The magnetism by the edge states in graphene is investigated theoretically. An instability of the pseudo-spin order of the edge states induces ferrimagnetic order in the presence of the Coulomb interaction. Although the next nearest-neighbor hopping can stabilize the pseudo-spin order, a strong Coulomb interaction makes the pseudo-spin unpolarized and real spin polarized. The magnetism of the edge states makes two peaks of the density of states in the conduction and valence energy bands near the Fermi point. Using a continuous model of the Weyl equation, we show that the edge-induced gauge field and the spin dependent mass terms are keys to make the magnetism of the edge states. A relationship between the magnetism of the edge states and the parity anomaly is discussed.
The electronic structure, bonding and magnetism in graphene containing vacancies are studied using density-functional methods. The single-vacancy graphene ground state is spin polarized and structurally flat. The unpolarized state is non planar only for finite segments. Systems containing periodic arrays of vacancies displays magnetic transitions and metal-insulator transitions.
We study edge state magnetism in graphene nanostructures using a mean field theory of the Hubbard model. We investigate how the magnetism of the zigzag edges of graphene is affected by the presence of other types of terminating edges and defects. By a detailed study of both regular shapes, such as polygonal nanodots and nanoribbons, and irregular shapes, we conclude that the magnetism in zigzag edges is very robust. Our calculations show that the zigzag edges that are longer than three to four repeat units are always magnetic, irrespective of other edges, regular or irregular. We, therefore, c…
Inducing magnetism in graphene holds great promises, such as controlling the exchange interaction with a gate electrode and generating exotic magnetic phases. Coating graphene with magnetic molecules or atoms has so far mostly lead to decreased graphene mobility. In the present work, we show that Pt-porphyrins adsorbed on graphene lead to an enhanced mobility and to gate-dependent magnetism. We report that porphyrins can be donor or acceptor, depending on graphene s initial doping. The porphyrins transfer charge and ionize around the charged impurities on graphene, decreasing the graphene dopi…
Although the unconventional $π$-magnetism at the zigzag edges of graphene holds promise for a wide array of applications, whether and to what degree it plays a role in their chemistry remains poorly understood. Here, we investigate the addition of a hydrogen atom $-$ the simplest yet the most experimentally relevant adsorbate $-$ to zigzag graphene nanoribbons (ZGNRs). We show that the $π$-magnetism governs the chemistry of ZGNRs, giving rise to a site-dependent reactivity of the carbon atoms and driving the hydrogenation process to the nanoribbon edges. Conversely, the chemisorbed hydrogen at…
Atomic defects have a significant impact in the low-energy properties of graphene systems. By means of first-principles calculations and tight-binding models we provide evidence that chemical impurities modify both the normal and the superconducting states of twisted bilayer graphene. A single hydrogen atom attached to the bilayer surface yields a triple-point crossing, whereas self-doping and three-fold symmetry-breaking are created by a vacant site. Both types of defects lead to time-reversal symmetry-breaking and the creation of local magnetic moments. Hydrogen-induced magnetism is found to…
We have studied magnetization of graphene nanocrystals obtained by sonic exfoliation of graphite. No ferromagnetism is detected at any temperature down to 2 K. Neither do we find strong paramagnetism expected due to the massive amount of edge defects. Rather, graphene is strongly diamagnetic, similar to graphite. Our nanocrystals exhibit only a weak paramagnetic contribution noticeable below 50K. The measurements yield a single species of defects responsible for the paramagnetism, with approximately one magnetic moment per typical graphene crystallite.
Removing a single-carbon vacancy introduces (quasi-)localized states for both and electrons in graphene. Interactions between the localized dangling bond and quasilocalized electrons of a single-carbon vacancy in graphene are predicted to control its magnetism. However, experimentally confirming this prediction through manipulating the interactions between the and electrons remains an outstanding challenge. Here we report the manipulation of magnetism of individual single-carbon vacancy in graphene by using a scanning tunnelling microscopy (STM) tip. Our spin-polarized STM measurements, comple…
We discuss several mechanisms of magnetism and band opening in graphene produced by its hydrogenation and fluorination that can be examined experimentally.
