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Single molecule magnets and single spin centres can be individually addressed when coupled to contacts forming an electrical junction. To control and engineer the magnetism of quantum devices, it is necessary to quantify how the structural and chemical environment of the junction affects the spin centre. Metrics such as coordination number or symmetry provide a simple method to quantify the local environment, but neglect the many-body interactions of an impurity spin coupled to contacts. Here, we utilize a highly corrugated hexagonal boron nitride monolayer to mediate the coupling between a cobalt spin in CoH x ( x =1,2) complexes and the metal contact. While hydrogen controls the total effective spin, the corrugation smoothly tunes the Kondo exchange interaction between the spin and the underlying metal. Using scanning tunnelling microscopy and spectroscopy together with numerical simulations, we quantitatively demonstrate how the Kondo exchange interaction mimics chemical tailoring and changes the magnetic anisotropy. The spins of single molecules and defect centres possess properties which can be strongly influenced by their material contacts in electrical junctions. Here, the authors study the coupling between cobalt hydride complexes and a Rh(111) contact, mediated through a hexagonal boron nitride layer.

Spin–spin correlations can be the driving force that favours certain ground states and are key in numerous models that describe the behaviour of strongly correlated materials. While the sum of collective correlations usually lead to a macroscopically measurable change in properties, a direct quantification of correlations in atomic scale systems is difficult. Here we determine the correlations between a strongly hybridized spin impurity on the tip of a scanning tunnelling microscope and its electron bath by varying the coupling to a second spin impurity weakly hybridized to the sample surface. Electronic transport through these coupled spins reveals an asymmetry in the differential conductance reminiscent of spin-polarized transport in a magnetic field. We show that at zero field, this asymmetry can be controlled by the coupling strength and is related to either ferromagnetic or antiferromagnetic spin–spin correlations in the tip. Spin-spin correlation is fundamental to many material properties but challenging to measure in nanomagnetic systems. Muenks et al . show that correlations between a localized spin and the electrons of its hosting bath can be quantified when coupled to another spin by an asymmetry in the differential conductance.

Combined scanning tunnelling and atomic force microscopy using a qPlus sensor enables the measurement of electronic and mechanic properties of two-dimensional materials at the nanoscale. In this work, we study hexagonal boron nitride ( h -BN), an atomically thin 2D layer, that is van der Waals-coupled to a Cu(111) surface. The system is of interest as a decoupling layer for functional 2D heterostructures due to the preservation of the h -BN bandgap and as a template for atomic and molecular adsorbates owing to its local electronic trapping potential due to the in-plane electric field. We obtain work function (Φ) variations on the h -BN/Cu(111) superstructure of the order of 100 meV using two independent methods, namely the shift of field emission resonances and the contact potential difference measured by Kelvin probe force microscopy. Using 3D force profiles of the same area we determine the relative stiffness of the Moiré region allowing us to analyse both electronic and mechanical properties of the 2D layer simultaneously. We obtain a sheet stiffness of 9.4 ± 0.9 N·m −1 , which is one order of magnitude higher than the one obtained for h -BN/Rh(111). Using constant force maps we are able to derive height profiles of h -BN/Cu(111) showing that the system has a corrugation of 0.6 ± 0.2 Å, which helps to demystify the discussion around the flatness of the h -BN/Cu(111) substrate.

Topological Insulators have been a major focus in condensed-matter physics over the past six years. It was realized that the spin polarized surface states of topological insulators can lead to novel applications in spintronics or even in quantum computing. The exciting physics includes the famous Majorana fermion, believed to arise when a topological insulator is brought in close proximity to a s-wave superconductor, resulting in an artificial p-wave like superconductor. This thesis contributes to this ongoing research by describing the underlying theory and investigating the necessary steps to create a successful interface between a topological insulator and a s-wave superconductor, thus laying the groundwork for probing the proximity effect in these interfaces with Scanning Tunneling Spectroscopy. Nb, Pb and PbBi structures were investigated and a suitable geometry, that was grown with a shadow mask, is presented.

Correlation is a fundamental statistical measure of order in interacting quantum systems. In solids, electron correlations govern a diverse array of material classes and phenomena such as heavy fermion compounds, Hunds metals, high-Tc superconductors, and the Kondo effect. Spin-spin correlations, notably investigated by Kaufman and Onsager in the 1940s 6, are at the foundation of numerous theoretical models but are challenging to measure experimentally. Reciprocal space methods can map correlations, but at the single atom limit new experimental probes are needed. Here, we determine the correlations between a strongly hybridized spin impurity and its electron bath by varying the coupling to a second magnetic impurity in the junction of a scanning tunneling microscope. Electronic transport through these coupled spins reveals an asymmetry in the differential conductance reminiscent of spin-polarized transport in a magnetic field. We show that at zero field, this asymmetry can be controlled by the coupling strength and is directly related to either ferromagnetic (FM) or antiferromagnetic (AFM) spin-spin correlations.

Single molecule magnets and single spin centers can be individually addressed when coupled to contacts forming an electrical junction. In order to control and engineer the magnetism of quantum devices, it is necessary to quantify how the structural and chemical environment of the junction affects the spin center. Metrics such as coordination number or symmetry provide a simple method to quantify the local environment, but neglect the many-body interactions of an impurity spin when coupled to contacts. Here, we utilize a highly corrugated hexagonal boron nitride (h-BN) monolayer to mediate the coupling between a cobalt spin in CoHx (x=1,2) complexes and the metal contact. While the hydrogen atoms control the total effective spin, the corrugation is found to smoothly tune the Kondo exchange interaction between the spin and the underlying metal. Using scanning tunneling microscopy and spectroscopy together with numerical simulations, we quantitatively demonstrate how the Kondo exchange interaction mimics chemical tailoring and changes the magnetic anisotropy.

Spin-bearing molecules can be stabilized on surfaces and in junctions with desirable properties such as a net spin that can be adjusted by external stimuli. Using scanning probes, initial and final spin states can be deduced from topographic or spectroscopic data, but how the system transitioned between these states is largely unknown. Here we address this question by manipulating the total spin of magnetic cobalt hydride complexes on a corrugated boron nitride surface with a hydrogen- functionalized scanning probe tip by simultaneously tracking force and conductance. When the additional hydrogen ligand is brought close to the cobalt monohydride, switching between a corre- lated S = 1 /2 Kondo state, where host electrons screen the magnetic moment, and a S = 1 state with magnetocrystalline anisotropy is observed. We show that the total spin changes when the system is transferred onto a new potential energy surface defined by the position of the hydrogen in the junction. These results show how and why chemically functionalized tips are an effective tool to manipulate adatoms and molecules, and a promising new method to selectively tune spin systems.