Electronic structure and magnetism of samarium and neodymium adatoms on free-standing graphene

TL;DR

This study investigates the electronic structure and magnetic properties of samarium and neodymium adatoms on free-standing graphene using advanced computational methods beyond standard DFT, revealing their magnetic states and the effects of electron correlations and spin-orbit coupling.

Contribution

The paper applies beyond-DFT methods to accurately determine the magnetic states of rare-earth adatoms on graphene, resolving discrepancies from simpler models and predicting experimentally verifiable magnetic behaviors.

Findings

Sm adatom is nonmagnetic with J=0 after advanced calculations.

Nd adatom remains magnetic with J=4.0.

Advanced methods align better with expected physical properties.

Abstract

The electronic structure of selected rare-earth atoms adsorbed on a free-standing graphene was investigated using methods beyond the conventional density functional theory (DFT+U, DFT+HIA and DFT+ED). The influence of the electron correlations and the spin-orbit coupling on the magnetic properties has been examined. The DFT+U method predicts both atoms to carry local magnetic moments (spin and orbital) contrary to a nonmagnetic $f^6$ ($J=0$) ground-state configuration of Sm in the gas phase. Application of DFT${}+{}$Hubbard-I (HIA) and DFT${}+{}$exact diagonalization (ED) methods cures this problem, and yields a nonmagnetic ground state with six $f$ electrons and $J=0$ for the Sm adatom. Our calculations show that Nd adatom remains magnetic, with four localized $f$ electrons and $J=4.0$. These conclusions could be verified by STM and XAS experiments.