We unveil the nature of the structural disorder in bottom-up zigzag graphene nanoribbons along with its effect on the magnetism and electronic transport on the basis of scanning probe microscopies and first-principles calculations. We find that edge-missing m-xylene units emerging during the cyclodehydrogenation step of the on-surface synthesis are the most common point defects. These "bite'' defects act as spin-1 paramagnetic centers, severely disrupt the conductance spectrum around the band extrema, and give rise to spin-polarized charge transport. We further show that the electronic conduct…
Isolated hydrogen atoms absorbed on graphene are predicted to induce magnetic moments. Here we demonstrate that the adsorption of a single hydrogen atom on graphene induces a magnetic moment characterized by a ~20 meV spin-split state at the Fermi energy. Our scanning tunneling microscopy (STM) experiments, complemented by first-principles calculations, show that such a spin-polarized state is essentially localized on the carbon sublattice complementary to the one where the H atom is chemisorbed. This atomically modulated spin-texture, which extends several nanometers away from the H atom, dri…
The pristine graphene is strongly diamagnetic. However, graphene with single carbon atom defects could exhibit paramagnetism with local magnetic moments ~ 1.5 per vacancy1-6. Theoretically, both the electrons and electrons of graphene contribute to the magnetic moment of the defects, and the pi magnetism is characterizing of two spin-split DOS (density-of-states) peaks close to the Dirac point1,6. Since its prediction, many experiments attempt to study this pi magnetism in graphene, whereas, only a notable resonance peak has been observed around the atomic defects6-9, leaving the pi magnetism …
By first principles calculations, we demonstrate that when decorated with photochromic molecules, it is possible to use light to reversibly control the magnetic properties of a nanoscale magnetic system. The combination of a graphene-based magnetic system and a photochromic azobenzene molecule is chosen as a model system. The {\it trans} and {\it cis} isomers of the azobenzene molecule that can be converted between each other by means of photoexcitations are found to have drastically different effects on the magnetic properties of the system. The results may pave the way for the future design …
The effects of biaxial strain on the impurity-induced magnetism in P-doped graphene (P-graphene) and N-doped silicene (N-silicene) are studied by means of spin-polarized density functional calculations, using the supercell approach. The calculations were performed for three different supercell sizes $4\times 4$, $5\times 5$, and $6\times 6$, in order to simulate three different dopant concentrations 3.1, 2.0 and 1.4 %, respectively. For both systems, the calculated magnetic moment is 1.0 $μ_B$ per impurity atom for the three studied concentrations. From the analysis of the electronic structure…
We address the electronic structure and magnetic properties of vacancies and voids both in graphene and graphene ribbons. Using a mean field Hubbard model, we study the appearance of magnetic textures associated to removing a single atom (vacancy) and multiple adjacent atoms (voids) as well as the magnetic interactions between them. A simple set of rules, based upon Lieb theorem, link the atomic structure and the spatial arrangement of the defects to the emerging magnetic order. The total spin $S$ of a given defect depends on its sublattice imbalance, but some defects with S=0 can still have l…
Magnetic carbon nanostructures are currently under scrutiny for a wide spectrum of applications. Here, we theoretically investigate armchair graphene nanoribbons patterned with asymmetric edge extensions consisting of laterally fused naphtho groups, as recently fabricated via on-surface synthesis. We show that an individual edge extension acts as a spin-$\frac{1}{2}$ center and develops a sizable spin-polarization of the conductance around the band edges. The Heisenberg exchange coupling between a pair of edge extensions is dictated by the position of the second naphtho group in the carbon bac…
Orbital angular momentum (OAM) of graphene electrons in a perpendicular magnetic field is calculated and corresponding magnetic moment is used to investigate the magnetism of perfect graphene. Variation in magnetization demonstrates its decrease with carrier-doping, plateaus in a large field, and de Haas-van Alphen oscillation. Regulation of magnetism by a parallel electric field is presented. The OAM originates from atomic-scale electronic motion in graphene lattice, and vector hopping interaction between carbon atomic orbitals is the building element. A comparison between OAM of graphene ele…
Magnetism is a prototypical phenomenon of quantum collective state, and has found ubiquitous applications in semiconductor technologies such as dynamic random access memory (DRAM). In conventional materials, it typically arises from the strong exchange interaction among the magnetic moments of d- or f-shell electrons. Magnetism, however, can also emerge in perfect lattices from non-magnetic elements. For instance, flat band systems with high density of states (DOS) may develop spontaneous magnetic ordering, as exemplified by the Stoner criterion. Here we report tunable magnetism in rhombohedra…
