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Register a new userOrigins of anomalously low Raman exponents in single-molecule magnets
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The Raman exponent of single-molecular magnetic relaxation may take various unexpected values because of rich phonon spectrum and spin-phonon coupling of molecular crystals. We systematically examine the origins of different abnormalities, and clarify misunderstandings in the past, particularly the appropriateness of the fitting procedures for the exponents. We find that exponential laws raised by optical phonons can yield spurious power laws with low exponents. This observation indicates long-standing misunderstandings for origins of low Raman exponents in a large bulk of single-molecule magnets. Resulting from spin-lattice coupling with optical modes, presence of these exponents suggests the importance of the local dynamical environment for the magnetic relaxation in this regime.
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Direct evidence of quantum coherence in a single-molecule magnet in frozen solution is reported with coherence times as long as T2 = 630 ns. We can strongly increase the coherence time by modifying the matrix in which the single-molecule magnets are embedded. The electron spins are coupled to the proton nuclear spins of both the molecule itself and interestingly, also to those of the solvent. The clear observation of Rabi oscillations indicates that we can manipulate the spin coherently, an essential prerequisite for performing quantum computations.
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.
We model magnetization processes that take place through tunneling in crystals of single-molecule magnets, such as Mn_12 and Fe_8. These processes take place when a field H is applied after quenching to very low temperatures. Magnetic dipolar interactions and spin flipping rules are essential ingredients of the model. The results obtained follow from Monte Carlo simulations and from the stochastic model we propose for dipole field diffusion. Correlations established before quenching are shown to later drive the magnetization process. We also show that in simple cubic lattices, m propto sqrt(t) at time t after H is applied, as observed in Fe_8, but only for 1+2log_10(h_d/h_w) time decades, where h_d is some near-neighbor magnetic dipolar field and a spin reversal can occur only if the magnetic field acting on it is within some field window (-h_w,h_w). However, the sqrt(t) behavior is not universal. For BCC and FCC lattices, m propto t^p, but p simeq 0.7 . An expression for p in terms of lattice parameters is derived. At later times the magnetization levels off to a constant value. All these processes take place at approximately constant magnetic energy if the annealing energy epsilon_a is larger than the tunneling windows energy width (i.e., if epsilon_a gtrsim gmu_B h_w S). Thermal processes come in only later on to drive further magnetization growth.
We show that correlations established before quenching to very low temperatures, later drive the magnetization process of systems of single molecule magnets, after a magnetic field is applied at t=0. We also show that in SC lattices, m propto sqrt(t), as observed in Fe_8, but only for 1+2*log_10(h_d/h_w) time decades, where h_d is a nearest neighbor dipolar magnetic field and a spin reversal can occur only if the field on it is within (-h_w,h_w). However, the sqrt(t) behavior is not universal. For BCC and FCC lattices, m propto t^p, but p simeq 0.7. The value to which m finally levels off is also given.
Lanthanide-based single-ion magnetic molecules can have large magnetic hyperfine interactions as well as large magnetic anisotropy. Recent experimental studies reported tunability of these properties by changes of chemical environments or by application of external stimuli for device applications. In order to provide insight onto the origin and mechanism of such tunability, here we investigate the magnetic hyperfine and nuclear quadrupole interactions for $^{159}$Tb nucleus in TbPc$_2$ (Pc=phthalocyanine) single-molecule magnets using multireference ab-initio methods including spin-orbit interaction. Since the electronic ground and first-excited (quasi)doublets are well separated in energy, the microscopic Hamiltonian can be mapped onto an effective Hamiltonian with an electronic pseudo-spin $S=1/2$. From the ab-initio-calculated parameters, we find that the magnetic hyperfine coupling is dominated by the interaction of the Tb nuclear spin with electronic orbital angular momentum. The asymmetric $4f$-like electronic charge distribution leads to a strong nuclear quadrupole interaction with significant non-axial terms for the molecule with low symmetry. The ab-initio calculated electronic-nuclear spectrum including the magnetic hyperfine and quadrupole interactions is in excellent agreement with experiment. We further find that the non-axial quadrupole interactions significantly influence the avoided level crossings in magnetization dynamics and that the molecular distortions affect mostly the Fermi contact terms as well as the non-axial quadrupole interactions.
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