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Register a new userSpin-spin cross-relaxation in single-molecule magnets
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Wernsdorfer Wolfgang
Publication date
2002
fields
Physics
and research's language is
English
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It is shown that dipolar and weak superexchange interactions between the spin systems of single-molecule magnets (SMM) play an important role in the relaxation of magnetization. These interactions can reduce or increase resonant tunneling. The one-body tunnel picture of SMMs is not always sufficient to explain the measured tunnel transitions. We propose to improve the picture by including also two-body tunnel transitions such as spin-spin cross-relaxation (SSCR). A Mn4 SMM is used as a model system to study the SSCR which plays also an important role for other SMMs like Mn12 or Fe8. At certain external fields, SSCRs can lead to quantum resonances which can show up in hysteresis loop measurements as well defined steps. A simple model allows us to explain quantitatively all observed transitions. Including three-body transitions or dealing with the many-body problem is beyond the slope of this paper.
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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.
We investigate theoretically the effects of intrinsic spin-relaxation on the spin-dependent transport through a single-molecule magnet (SMM), which is weakly coupled to ferromagnetic leads. The tunnel magnetoresistance (TMR) is obtained by means of the rate-equation approach including not only the sequential but also the cotunneling processes. It is shown that the TMR is strongly suppressed by the fast spin-relaxation in the sequential region and can vary from a large positive to slight negative value in the cotunneling region. Moreover, with an external magnetic field along the easy-axis of SMM, a large negative TMR is found when the relaxation strength increases. Finally, in the high bias voltage limit the TMR for the negative bias is slightly larger than its characteristic value of the sequential region, however it can become negative for the positive bias caused by the fast spin-relaxation.
Magnetization, AC susceptibility and $mu$SR measurements have been performed in neutral phthalocyaninato lanthanide ([LnPc$_2]^0$) single molecule magnets in order to determine the low-energy levels structure and to compare the low-frequency spin excitations probed by means of macroscopic techniques, such as AC susceptibility, with the ones explored by means of techniques of microscopic character, such as $mu$SR. Both techniques show a high temperature thermally activated regime for the spin dynamics and a low temperature tunneling one. While in the activated regime the correlation times for the spin fluctuations estimated by AC susceptibility and $mu$SR basically agree, clear discrepancies are found in the tunneling regime. In particular, $mu$SR probes a faster dynamics with respect to AC susceptibility. It is argued that the tunneling dynamics probed by $mu$SR involves fluctuations which do not yield a net change in the macroscopic magnetization probed by AC susceptibiliy. Finally resistivity measurements in [TbPc$_2]^0$ crystals show a high temperature nearly metallic behaviour and a low temperature activated behaviour.
A new family of supramolecular, antiferromagnetically exchange-coupled dimers of single-molecule magnets (SMMs) has recently been reported [W. Wernsdorfer, N. Aliaga-Alcalde, D.N. Hendrickson, and G. Christou, Nature 416, 406 (2002)]. Each SMM acts as a bias on its neighbor, shifting the quantum tunneling resonances of the individual SMMs. Hysteresis loop measurements on a single crystal of SMM-dimers have now established quantum tunneling of the magnetization via entangled states of the dimer. This shows that the dimer really does behave as a quantum-mechanically coupled dimer. The transitions are well separated, suggesting long coherence times compared to the time scale of the energy splitting. This result is of great importance if such systems are to be used for quantum computing. It also allows the measurement of the longitudinal and transverse superexchange coupling constants.
Four discrete MnIII/MnII tetra-nuclear complexes with double-cuboidal core were synthesized. dc magnetic measurements show that both Mn2+ - Mn3+ and Mn3+ - Mn3+ magnetic interactions are ferromagnetic in three samples leading to an S = 9 ground state for the Mn4 unit. Furthermore, these complexes are Single-Molecule Magnets (SMMs) clearly showing both thermally activated and ground state tunneling regimes. Slight changes in the [Mn4] core geometry result in an S = 1 ground state in fourth sample. A one-dimensional assembly of [Mn4] units was obtained in the same synthetic conditions with the subsequent addition of NaN3. Double chair-like N3- bridges connect identical [Mn4] units into a chain arrangement. This material behaves as an Ising assembly of S = 9 tetramers weakly antiferromagnetically coupled. Slow relaxation of the magnetization is observed at low temperature for the first time in an antiferromagnetic chain, following an activated behavior with 47 K and tau_0 = 7x10^-11 s. The observation of this original thermally activated relaxation process is induced by finite-size effects and in particular by the non-compensation of spins in segments of odd-number units. Generalizing the known theories on the dynamic properties of poly-disperse finite segments of antiferromagnetically coupled Ising spins, the theoretical expression of the characteristic energy gaps were estimated and successfully compared to the experimental values.
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