Realizing magnetism in graphene/carbon nanostructures is a decade-long challenge. The magnetic edge state and half metallicity in zigzag graphene nanoribbons are particularly promising [Y.-W. Son, et al., Nature 444, 347 (2006)]. However, its experimental realization has been hindered by the stringent requirement of the mono-hydrogenated zigzag edge. Using first-principle calculations, we predict that free-carrier doping can overcome this challenge and realize ferromagnetism and half-metallicity in narrow graphene nanoribbons of general types of edge structures. This magnetism exists within th…
We study in this paper the edge polarizations and their consequences for a biased Bernal stacked bilayer graphene nanoribbon with zigzag termination. The magnetic states are classified according to the interlayer and intralayer couplings between the edge polarizations, and the magnetic phase diagram of doping versus bias voltage is given. Coplanar magnetic phase is found and the variation of its magnetic structure with the bias voltage is investigated. For all the magnetic states, we also discuss the possibility of the half-metallicity, and for a ribbon with perfect zigzag edges we predict sev…
Magnetism in single-side hydrogenated (C$_2$H) and fluorinated (C$_2$F) graphene is analyzed in terms of the Heisenberg model with parameters determined from first principles. We predict a frustrated ground state for both systems, which means the instability of collinear spin structures and sheds light on the absence of a conventional magnetic ordering in defective graphene demonstrated in recent experiments. Moreover, our findings suggest a highly correlated magnetic behavior at low temperatures offering the possibility of a spin-liquid state.
We explore possible ways to manipulate the intrinsic edge magnetism in hexagonal graphene nanoflake with zigzag edges, using density functional theory supplemented with on-site Coulomb interaction. The effect of carrier doping, chemical modification at the edge, and finite temperature on the edge magnetism has been studied. The magnetic phase diagram with varied carrier doping, and on-site Coulomb interaction is found to be complex. In addition to the intrinsic antiferromag- netic solution, as predicted for charge neutral hexagonal nanoflake, fully polarized ferromagnetic, and mixed phase solu…
Magnetic materials and nanostructures based on carbon offer unique opportunities for future technological applications such as spintronics. This article reviews graphene-derived systems in which magnetic correlations emerge as a result of reduced dimensions, disorder and other possible scenarios. In particular, zero-dimensional graphene nanofragments, one-dimensional graphene nanoribbons, and defect-induced magnetism in graphene and graphite are covered. Possible physical mechanisms of the emergence of magnetism in these systems are illustrated with the help of computational examples based on …
It is shown that apart from well-known factors, like temperature, substrate, and edge reconstruction effects, also the presence of external contacts is destructive for the formation of magnetic moments at the edges of graphene nanoribbons. The edge magnetism gradually decreases when graphene/electrode interfaces become more and more transparent for electrons. In addition to the graphene/electrode coupling strength, also the aspect ratio parameter, i.e. a width/length ratio of the graphene nanoribbon, is crucial for the suppression of edge magnetism. The present theory uses a tight-binding meth…
The influence of carrier density on magnetism in a zigzag graphene nanoribbon is studied in a $π$-orbital Hubbard-model mean-field approximation. Departures from half-filling alter the magnetism, leading to states with charge density variation across the ribbon and parallel spin-alignment on opposite edges. Finite carrier densities cause the spin-density near the edges to decrease steadily, leading eventually to the absence of magnetism. At low doping densities the system shows a tendency to multiferroic order in which edge charges and spins are simultaneously polarized.
The presence of defects can introduce important changes in the electronic structure of graphene, leading to phenomena such as C magnetism. In addition, vacancies are reactive and permit the incorporation of dopants. This paper discusses the electronic properties of defective graphene for O and B decoration. Phonon calculations allow us to address directly the stability of the systems under study. We show that it is possible to obtain magnetic solutions with and without dangling bonds, demonstrating that C magnetism can be achieved in the presence of B and O.
Using the determinant quantum Monte-Carlo method, we elucidate the strain tuning of edge magnetism in zigzag graphene nanoribbons. Our intensive numerical results show that a relatively weak Coulomb interaction may induce a ferromagnetic-like behaviour with a proper strain, and the edge magnetism can be enhanced greatly as the strain along the zigzag edge increases, which provides another way to control graphene magnetism even at room temperature.
