Mapping Orbital-Resolved Magnetism in Single Lanthanide Atoms

Aparajita Singha, Daria Sostina, Christoph Wolf, Safa L. Ahmed, Denis Krylov, Luciano Colazzo, Pierluigi Gargiani, Stefano Agrestini, Woo Suk Noh, Jae Hoon Park, Marina Pivetta, Stefano Rusponi, Harald Brune, Andreas J. Heinrich, Alessandro Barla, Fabio Donati

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

Single lanthanide atoms and molecules are promising candidates for atomic data storage and quantum logic due to the long lifetime of their magnetic quantum states. Accessing and controlling these states through electrical transport requires precise knowledge of their electronic configuration at the level of individual atomic orbitals, especially of the outer shells involved in transport. However, no experimental techniques have so far shown the required sensitivity to probe single atoms with orbital selectivity. Here we resolve the magnetism of individual orbitals in Gd and Ho single atoms on MgO/Ag(100) by combining X-ray magnetic circular dichroism with multiplet calculations and density functional theory. In contrast to the usual assumption of bulk-like occupation of the different electronic shells, we establish a charge transfer mechanism leading to an unconventional singly ionized configuration. Our work identifies the role of the valence electrons in determining the quantum level structure and spin-dependent transport properties of lanthanide-based nanomagnets.

Original languageEnglish
Pages (from-to)16162-16171
Number of pages10
JournalACS Nano
Volume15
Issue number10
DOIs
StatePublished - 26 Oct 2021

Keywords

  • X-ray magnetic circular dichroism
  • charge transfer
  • lanthanide magnetism
  • orbital resolved magnetism
  • single atoms

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