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This content will become publicly available on November 18, 2025

Title: Low-energy magnetic states of Tb adatom on graphene
Abstract Electronic structure and magnetic interactions of a Tb adatom on graphene are investigated from first principles using combination of density functional theory and multiconfigurational quantum chemistry techniques including spin–orbit coupling (SOC) . We determine that the six-fold symmetry hollow site is the preferred adsorption site and investigate electronic spectrum for different adatom oxidation states including Tb3+, Tb2+, Tb1+, and Tb0. For all charge states, the Tb 4 f 8 configuration is retained with other adatom valence electrons being distributed over 5 d x y , 5 d x 2 + y 2 , and 6 s / 5 d 0 single-electron orbitals. We find strong intra-site adatom exchange coupling that ensures that the 5 d 6 s spins are parallel to the4fspin. For Tb3+, the energy levels can be described by theJ = 6 multiplet split by the graphene crystal field (CF). For other oxidation states, the interaction of4felectrons with spin and orbital degrees of freedom of 6 s 5 d electrons in the presence of SOC results in the low-energy spectrum composed closely lying effective multiplets that are split by the graphene CF. Stable magnetic moment is predicted for Tb3+and Tb2+adatoms due to uniaxial magnetic anisotropy and effective anisotropy barrier around 440 cm−1controlled by the temperature assisted quantum tunneling of magnetization through the third excited doublet. On the other hand, in-plane magnetic anisotropy is found for Tb1+and Tb0adatoms. Our results indicate that the occupation of the 6 s 5 d orbitals can dramatically affect the magnetic anisotropy and magnetic moment stability of rare earth adatoms.  more » « less
Award ID(s):
2044049
PAR ID:
10636329
Author(s) / Creator(s):
; ;
Publisher / Repository:
Journal of Physics - Condensed Matter
Date Published:
Journal Name:
Journal of Physics: Condensed Matter
Volume:
37
Issue:
5
ISSN:
0953-8984
Page Range / eLocation ID:
055803
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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