Graphene is a nonmagnetic semimetal and cannot be directly used as electronic or spintronic devices. We demonstrate that graphene quantum dots (GQDs) can exhibit strong edge magnetism and tunable energy gaps due to the presence of localized edge states. By using large-scale first principle density functional theory (DFT) calculations and detailed analysis based on model Hamiltonians, we can show that the zigzag edge states in GQDs become much stronger and more localized as the system size increases. The enhanced edge states induce strong electron-electron interactions along the edges of GQDs, …
We study the magnetization of square and hexagonal graphene dots. It is shown that two classes of hexagonal dots have a second order phase transition at a critical Hubbard energy $U$, whoose value is similar to the one in bulk graphene, albeit the dots do not have a density of states proportional to the absolute value of the energy, relatively to the Dirac point. Furthermore, we show that a particular class of hexagonal dots having zig-zag edges, does not exhibit zero energy edge states. We also study the effect of uniaxial strain on the evolution of the magnetization of square dots, and find …
Twisted graphene bilayers develop highly localised states around AA-stacked regions for small twist angles. We show that interaction effects may induce either an antiferromagnetic (AF) and a ferromagnetic (F) polarization of said regions, depending on the electrical bias between layers. Remarkably, F-polarised AA regions under bias develop spiral magnetic ordering, with a relative $120^\circ$ misalignment between neighbouring regions due to a frustrated antiferromagnetic exchange. This remarkable spiral magnetism emerges naturally without the need of spin-orbit coupling, and competes with the …
Twisted graphene bilayers (TGBs) have low-energy van Hove singularities (VHSs) that are strongly localized around AA-stacked regions of the moire pattern. Therefore, they exhibit novel many-body electronic states, such as Mott-like insulator and unconventional superconductivity. Unfortunately, these strongly correlated states were only observed in magic angle TGBs with the twist angle theta~1.1°, requiring a precisely tuned structure. Is it possible to realize exotic quantum phases in the TGBs not limited at the magic angle? Here we studied electronic properties of a TGB with theta~1.64° and d…
In order to study a magnetic principle of carbon based materials, multiple spin state of zigzag edge modified graphene molecules are analyzed by the first principle density functional theory to select suitable modification element. Radical carbon modified C64H17 shows that the highest spin state is most stable, which arises from two up-spin's tetrahedral molecular orbital configuration at zigzag edge. In contrast, oxygen modified C59O5H17 show the lowest spin state to be most stable due to four spins cancellation at oxygen site. Boron modified C59B5H22 have no π-molecular orbit at boron site t…
We present the results of ab-initio density functional theory based calculations of the stability and reconstruction of zigzag edges in triangular graphene quantum dots. We show that, while the reconstructed pentagon-heptagon zigzag edge structure is more stable in the absence of hydrogen, ideal zigzag edges are energetically favored by hydrogen passivation. Zero-energy band exists in both structures when passivated by hydrogen, however in case of pentagon-heptagon zigzag, this band is found to have stronger dispersion, leading to the loss of net magnetization.
We report {\it ab initio} calculations of the structural, electronic and magnetic properties of a graphene monolayer substitutionally doped with Co (Co$_{sub}$) atoms. We focus in Co because among traditional ferromagnetic elements (Fe, Co and Ni), only Co$_{sub}$ atoms induce spin-polarization in graphene. Our results show the complex magnetism of Co substitutional impurites in graphene, which is mapped into simple models such as the $π$-vacancy and Heisenberg model. The links established in our work can be used to bring into contact the engineering of nanostructures with the results of $π$-m…
We report a strain-controlled tuning of magnetism in transition-metal-atom-decorated graphene. Our first-principles calculations demonstrate that strain can lead to a sudden change in the magnetic configuration of a transition metal (TM) adatom and the local atomic structure in the sur- rounding graphene layer, which have a dramatic effect on the effective exchange coupling between neighboring TM atoms. A strong spin-dependent hybridization between TM d and graphene 1/4 orbital states, derived from the orbital selection rule of the local lattice symmetry, is responsible for the determination o…
The magnetic properties of disordered graphene and irradiated graphite are systematically studied using a combination of mean-field Hubbard model and first-principles calculations. By considering large-scale disordered models of graphene, I conclude that only single-atom defects can induce ferromagnetism in graphene-based materials. The preserved stacking order of graphene layers is shown to be another necessary condition for achieving a finite net magnetic moment of irradiated graphite. Ab initio calculations of hydrogen binding and diffusion and of interstitial-vacancy recombination further …
