M. R. Wegewijs

Electron transport through single Mn12 molecular magnets

We report transport measurements through a single-molecule magnet, the Mn12 derivative [Mn12O12(O2C-C6H4-SAc)16(H2O)4], in a single-molecule transistor geometry. Thiol groups connect the molecule to gold electrodes that are fabricated by electromigration. Striking observations are regions of complete current suppression and excitations of negative differential conductance on the energy scale of the anisotropy barrier of the molecule. Transport calculations, taking into account the high-spin ground state and magnetic excitations of the molecule, reveal a blocking mechanism of the current involving nondegenerate spin multiplets.

Electron Transport through SingleMn12Molecular Magnets

We report transport measurements through a single-molecule magnet, the Mn12 derivative [Mn12O12(O2C-C6H4-SAc)16(H2O)4], in a single-molecule transistor geometry. Thiol groups connect the molecule to gold electrodes that are fabricated by electromigration. Striking observations are regions of complete current suppression and excitations of negative differential conductance on the energy scale of the anisotropy barrier of the molecule. Transport calculations, taking into account the high-spin ground state and magnetic excitations of the molecule, reveal a blocking mechanism of the current involving nondegenerate spin multiplets.

Electric Field Controlled Magnetic Anisotropy in a Single Molecule

We have measured quantum transport through an individual Fe(4) single-molecule magnet embedded in a three-terminal device geometry. The characteristic zero-field splittings of adjacent charge states and their magnetic field evolution are observed in inelastic tunneling spectroscopy. We demonstrate that the molecule retains its magnetic properties and, moreover, that the magnetic anisotropy is significantly enhanced by reversible electron addition/subtraction controlled with the gate voltage. Single-molecule magnetism can thus be electrically controlled.

Quantum-tunneling-induced Kondo effect in single molecular magnets.

We consider transport through a single-molecule magnet strongly coupled to metallic electrodes. We demonstrate that, for a half-integer spin of the molecule, electron and spin tunneling cooperate to produce both quantum tunneling of the magnetic moment and a Kondo effect in the linear conductance. The Kondo temperature depends sensitively on the ratio of the transverse and easy-axis anisotropies in a nonmonotonic way. The magnetic symmetry of the transverse anisotropy imposes a selection rule on the total spin for the occurrence of the Kondo effect which deviates from the usual even-odd alternation.

Kondo-transport spectroscopy of single molecule magnets.

We demonstrate that in a single molecule magnet strongly coupled to electrodes the Kondo effect involves all magnetic excitations. This Kondo effect is induced by the quantum tunneling of the magnetic moment. Importantly, the Kondo temperature TK can be much larger than the magnetic splittings. We find a strong modulation of the Kondo effect as a function of the transverse anisotropy parameter or a longitudinal magnetic field. Both for integer and half-integer spin this can be used for an accurate transport spectroscopy of the magnetic states in low magnetic fields on the order of the easy-axis anisotropy parameter. We set up a relationship between the Kondo effects for successive integer and half-integer spins.

Nonlinear thermoelectric properties of molecular junctions with vibrational coupling

We present a detailed study of the non-linear thermoelectric properties of a molecular junction, represented by a dissipative Anderson-Holstein model. A single orbital level with strong Coulomb interaction is coupled to a localized vibrational mode and we account for both electron and phonon exchange with both electrodes, investigating how these contribute to the heat and charge transport. We calculate the efficiency and power output of the device operated as a heat to electric power converter and identify the optimal operating conditions, which are found to be qualitatively changed by the presence of the vibrational mode. Based on this study of a generic model system, we discuss the desirable properties of molecular junctions for thermoelectric applications.

Spin Quantum Tunneling in Single Molecular Magnets: Fingerprints in Transport Spectroscopy of Current and Noise

We demonstrate that transport spectroscopy of single molecular magnets shows signatures of quantum tunneling at low temperatures. We find current and noise oscillations as a function of bias voltage due to a weak violation of spin-selection rules by quantum tunneling processes. The interplay with Boltzmann suppression factors leads to fake resonances with temperature-dependent position which do not correspond to any charge excitation energy. Furthermore, we find that quantum tunneling can completely suppress transport if the transverse anisotropy has a high symmetry.

Charge transport through single molecules, quantum dots and quantum wires

We review recent progress in the theoretical description of correlation and quantum fluctuation phenomena in charge transport through single molecules, quantum dots and quantum wires. Various physical phenomena are addressed, relating to cotunneling, pair-tunneling, adiabatic quantum pumping, charge and spin fluctuations, and inhomogeneous Luttinger liquids. We review theoretical many-body methods to treat correlation effects, quantum fluctuations, non-equilibrium physics, and the time evolution into the stationary state of complex nanoelectronic systems.

Spintronic magnetic anisotropy

Superparamagnetism (preferential alignment of spins along an easy axis) is a useful effect for spintronic applications as it prevents spin reversal. It is now shown that high-spin quantum dots can become magnetically anisotropic when coupled to nearby ferromagnets—‘artificial’ superparamagnets.

Pumping of Vibrational Excitations in the Coulomb-Blockade Regime in a Suspended Carbon Nanotube

Low-temperature transport spectroscopy measurements on a suspended few-hole carbon nanotube quantum dot are presented, showing a gate-dependent harmonic excitation spectrum which, strikingly, occurs in the Coulomb-blockade regime. The quantized excitation energy corresponds to the scale expected for longitudinal vibrations of the nanotube. The electronic transport processes are identified as cotunnel-assisted sequential tunneling, resulting from nonequilibrium occupation of the mechanical mode. They appear only above a high-bias threshold at the scale of electronic nanotube excitations. We discuss models for the pumping process that explain the enhancement of the nonequilibrium occupation and show that it is connected to a subtle interplay between electronic and vibrational degrees of freedom.