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Register a new userTunneling and inversion symmetry in single-molecule magnets: the case of the Mn12 wheel molecule
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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.
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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.
The magnetic properties of a monolayer of Mn12 single molecule magnets grafted onto a Si substrate have been investigated using depth-controlled $beta$-detected nuclear magnetic resonance. A low energy beam of spin polarized radioactive 8Li was used to probe the local static magnetic field distribution near the Mn12 monolayer in the Si substrate. The resonance linewidth varies strongly as a function of implantation depth as a result of the magnetic dipolar fields generated by the Mn12 electronic magnetic moments. The temperature dependence of the linewidth indicates that the magnetic properties of the Mn12 moments in this low dimensional configuration differ from bulk Mn12.
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.
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.
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