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 CoHx (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.

A procedure is proposed to optimize a high-pass filter enabling one to subtract the broadband background signals inherent in Raman spectra. A spectral approach is used to analyze the characteristics of the filter and the distortions in the processed spectra. Examples of the processing of real spectra are presented.

Experimental investigations of spin-polarized electron confinement in nanostructures by scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) are reviewed. To appreciate the experimental results on the electronic level, the physical basis of STM is elucidated with special emphasis on the correlation between differential conductance, as measured by STS, and the electron density of states, which is accessible in ab initio theory. Experimental procedures which allow one to extract the electron dispersion relation from energy-dependent and spatially resolved STM and STS studies of electron confinement are reviewed. The role of spin polarization in electron confinement is highlighted by both experimental and theoretical insights, which indicate variation of the spin polarization in sign and magnitude on the nanometer scale. This review provides compelling evidence for the necessity to include spatial-dependent spin-resolved electronic properties for an in-depth understanding and quantitative assessment of electron confinement in magnetic nanostructures and interaction between magnetic adatoms.

We present a novel approach to spin manipulation in atomic-scale nanostructures. Our ab initio calculations clearly demonstrate that it is possible to tune magnetic properties of subnanometer structures by adjusting the geometry of the system. By the example of two surface-based systems we demonstrate the following. (i) The magnetic moment of a single adatom coupled to a buried magnetic Co layer can be stabilized in either a ferromagnetic or an antiferromagnetic configuration depending on the spacer thickness. It is found that a buried Co layer has a profound effect on the exchange interaction between two magnetic impurities on the surface. (ii) The exchange interaction between magnetic adatoms can be manipulated by introducing artificial nonmagnetic Cu chains to link them.

We review the state of the art of surface magnetic property control with non-magnetic means, concentrating on metallic surfaces and techniques such as charge-doping or external electric field (EEF) application. Magneto-electric coupling via EEF-based charge manipulation is discussed as a way to tailor single adatom spins, exchange interaction between adsorbates or anisotropies of layered systems. The mechanisms of paramagnetic and spin-dependent electric field screening and the effect thereof on surface magnetism are discussed in the framework of theoretical and experimental studies. The possibility to enhance the effect of EEF by immersing the target system into an electrolyte or ionic liquid is discussed by the example of substitutional impurities and metallic alloy multilayers. A similar physics is pointed out for the case of charge traps, metallic systems decoupled from a bulk electron bath. In that case the charging provides the charge carrier density changes necessary to affect the magnetic moments and anisotropies in the system. Finally, the option of using quasi-free electrons rather than localized atomic spins for surface magnetism control is discussed with the example of Shockley-type metallic surface states confined to magnetic nanoislands.