A critical analysis of vacancy-induced magnetism in mono and bilayer graphene

Abstract

The observation of intrinsic magnetic order in graphene and graphene-based materials relies on the formation of magnetic moments and a sufficiently strong mutual interaction. Vacancies are arguably considered the primary source of magnetic moments. Here we present an in-depth density functional theory study of the spin-resolved electronic structure of (monoatomic) vacancies in graphene and bilayer graphene. We use two different methodologies: supercell calculations with the SIESTA code and cluster-embedded calculations with the ALACANT package. Our results are conclusive: The vacancy-induced extended $\pi$ magnetic moments, which present long-range interactions and are capable of magnetic ordering, vanish at any experimentally relevant vacancy concentration. This holds for $\sigma$-bond passivated and un-passivated reconstructed vacancies, although, for the un-passivated ones, the disappearance of the $\pi$ magnetic moments is accompanied by a very large magnetic susceptibility. Only for the unlikely case of a full $\sigma$-bond passivation, preventing the reconstruction of the vacancy, a full value of 1${\mu }_B$ for the $\pi$ extended magnetic moment is recovered for both mono and bilayer cases. Our results put on hold claims of vacancy-induced ferromagnetic or antiferromagnetic order in graphene-based systems, while still leaving the door open to $\sigma$-type paramagnetism.

arXiv commentSubmitted to Phys. Rev B, 9 pages

References in corpus (39)

• The SIESTA method for ab initio order-N materials simulation
• Efficient index handling of multidimensional periodic boundary conditions
• Van der Waals Density Functional for General Geometries
• Half-Metallic Graphene Nanoribbons
• Selfconsistent order-N density-functional calculations for very large systems
• Efficient implementation of a van der Waals density functional: Application to double-wall carbon nanotubes
• Magnetism in Graphene Induced by Single-Atom Defects
• Electronic and Magnetic Properties of Nanographite Ribbons
• The missing atom as a source of carbon magnetism
• Spin-half paramagnetism in graphene induced by point defects
• Magnetism in graphene nano-islands
• Self-passivating edge reconstructions of graphene
• Spatially Resolving Spin-split Edge States of Chiral Graphene Nanoribbons
• Structure, Stability, Edge States and Aromaticity of Graphene Ribbons
• Room-temperature ferromagnetism in graphite driven by 2D networks of point defects
• Disorder Induced Localized States in Graphene
• Magnetic nanographite
• Vacancy induced magnetism in graphene and graphene ribbons
• Ferromagnetism in Oriented Graphite Samples
• Local defects and ferromagnetism in graphene layers
• Metallic Graphene Nanodisks
• Half-metallic graphene nanodots
• Stability of edge states and edge magnetism in graphene nanoribbons
• Electronic and structural characterization of divacancies in irradiated graphene
• First principles study of magnetism in nanographenes
• Hydrogenated Graphene Nanoribbons for Spintronics
• A Defective Graphene Phase Predicted to be a Room Temperature Ferromagnetic Semiconductor
• Magnetoresistance and Magnetic Ordering Fingerprints in Hydrogenated Graphene
• Experimental Evidence for Two-Dimensional Magnetic Order in Proton Bombarded Graphite
• Magnetic moments in the presence of topological defects in graphene
• Ground-state properties of nanographite systems with zigzag-shaped edges
• Direct Imaging of Graphene Edges: Atomic Structure and Electronic Scattering
• A new type of vacancy-induced localized states in multilayer graphene
• An upper bound for the magnetic force gradient in graphite
• Magnetism and structure at a vacancy in graphene
• Monovacancy-induced magnetism in graphene bilayers
• Impurity band induced by point defects in graphene
• Density of states of a graphene in the presence of strong point defects
• Hysteresis loops of the magnetoconductance in graphene devices

Cited by in corpus (41)

• Graphene Spintronics
• Dual origin of defect magnetism in graphene and its reversible switching by molecular doping
• The Physics of Kondo Impurities in Graphene
• Electronic Structures of N-doped Graphene with Native Point Defects
• Vacancy in graphene: insight on magnetic properties from theoretical modeling
• Vacancy in graphene: insight on magnetic properties from theoretical modeling
• Direct imaging of monovacancy-hydrogen complexes in single graphitic layer
• Substitutional 4d and 5d Impurities in Graphene
• Hydrogenation-induced ferromagnetism on graphite surfaces
• Electronic structure of vacancy resonant states in graphene: a critical review of the single vacancy case
• Kondo effect with diverging hybridization: possible realization in graphene with vacancies
• Spin coupling around a carbon atom vacancy in graphene
• Modelling magnetism of C at O and B monovacancies in graphene
• Intertwined Lattice Deformation and Magnetism in Monovacancy Graphene
• On the connection between structural distortion and magnetism in graphene with a single vacancy
• Block Lanczos density-matrix renormalization group method for general Anderson impurity models: Application to magnetic impurity problems in graphene
• Point Defects in Twisted Bilayer Graphene: A Density Functional Theory Study
• Defect-induced magnetism and Yu-Shiba-Rusinov states in twisted bilayer graphene
• Coulomb charging energy of vacancy-induced states in graphene
• Hyperfine magnetic field in ferromagnetic graphite
• Pressure induced magnetism in rotated graphene bilayers
• Disorder-mediated Kondo effect in graphene
• Competing magnetism in $\pi$ electrons in graphene with a single carbon vacancy
• Knock-on damage in bilayer graphene: indications for a catalytic pathway
• Vacancy mediated magnetization and healing of a graphene monolayer
• Interaction between single vacancies in graphene sheet: An ab initio calculation
• Transport signatures of Kondo physics and quantum criticality in graphene with magnetic impurities
• Gate-dependent vacancy diffusion in graphene
• Theoretical Analysis on Pseudo-Degenerate Zero-Energy Modes in Vacancy-Centered Hexagonal Armchair Nanographene
• Spin signatures in the electrical response of graphene nanogaps
• Spin relaxation in disordered graphene: Interplay between puddles and defect-induced magnetism
• Anomalous exchange interaction between intrinsic spins in conducting graphene systems
• Vacancy-induced tunable Kondo effect in twisted bilayer graphene
• Origin of $sp$-electron magnetism in Graphitic Carbon Nitride
• Tunable magnetism of a single-carbon vacancy in graphene
• Collective resonances near zero energy induced by a point defect in bilayer graphene
• Pseudospin-mediated Atomic-scale Vortices and Their Quantum Interferences in Monolayer Graphene
• Monovacancy paramagnetism in neutron-irradiated graphite probed by ${}^{13}$C NMR
• Novel mechanism for weak magnetization with high Curie temperature observed in H-adsorption on graphene
• Magnetic correlation effects by the topological zero mode in a hydrogenated graphene vacancy $V_{111}$
• Ferromagnetism in graphene traced to an antisymmetric orbital combination of involved electronic states