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Multiorbital Interactions and Spin Polarization in Single Rare-Earth Adatoms

Massine Kelai1,2, Stefano Reale1,2,3, Roberto Robles4, Jaehyun Lee1,5, Divya Jyoti4,6, Philippe Ohresser7, Edwige Otero7, Fadi Choueikani7, Fabrice Scheurer8 et al.

Nicolás Lorente4,6, Deung-Jang Choi4,6,9, Aparajita Singha10, and Fabio Donati1,5,*

  • *Contact author: donati.fabio@qns.science

Phys. Rev. Lett. 135, 106203 – Published 5 September, 2025

DOI: https://doi.org/10.1103/mkqz-p424

Abstract

Surface-adsorbed rare-earth nanostructures are ideal platforms to investigate the interplay between intra-atomic interactions and multiorbital spin configurations. However, addressing these properties has posed severe experimental and theoretical challenges. Here, we use the orbital selectivity offered by x-ray absorption spectroscopy to quantify the Coulomb integrals of Nd atoms on conductive surfaces directly from experimental quantities, as well as the variation of individual orbital occupation upon cluster nucleation. Using x-ray magnetic circular dichroism we identify magnetic moments of the order of 0.1−0.2  μB at the 5d orbitals and their magnetic coupling with the 4f spins. Our results validate orbital-resolved x-ray spectroscopy as a reliable method for quantifying complex multiorbital interactions in surface-adsorbed lanthanides.

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