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Mutually interacting magnetic atoms coupled to a superconductor have gained enormous interest due to their potential for the realization of topological superconductivity. Individual magnetic impurities produce states within the superconducting energy gap known as Yu–Shiba–Rusinov (YSR) states. Here, using the tip of a scanning tunneling microscope, we artificially craft spin arrays consisting of an Fe adatom interacting with an assembly of interstitial Fe atoms (IFA) on a superconducting oxygen-reconstructed Ta(100) surface and show that the magnetic interaction between the adatom and the IFA assembly can be tuned by adjusting the number of IFAs in the assembly. The YSR state experiences a characteristic crossover in its energetic position and particle–hole spectral weight asymmetry when the Kondo resonance shows spectral depletion around the Fermi energy. By the help of slave-boson mean-field theory (SBMFT) and numerical renormalization group (NRG) calculations we associate the crossover with the transition from decoupled Kondo singlets to an antiferromagnetic ground state of the Fe adatom spin and the IFA assembly effective spin.

Recently the oxygen-reconstructed tantalum surface Ta(001)-p(3×3)-O has experienced considerable attention due its use as a potential platform for Majorana physics in adatom chains. Experimental studies using scanning tunneling microscopy and spectroscopy found rich atomic and electronic structures already for the clean Ta(001)-O surface, which we combine here with ab initio methods. We discover two metastable superstructures at the root of the different topographic patterns, discuss its emergence during annealing, and identify the electronic properties. The latter is determined as the sole origin for the contrast reversal seen at positive bias. The observed effects are essentially connected to the two distinct oxygen states appearing on the surface in different geometries. The second superstructure was found in simulations by introducing oxygen vacancies, what was also observed in tantalum pentoxide systems. Additionally we study the charge distribution on the oxidized surface and underline its importance for the adsorption process of polarizable atoms and molecules.

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