Functionalization of a scanning microscopy probe with a single nickelocene allows reproducible spin-sensitive measurements of magnetic systems on surfaces. The triplet ground state of the nickelocene tip gives rise to a characteristic inelastic electron spin-flip excitation, which can change upon interaction with spin systems on the surface. These changes, together with theoretical simulations, enable us to determine the local spin moment on the surface. In this paper, we discuss the experimental and theoretical aspects of nickelocene-tip measurements. We rationalize the interactions between the nickelocene spin and the magnetic centers using a spin Heisenberg and dipole model, complemented by cotunneling theory, and compare the simulated dI/dV with selected experimental results. We developed a Python script to simulate this magnetic interaction, which is available on GitHub.

Department of Condensed Matter Physics Faculty of Mathematics and Physics Charles University Prague Czech Republic

Institute of Physics Academy of Sciences of the Czech Republic Cukrovarnicka 10 Prague 6 CZ 16200 Czech Republic

Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research Institute Palacký University Olomouc Olomouc 78371 Czech Republic

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