This perspectives article takes a broad view of the current understanding of magnetic bistability and magnetic quantum tunneling in single-molecule magnets (SMMs), focusing on three families of relatively simple, low-nuclearity transition metal clusters: spin S = 4 II 4 Ni , III 3 Mn (S = 2 and 6) and III 6 Mn (S = 4 and 12). The Mn III complexes are related by the fact that they contain triangular III 3 Mn units in which the exchange may be switched from antiferromagnetic to ferromagnetic without significantly altering the coordination around the Mn III centers, thereby leaving the single-ion physics more-or-less unaltered. This allows for a detailed and systematic study of the way in which the individual-ion anisotropies project onto the molecular spin ground state in otherwise identical low-and high-spin molecules, thus providing unique insights into the key factors that control the quantum dynamics of SMMs, namely: (i) the height of the kinetic barrier to magnetization relaxation; and (ii) the transverse interactions that cause tunneling through this barrier. Numerical calculations are supported by an unprecedented experimental data set (17 different compounds), including very detailed spectroscopic information obtained from high-frequency electron paramagnetic resonance and low-temperature hysteresis measurements. Comparisons are made between the giant spin and multi-spin phenomenologies. The giant spin approach assumes the ground state spin, S, to be exact, enabling implementation of simple anisotropy projection techniques. This methodology provides a basic understanding of the concept of anisotropy dilution whereby the cluster anisotropy decreases as the total spin increases, resulting in a barrier that depends weakly on S. This partly explains why the record barrier for a SMM (86 K for Mn 6 ) has barely increased in the 15 years since the first studies of Mn 12 -acetate, and why the tiny Mn 3 molecule can have a barrier approaching 60% of this record. Ultimately, the giant spin approach fails to capture all of the key physics, although it works remarkably well for the purely ferromagnetic cases. Nevertheless, diagonalization of the multi-spin Hamiltonian matrix is necessary in order to fully capture the interplay between exchange and local anisotropy, and the resultant spin-state mixing which ultimately gives rise to the tunneling matrix elements in the high symmetry SMMs (ferromagnetic Mn 3 and Ni 4 ). The simplicity (low-nuclearity, high-symmetry, weak disorder, etc..) of the molecules highlighted in this study proves to be of crucial importance. Not only that, these simple molecules may be considered among the best SMMs: Mn 6 possesses the record anisotropy barrier, and Mn 3 is the first SMM to exhibit quantum tunneling selection rules that reflect the intrinsic symmetry of the molecule.
Engineering the interaction between light and matter is an important goal in the emerging field of quantum opto-electronics. Thanks to the use of cavity quantum electrodynamics architectures, one can envision a fully hybrid multiplexing of quantum conductors. Here we use such an architecture to couple two quantum dot circuits. Our quantum dots are separated by 200 times their own size, with no direct tunnel and electrostatic couplings between them. We demonstrate their interaction, mediated by the cavity photons. This could be used to scale up quantum bit architectures based on quantum dot circuits or simulate on-chip phonon-mediated interactions between strongly correlated electrons.
The synthesis and characterisation of a large family of hexametallic [Mn(III)(6)] Single-Molecule Magnets of general formula [Mn(III)(6)O(2)(R-sao)(6)(X)(2)(sol)(4-6)] (where R = H, Me, Et; X = (-)O(2)CR' (R' = H, Me, Ph etc) or Hal(-); sol = EtOH, MeOH and/or H(2)O) are presented. We show how deliberate structural distortions of the [Mn(3)O] trinuclear moieties within the [Mn(6)] complexes are used to tune their magnetic properties. These findings highlight a qualitative magneto-structural correlation whereby the type (anti- or ferromagnetic) of each Mn(2) pairwise magnetic exchange is dominated by the magnitude of each individual Mn-N-O-Mn torsion angle. The observation of magneto-structural correlations on such large polymetallic complexes is rare and represents one of the largest studies of this kind.
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