Spin-State Engineering of Single Titanium Adsorbates on Ultrathin Magnesium Oxide

Abstract

Single atomic adsorbates on ultrathin insulating films provide a promising route toward bottom-up quantum architectures based on atomically identical yet individually addressable spin qubits on solid surfaces. A key challenge in engineering quantum-coherent spin nanostructures lies in understanding and controlling the spin state of individual adsorbates. In this work, we investigate single titanium (Ti) atoms adsorbed on MgO/Ag(100) surfaces using a combined scanning tunneling microscopy and electron spin resonance. Our measurements reveal two distinct spin states, $S=1/2$ and $S=1$, depending on the local adsorption site and the thickness of the MgO film. Density functional theory calculations suggest a Ti${}^{+}$ configuration for the Ti adsorbates with approximately 3 electrons in the 4$s$ and 3$d$ valence shells. Using a multi-orbital atomic multiplet calculations the site dependence of the spin can be rationalized as a charge redistribution between spin-polarizing and depolarizing orbitals. These findings underscore the potential of surface-supported single atoms as spin qubits with tunable spin and charge states, enabling atom-by-atom control in the realization of a versatile quantum platform on surfaces.

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• Overcoming limitations on gate fidelity in noisy static exchange-coupled surface qubits
• Theory of Electron Spin Resonance Scanning Tunneling Microscopy: The First Decade