Mapping Orbital-Resolved Magnetism in Single Lanthanide Atoms.

Area of Science:

• Quantum physics
• Materials science
• Atomic magnetism

Background:

• Single lanthanide atoms offer potential for atomic data storage and quantum logic due to stable magnetic quantum states.
• Understanding electronic configurations at the orbital level is essential for controlling these states via electrical transport.
• Existing experimental methods lack the sensitivity to probe single atoms with orbital resolution.

Purpose of the Study:

• To experimentally resolve the orbital magnetism of individual Gadolinium (Gd) and Holmium (Ho) atoms on a MgO/Ag(100) surface.
• To determine the electronic configuration and charge state of these single lanthanide atoms.
• To elucidate the role of valence electrons in the quantum properties of lanthanide-based nanomagnets.

Main Methods:

• Combining X-ray magnetic circular dichroism (XMCD) with advanced computational techniques.
• Utilizing multiplet calculations and density functional theory (DFT) for data interpretation.
• Probing single Gd and Ho atoms adsorbed on a MgO/Ag(100) thin film.

Main Results:

• Successfully resolved the magnetic signals from individual atomic orbitals of single Gd and Ho atoms.
• Identified an unconventional singly ionized configuration, challenging the assumption of bulk-like electronic shell occupation.
• Established a charge transfer mechanism influencing the electronic structure.

Conclusions:

• The study provides unprecedented orbital-resolved insights into the magnetism of single lanthanide atoms.
• The findings highlight the importance of valence electron configuration in determining quantum behavior and spin-dependent transport.
• This work paves the way for designing and controlling lanthanide-based nanomagnets for future quantum technologies.