Controlling electronic transport through a single-molecule junction is crucial for molecular electronics or spintronics. In magnetic molecular devices, the spin degree-of-freedom can be used to this end since the magnetic properties of the magnetic ion centers fundamentally impact the transport through the molecules. Here we demonstrate that the electron pathway in a single-molecule device can be selected between two molecular orbitals by varying a magnetic field, giving rise to a tunable anisotropic magnetoresistance up to 93%. The unique tunability of the electron pathways is due to the magnetic reorientation of the transition metal center, resulting in a re-hybridization of molecular orbitals. We obtain the tunneling electron pathways by Kondo effect, which manifests either as a peak or a dip line shape. The energy changes of these spin-reorientations are remarkably low and less than one millielectronvolt. The large tunable anisotropic magnetoresistance could be used to control electronic transport in molecular spintronics.

We propose a protocol for the manipulation of a three-level artificial atom in Lambda ($\mathrm{\Lambda }$) configuration. It allows faithful, selective and robust population transfer analogous to stimulated Raman adiabatic passage ($\mathrm{\Lambda }$-STIRAP), in last-generation superconducting artificial atoms, where protection from noise implies the absence of a direct pump coupling. It combines the use of a two-photon pump pulse with suitable advanced control, operated by a slow modulation of the phase of the external fields, leveraging on the stability of semiclassical microwave drives. This protocol is a building block for manipulation of microwave photons in complex quantum architectures. Its demonstration would be a benchmark for the implementation of a class of multilevel advanced control procedures for quantum computation and microwave quantum photonics in systems based on artificial atoms.

We report an electrochemical gating approach with ∼100% efficiency to tune the conductance of single-molecule 4,4′-bipyridine junctions.

Electrical and mechanical properties of elongated gold-molecule-gold junctions formed by tolane-type molecules with different anchoring groups (pyridyl, thiol, amine, nitrile and dihydrobenzothiophene) were studied in current-sensing force spectroscopy experiments and density functional simulations. Correlations between forces, conductances and junction geometries demonstrate that aromatic tolanes bind between electrodes as single molecules or as weakly-conductive dimers held by mechanically-weak π − π stacking. In contrast with the other anchors that form only S-Au or N-Au bonds, the pyridyl ring also forms a highly-conductive cofacial link to the gold surface. Binding of multiple molecules creates junctions with higher conductances and mechanical strengths than the single-molecule ones.