Magnetic properties of graphenic carbon nanostructures, relevant for future spintronic applications, depend crucially on doping and on the presence of defects. In this paper we study the magnetism of the recently detected substitutional Ni (Ni(sub)) impurities. Ni(sub) defects are non-magnetic in flat graphene and develop a non-zero magnetic moment only in metallic nanotubes. This surprising behavior stems from the peculiar curvature dependence of the electronic structure of Ni(sub). A similar magnetic/non-magnetic transition of Ni(sub) can be expected by applying anisotropic strain to a flat …
It is argued that the subtle crossover from decoherence-dominated classical magnetism to fluctuation-dominated quantum magnetism is experimentally accessible in graphene nanoribbons. We show that the width of a nanoribbon determines whether the edge magnetism is on the classical side, on the quantum side, or in between. In the classical regime, decoherence is dominant and leads to static spin polarizations at the ribbon edges, which are well described by mean-field theories. The quantum Zeno effect is identified as the basic mechanism which is responsible for the spin polarization and thereby …
Atomic vacancies have a strong impact in the mechanical, electronic and magnetic properties of graphene-like materials. By artificially generating isolated vacancies on a graphite surface and measuring their local density of states on the atomic scale, we have shown how single vacancies modify the electronic properties of this graphene-like system. Our scanning tunneling microscopy experiments, complemented by tight binding calculations, reveal the presence of a sharp electronic resonance at the Fermi energy around each single graphite vacancy, which can be associated with the formation of loc…
In the presence of the Hubbard interaction, graphene zigzag nanoribbons have spontaneous edge magnetism with anti-parallel configuration, whose amplitude can be tuned by a transversal electric field. As the electric field increases or decreases across a critical value, the edges are demagnetized or re-magnetized, respectively. A magnetic field at each edge determines the orientation of the re-magnetization. Thus, a combination of slowly varying transversal electric field and magnetic field in monolayer graphene zigzag nanoribbon could drive the quantum system into a bistability loop. The same …
The magnetic and spin transport properties of a carbon chain between two armchair graphene nanoribbon (AGNR) electrodes were studied using tight-binding Hamiltonian, mean-field Hubbard model and Landauer-Butikker formalism. The results showed that only odd-numbered carbon chains show intrinsic magnetic moments in chain-graphene junctions. It was also found that the electronic, magnetic and spin transport properties of carbon chain-graphene junctions strongly depend on the position and the length of the carbon chains between AGNR electrodes. Interestingly, we found a fully spin-polarized transm…
We review recent progress on spins and magnetism in 2D materials including graphene, transition metal dichalcogenides, and 2D magnets. We also discuss challenges and prospects for the future of spintronics with 2D van der Waals heterostructures.
We study the magnetic properties of graphene edges and graphene/graphane interfaces under the influence of electrostatic gates. For this, an effective low-energy theory for the edge states, which is derived from the Hubbard model of the honeycomb lattice, is used. We first study the edge state model in a mean-field approximation for the Hubbard Hamiltonian and show that it reproduces the results of the extended 2D lattice theory. Quantum fluctuations around the mean-field theory of the effective one-dimensional model are treated by means of the bosonization technique in order to check the stab…
Magnetic force microscopy (MFM) signals have recently been detected from whole pieces of mechanically exfoliated graphene and molybdenum disulfide (MoS2) nanosheets and magnetism of the two nanomaterials was claimed based on these observations. However, non-magnetic interactions or artefacts are commonly associated with MFM signals, which makes the interpretation of MFM signals not straightforward. A systematic investigation has been done to examine possible sources of the MFM signals from graphene and MoS2 nanosheets and whether the MFM signals can be correlated with magnetism. It is found th…
Using first-principles calculations, we explore the electronic and magnetic properties of graphene nanomesh (GNM), a regular network of large vacancies, produced either by lithography or nanoimprint. When removing an equal number of A and B sites of the graphene bipartite lattice, the nanomesh made mostly of zigzag (armchair) type edges exhibit antiferromagnetic (spin unpolarized) states. In contrast, in situation of sublattice symmetry breaking, stable ferri(o)magnetic states are obtained. For hydrogen-passivated nanomesh, the formation energy is dramatically decreased, and ground state is fo…
Vacancies in graphene lead to the appearance of localized electronic states with non-vanishing spin moments. Using a mean-field Hubbard model and an effective double-quantum dot description we investigate the influence of strain on localization and magnetic properties of the vacancy-induced states in semiconducting armchair nanoribbons. We find that the exchange splitting of a single vacancy and the singlet-triplet splitting for two vacancies can be widely tuned by applying uniaxial strain, which is crucial for spintronic applications.
