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Main Authors: Phark, Soo-hyon, Bui, Hong Thi, Seo, We-hyo, Liu, Yaowu, Sheina, Valeria, Lee, Curie, Wolf, Christoph, Heinrich, Andreas J., Robles, Roberto, Lorente, Nicolas
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2507.23299
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author Phark, Soo-hyon
Bui, Hong Thi
Seo, We-hyo
Liu, Yaowu
Sheina, Valeria
Lee, Curie
Wolf, Christoph
Heinrich, Andreas J.
Robles, Roberto
Lorente, Nicolas
author_facet Phark, Soo-hyon
Bui, Hong Thi
Seo, We-hyo
Liu, Yaowu
Sheina, Valeria
Lee, Curie
Wolf, Christoph
Heinrich, Andreas J.
Robles, Roberto
Lorente, Nicolas
contents 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.
format Preprint
id arxiv_https___arxiv_org_abs_2507_23299
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Spin-State Engineering of Single Titanium Adsorbates on Ultrathin Magnesium Oxide
Phark, Soo-hyon
Bui, Hong Thi
Seo, We-hyo
Liu, Yaowu
Sheina, Valeria
Lee, Curie
Wolf, Christoph
Heinrich, Andreas J.
Robles, Roberto
Lorente, Nicolas
Mesoscale and Nanoscale Physics
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.
title Spin-State Engineering of Single Titanium Adsorbates on Ultrathin Magnesium Oxide
topic Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2507.23299