Single-Spin Sensing: A Molecule-on-Tip Approach.

Magnetometry plays a pivotal role in addressing the requirements of ultradense storage technology and overcoming challenges associated with downscaled spin qubits. A promising approach for atomic-scale single-spin sensing involves utilizing a magnetic molecule as a spin sensor, although such a realization is still in its early stages. To tackle this challenge and underscore the potential of this method, we combined a nickelocene molecule with scanning tunneling microscopy to perform versatile spin-sensitive imaging of magnetic surfaces. We investigated model Co islands on Cu(111) of different thicknesses having variable magnetic properties. Our method demonstrates robustness and reproducibility, providing atomic-scale sensitivity to spin polarization and magnetization orientation, owing to a direct exchange coupling between the nickelocene-terminated tip and the Co surfaces. We showcase the accessibility of magnetic exchange maps using this technique, revealing unique signatures in magnetic corrugation, which are well described by computed spin-density maps. These advancements significantly improve our capacity to probe and visualize magnetism at the atomic level.