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Register a new userThe role of the quadrupolar interaction in the tunneling dynamics of lanthanide molecular magnets
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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.
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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.
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.
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.
Reply to the Comment of J.J. Alonso and J.F. Fernandez on the paper Hole-digging in ensembles of tunneling molecular magnets of I.S. Tupitsyn, P.C.E. Stamp and N.V. Prokofev (Phys. Rev. B 69, 132406, (2004)).
Molecular electronic devices are the upmost destiny of the miniaturization trend of electronic components. Although not yet reproducible on large scale, molecular devices are since recently subject of intense studies both experimentally and theoretically, which agree in pointing out the extreme sensitivity of such devices on the nature and quality of the contacts. This chapter intends to provide a general theoretical framework for modelling electronic transport at the molecular scale by describing the implementation of a hybrid method based on Green function theory and density functional algorithms. In order to show the presence of contact-dependent features in the molecular conductance, we discuss three archetypal molecular devices, which are intended to focus on the importance of the different sub-parts of a molecular two-terminal setup.
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