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We present a method to fabricate insulated gold mechanically controlled break junctions (MCBJ) by coating the metal with a thin layer of aluminum oxide using plasma enhanced atomic layer deposition. The Al2O3 thickness deposited on the MCBJ devices was varied from 2 to 15nm to test the suppression of leakage currents in deionized water and phosphate buffered saline. Junctions coated with a 15 nm thick oxide layer yielded atomically sharp electrodes and negligible conductance counts in the range of 1 to 10-4 G0 (1 G0=77 μS), where single-molecule conductances are commonly observed. The insulated devices were used to measure the conductance of an amphiphilic oligophenylene ethynylene derivative in deionized water. [ABSTRACT FROM AUTHOR]

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 K and magnetic fields of 6 T, improving on previously reported aluminum based superconducting nanojunctions. As a proof of concept, we show three-terminal superconductive transport measurements through an individual Fe4 single-molecule magnet. [ABSTRACT FROM AUTHOR]

We have investigated charge transport in single-molecule junctions using gold nanoelectrodes at room and cryogenic (10 K) temperatures. A statistical analysis of the low-bias conductance, measured during the stretching of the molecular junctions, shows that the most probable single-molecule conductance is insensitive to the temperature as expected for off-resonant coherent transport. Low-temperature current-voltage measurements show that these junction conformations have a smooth tunnelinglike shape. While separating the electrodes further we find that, in about one-fourth of the cases, the junction switches in an abrupt way to a configuration with I-V characteristics exhibiting a gap around zero bias and resonances at finite bias. The analysis of the I-V shape and of the conductance distance dependence suggests a stretching-induced transition from the strong to the weak electronic coupling regime. The transition involves a large renormalization of the injection barrier and of the electronic coupling between the molecule and the electrodes. [ABSTRACT FROM AUTHOR]

Inspired by cotunneling spectroscopy of spin-states in a single OPE5-based molecule, we investigate the prospects for electric control of magnetism in purely organic molecules contacted in a three-terminal geometry. Using the gate electrode, the molecule is reversibly switched between three different redox states, with magnetic spectra revealing both ferromagnetic and antiferromagnetic exchange couplings on the molecule. These observations are shown to be captured by an effective low-energy Heisenberg model, which we substantiate microscopically by a simple valence bond description of the molecule. These preliminary findings suggest an interesting route towards functionalized all-organic molecular magnetism. [ABSTRACT FROM AUTHOR]

It is known that the quantum mechanical ground state of a nanoscale junction has a significant impact on its electrical transport properties. This becomes particularly important in transistors consisting of a single molecule. Because of strong electron-electron interactions and the possibility of accessing ground states with high spins, these systems are eligible hosts of a current-blockade phenomenon called a ground-state spin blockade. This effect arises from the inability of a charge carrier to account for the spin difference required to enter the junction, as that process would violate the spin selection rules. Here, we present a direct experimental demonstration of a ground-state spin blockade in a high-spin single-molecule transistor. The measured transport characteristics of this device exhibit a complete suppression of resonant transport due to a ground-state spin difference of 3/2 between subsequent charge states. Strikingly, the blockade can be reversibly lifted by driving the system through a magnetic ground-state transition in one charge state, using the tunability offered by both magnetic and electric fields. [ABSTRACT FROM AUTHOR]