Harmonic oscillator wave functions of a self-assembled InAs quantum dot measured by scanning tunneling microscopy.

InAs quantum dots embedded in an AlAs matrix inside a double barrier resonant tunneling diode are investigated by cross-sectional scanning tunneling spectroscopy. The wave functions of the bound quantum dot states are spatially and energetically resolved. These bound states are known to be responsible for resonant tunneling phenomena in such quantum dot diodes. The wave functions reveal a textbook-like one-dimensional harmonic oscillator behavior showing up to five equidistant energy levels of 80 meV spacing. The derived effective oscillator mass of m* = 0.24m0 is 1 order of magnitude higher than the effective electron mass of bulk InAs that we attribute to the influence of the surrounding AlAs matrix. This underlines the importance of the matrix material for tailored QD devices with well-defined properties.

Controlling electronic access to the spin excitations of a single molecule in a tunnel junction.

Spintronic phenomena underpin new device paradigms for data storage and sensing. Scaling these down to the single molecule level requires controlling the properties of current-carrying molecular orbitals to enable access to spin states through phenomena such as inelastic electron tunnelling. Here we show that the spintronic properties of a tunnel junction containing a single molecule can be controlled using the local environment as a pseudo-gate. For tunnelling through iron phthalocyanine (FePc) on an insulating copper nitride (Cu2N) monolayer above Cu(001), we find that spin transitions may be strongly excited depending on the binding site of the central Fe atom. Different interactions between the Fe and the underlying Cu or N atoms shift the Fe d orbitals with respect to the Fermi energy and control the relative strength of the spin excitations; this effect is captured in a simple co-tunnelling model. This work demonstrates the importance of the atomic-scale environment for the development of single molecule spintronic devices.

Sub-molecular modulation of a 4f driven Kondo resonance by surface-induced asymmetry.

Coupling between a magnetic impurity and an external bath can give rise to many-body quantum phenomena, including Kondo and Hund's impurity states in metals, and Yu-Shiba-Rusinov states in superconductors. While advances have been made in probing the magnetic properties of d-shell impurities on surfaces, the confinement of f orbitals makes them difficult to access directly. Here we show that a 4f driven Kondo resonance can be modulated spatially by asymmetric coupling between a metallic surface and a molecule containing a 4f-like moment. Strong hybridization of dysprosium double-decker phthalocyanine with Cu(001) induces Kondo screening of the central magnetic moment. Misalignment between the symmetry axes of the molecule and the surface induces asymmetry in the molecule's electronic structure, spatially mediating electronic access to the magnetic moment through the Kondo resonance. This work demonstrates the important role that molecular ligands have in mediating electronic and magnetic coupling and in accessing many-body quantum states.

Tunable magnetoresistance in an asymmetrically coupled single-molecule junction.

Phenomena that are highly sensitive to magnetic fields can be exploited in sensors and non-volatile memories. The scaling of such phenomena down to the single-molecule level may enable novel spintronic devices. Here, we report magnetoresistance in a single-molecule junction arising from negative differential resistance that shifts in a magnetic field at a rate two orders of magnitude larger than Zeeman shifts. This sensitivity to the magnetic field produces two voltage-tunable forms of magnetoresistance, which can be selected via the applied bias. The negative differential resistance is caused by transient charging of an iron phthalocyanine (FePc) molecule on a single layer of copper nitride (Cu2N) on a Cu(001) surface, and occurs at voltages corresponding to the alignment of sharp resonances in the filled and empty molecular states with the Cu(001) Fermi energy. An asymmetric voltage-divider effect enhances the apparent voltage shift of the negative differential resistance with magnetic field, which inherently is on the scale of the Zeeman energy. These results illustrate the impact that asymmetric coupling to metallic electrodes can have on transport through molecules, and highlight how this coupling can be used to develop molecular spintronic applications.

Interplay between the Kondo effect and the Ruderman-Kittel-Kasuya-Yosida interaction.

The interplay between the Ruderman-Kittel-Kasuya-Yosida interaction and the Kondo effect is expected to provide the driving force for the emergence of many phenomena in strongly correlated electron materials. Two magnetic impurities in a metal are the smallest possible system containing all these ingredients and define a bottom-up approach towards a long-term understanding of concentrated/dense systems. Here we report on the experimental and theoretical investigation of iron dimers buried below a Cu(100) surface by means of low-temperature scanning tunnelling spectroscopy combined with density functional theory and numerical renormalization group calculations. The Kondo effect, in particular the width of the Abrikosov-Suhl resonance, is strongly altered or even suppressed due to magnetic coupling between the impurities. It oscillates as a function of dimer separation revealing that it is related to indirect exchange interactions mediated by the conduction electrons.