Strong bonding and high spin-polarization of lanthanide atoms on vacancies in graphene

Abstract

The atomic structures, adsorption energies, and spin polarizations of lanthanide (Ln = La-Gd) atoms adsorbed on the single and double vacancies in graphene are investigated systematically by the first- principles calculations. The calculations show that the Ln atoms adsorb on the centers of the vacancies with large adsorption energies, in the range of 3.57 ∼ 8.45 eV. The adsorbed Ln atoms also dope a large number of electrons into the graphene. Most of the Ln atoms are highly spin-polarized. The strong adsorption and high spin polarization gives these systems potential application in spintronic and catalyst materials.

Adsorption of Lanthanide Atoms on Graphene: Similar, Yet Different

“…The density of states (DOS) is one of the most important and frequently analyzed electronic characteristics of graphenerelated materials, including those doped with lanthanides. 1 4 , 1 6 , 1 7 , 1 9 , 2 0 The point that the previous works 14,16,17,19,20 have in common is that the limits of energies analyzed is not very far from the Fermi level, for obvious reasons of studying the conductivity properties, comprising at best from −10 to 5 eV. 16 In our case, DOS plots (Figures 4 and S1) for different G+Ln complexes, as could be expected, exhibit individual distinctive features.…”

“…One of the most relevant observations in this context is that, to the best of our knowledge, none of the published research reports consider the full series (that is, La and 14 lanthanides) of 4 f elements adsorbed on graphene. At best, all the early lanthanides are included (La, Ce, Pr, Nd, Pm, Sm, Eu, and Gd interacting with single and double vacancies), , or representative elements are selected rather randomly (Nd, Sm, Eu, Gd, Dy, and Yb on defect-free graphene; , Nd, Pm, Sm, Eu, Gr, Er, Tm, Yb, and Lu on nitrogenated holey doped graphene g-C 2 N; Er, Tm, and Yb on graphene/WSe 2 heterostructures). Instead, the analysis is limited to one or two lanthanides, such as Eu, Gd, Dy, − La, and Lu .…”

Strong Bending Distortion of a Supercoronene Graphene Model upon Adsorption of Lanthanide Atoms

“…The systematic theoretical study of the interaction of a broad variety of chemical elements (especially metals) with graphene and graphene-based substrates is an indispensable tool in the search of new efficient approaches for modifying physical, chemical, and other properties of this important class of nanomaterials. − An especially important and intriguing case involves the lanthanide metals (including La itself and the Ce–Lu series) due to their particularly complex 4f electron configurations that can have a strong and nontrivial influence on graphene properties and raise significant challenges in the quantum-chemical treatment. Several density functional theory (DFT) studies have been undertaken with periodic graphene models, but never comprising the full series of 15 elements, ,,− with the only exception being our recent report …”