (2002) 406.
Quantum tunneling dominates the low temperature magnetization dynamics in molecular magnets and presents features that are strongly system dependent. The current discussion is focused on the terbium(III) bis(phtalocyanine) ([TbPc$_2$]$^{-1}$) complex, that should serve as a prototypical case for lanthanide molecular magnets. We analyze numerically the effect of non-axial interactions on the magnitude of the intrinsic tunnel splitting and show that usual suspects like the transverse ligand field and Zeeman interaction fail to explain the experimentally observed dynamics. We then propose through the nuclear quadrupolar interaction a viable mechanism that mixes, otherwise textit{almost} degenerate hyperfine states.
It is shown that a single molecular magnet placed in a rapidly oscillating magnetic field displays the phenomenon of quenching of tunneling processes. The results open a way to manipulate the quantum states of molecular magnets by means of radiation in the terahertz range. Our analysis separates the time evolution into slow and fast components thereby obtaining an effective theory for the slow dynamics. This effective theory presents quenching of the tunnel effect. In particular, stands out its difference with the so-called coherent destruction of tunneling. We support our prediction with numerical evidence based on an exact solution of the Schrodingers equation.
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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.
The nuclear spin-mediated quantum relaxation of ensembles of tunneling magnetic molecules causes a hole to appear in the distribution of internal fields in the system. The form of this hole, and its time evolution, are studied using Monte Carlo simulations. It is shown that the line-shape of the tunneling hole in a weakly polarised sample must have a Lorentzian lineshape- the short-time half-width $xi_o$ in all experiments done so far should be $sim E_0$, the half-width of the nuclear spin multiplet. After a time $tau_o$, the single molecule tunneling relaxation time, the hole width begins to increase rapidly. In initially polarised samples the disintegration of resonant tunneling surfaces is found to be very fast.
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