Quantum interference oscillations of the superparamagnetic blocking in an Fe8 molecular nanomagnet

We show that the dynamic magnetic susceptibility and the superparamagnetic blocking temperature of an Fe8 single molecule magnet oscillate as a function of the magnetic field Hx applied along its hard magnetic axis. These oscillations are associated with quantum interferences, tuned by Hx, between different spin tunneling paths linking two excited magnetic states. The oscillation period is determined by the quantum mixing between the ground S=10 and excited multiplets. These experiments enable us to quantify such mixing. We find that the weight of excited multiplets in the magnetic ground state of Fe8 amounts to approximately 11.6%.Comment: Accepted in Phys. Rev. Let

Franck-Condon Blockade in a Single-Molecule Transistor

We investigate vibron-assisted electron transport in single-molecule transistors containing an individual Fe4 Single-Molecule Magnet. We observe a strong suppression of the tunneling current at low bias in combination with vibron-assisted excitations. The observed features are explained by a strong electron-vibron coupling in the framework of the Franck-Condon model supported by density-functional theory

Quantum Landauer erasure with a molecular nanomagnet

The erasure of a bit of information is an irreversible operation whose minimal entropy production of kB ln 2 is set by the Landauer limit1. This limit has been verified in a variety of classical systems, including particles in traps2, 3 and nanomagnets4. Here, we extend it to the quantum realm by using a crystal of molecular nanomagnets as a quantum spin memory and showing that its erasure is still governed by the Landauer principle. In contrast to classical systems, maximal energy efficiency is achieved while preserving fast operation owing to its high-speed spin dynamics. The performance of our spin register in terms of energy–time cost is orders of magnitude better than existing memory devices to date. The result shows that thermodynamics sets a limit on the energy cost of certain quantum operations and illustrates a way to enhance classical computations by using a quantum system

Probing Transverse Magnetic Anisotropy by Electronic Transport through a Single-Molecule Magnet

By means of electronic transport, we study the transverse magnetic anisotropy of an individual Fe$_4$ single-molecule magnet (SMM) embedded in a three-terminal junction. In particular, we determine in situ the transverse anisotropy of the molecule from the pronounced intensity modulations of the linear conductance, which are observed as a function of applied magnetic field. The proposed technique works at temperatures exceeding the energy scale of the tunnel splittings of the SMM. We deduce that the transverse anisotropy for a single Fe$_4$ molecule captured in a junction is substantially larger than the bulk value.Comment: 18 pages with 16 figures; version as publishe

Superconducting molybdenum-rhenium electrodes for single-molecule transport studies

We demonstrate that electronic transport through single molecules or molecular ensembles, commonly based on gold (Au) electrodes, can be extended to superconducting electrodes by combining gold with molybdenum-rhenium (MoRe). This combination induces proximity-effect superconductivity in the gold to temperatures of at least 4.6 Kelvin and magnetic fields of 6 Tesla, improving on previously reported aluminum based superconducting nanojunctions. As a proof of concept, we show three-terminal superconductive transport measurements through an individual Fe$_4$ single-molecule magnet.Comment: 4 pages, 3 figure

Magnetic dipolar ordering and quantum phase transition in Fe8 molecular magnet

We show that a crystal of mesoscopic Fe8 single molecule magnets is an experimental realization of the Quantum Ising Phase Transition (QIPT) model in a transverse field, with dipolar interactions. Quantum annealing has enabled us to explore the QIPT at thermodynamical equilibrium. The phase diagram and critical exponents we obtain are compared to expectations for the mean-field QIPT Universality class.Comment: 5 pages 4 figure

Exchange coupling inversion in a high-spin organic triradical molecule

The magnetic properties of a nanoscale system are inextricably linked to its local environment. In ad-atoms on surfaces and inorganic layered structures the exchange interactions result from the relative lattice positions, layer thicknesses and other environmental parameters. Here, we report on a sample-dependent sign inversion of the magnetic exchange coupling between the three unpaired spins of an organic triradical molecule embedded in a three-terminal device. This ferro-to-antiferromagnetic transition is due to structural distortions and results in a high-to-low spin ground state change in a molecule traditionally considered to be a robust high-spin quartet. Moreover, the flexibility of the molecule yields an in-situ electric tunability of the exchange coupling via the gate electrode. These findings open a route to the controlled reversal of the magnetic states in organic molecule-based nanodevices by mechanical means, electrical gating or chemical tailoring

Alignment Of Magnetic Anisotropy Axes In Crystals Of Mn12 Acetate And Mn12-tBuAc Molecular Nanomagnets: Angle-Dependent Ac Susceptibility Study

We report the results of angular-dependent ac susceptibility experiments performed on two derivatives of Mn12 single-molecular magnets: the well-known Mn12 acetate, which contains disordered acetic acid molecules in interstitial sites of the crystal structure and Mn12-tBuAc, for which solvent molecules are very well ordered in the structure. Our results show (a) that the angular variation is very similar in the two compounds investigated and compatible with a maximum misalignment of the anisotropy axes of less than 3° and (b) that the tunneling rate is faster for the better ordered Mn12-tBuAc compound. These experiments question interstitial disorder as the dominant origin of the thermally activated tunneling phenomenon

Crystal size dependence of dipolar ferromagnetic order between Mn6 molecular nanomagnets

We study how crystal size influences magnetic ordering in arrays of molecular nanomagnets coupled by dipolar interactions. Compressed fluid techniques have been applied to synthesize crystals of Mn6 molecules (spin S = 12) with sizes ranging from 28 µm down to 220 nm. The onset of ferromagnetic order and the spin thermalization rates have been studied by means of ac susceptibility measurements. We find that the ordered phase remains ferromagnetic, as in the bulk, but the critical temperature Tc decreases with crystal size. Simple magnetostatic energy calculations, supported by Monte Carlo simulations, account for the observed drop in Tc in terms of the minimum attainable energy for finite-sized magnetic domains limited by the crystal boundaries. Frequency-dependent susceptibility measurements give access to the spin dynamics. Although magnetic relaxation remains dominated by individual spin flips, the onset of magnetic order leads to very long spin thermalization time scales. The results show that size influences the magnetism of dipolar systems with as many as 1011 spins and are relevant for the interpretation of quantum simulations performed on finite lattices