A bosonic field theory is derived for the tunable edge magnetism at graphene zigzag edges. The derivation starts from an effective fermionic theory for the interacting graphene edge states, derived previously from a two-dimensional interacting tight-binding model for graphene. The essential feature of this effective model, which gives rise to the weak edge magnetism, is the momentum-dependent non-local electron-electron interaction. It is shown that this momentum-dependence may be treated by an extension of the bosonization technique, and leads to interactions of the bosonic fields. These inte…
The recent discovery of two-dimensional magnetic insulators has generated a great deal of excitement over their potential for nanoscale manipulation of spin or magnetism. One intriguing use for these materials is to put them in contact with graphene, with the goal of making graphene magnetic while maintaining its unique electronic properties. Such a system could prove useful in applications such as magnetic memories, or could serve as a host for exotic states of matter. Proximity to a magnetic insulator will alter the spin transport properties of graphene, and the strength of this interaction …
We perform density functional theory calculations for the determination of the structural and electronic properties of epitaxial graphene on 4H-SiC(000$\bar{1}$). Using commensurate supercells that minimize non-physical stresses we show that, in contrast with Si-face epitaxial films, the first graphene layer that forms on the C-face of SiC is purely metallic with its $π$-bands partially preserved. Typical free-standing characteristics are fully recovered with a second graphene layer. We moreover discuss on the magnetic properties of the interface and the absence of Fermi-level pinning effects …
Orbital magnetism is studied for graphene flakes with various shapes and edge configurations using the tight-binding approximation. In the low-temperature regime where the thermal energy is much smaller than to the energy level spacing, the susceptibility rapidly changes between diamagnetism and paramagnetism as a function of Fermi energy, in accordance with the energy level structure. The susceptibility at charge neutral point is generally larger in armchair flake than in zigzag flake, and larger in hexagonal flake than in triangular flake. As the temperature increases, the discrete structure…
A possibility to control magnetic properties by using electric fields is one of the most desirable characteristics for spintronics applications. Finding a suitable material remains an elusive goal, with only a few candidates found so far. Graphene is one of them and offers a hope due to its weak spin-orbit interaction, the ability to control electronic properties by the electric field effect and the possibility to introduce paramagnetic centres such as vacancies and adatoms. Here we show that adatoms magnetism in graphene is itinerant and can be controlled by doping, so that magnetic moments c…
Hydrogen adatoms are one of the most the promising proposals for the functionalization of graphene. Hydrogen induces narrow resonances near the Dirac energy, which lead to the formation of magnetic moments. Furthermore, they also create local lattice distortions which enhance the spin-orbit coupling. The combination of magnetism and spin-orbit coupling allows for a rich variety of phases, some of which have non trivial topological features. We analyze the interplay between magnetism and spin-orbit coupling in ordered arrays of hydrogen on graphene monolayers, and classify the different phases …
We study the spin relaxation in graphene due to magnetic moments induced by defects. We propose and employ in our studies a microscopic model that describes magnetic impurity scattering processes mediated by charge puddles. This model incorporates the spin texture related to the defect-induced state. We calibrate our model parameters using experimentally-inferred values. The results we obtain for the spin relaxation times are in very good agreement with experimental findings. Our study leads to a comprehensive explanation for the short spin relaxation times reported in the experimental literat…
We report a thorough study of the reducibility of edge correlation effects in graphene to much-simplified effective models for the edge states. The latter have been used before in specially tailored geometries. By a systematic investigation of corrections due to the bulk states in second order perturbation theory, we show that the reduction to pure edge state models is well-justified in general geometries. The framework of reduced models discussed here enables the study of non-mean-field correlation physics for system sizes far beyond the reach of conventional methods, such as, e.g., quantum M…
Edge states in narrow quasi two-dimensional nanostructures determine, to a large extent, their electric, thermoelectric and magnetic properties. Non-magnetic edge states may quite often lead to topological insulator type behavior. However another scenario develops when the zigzag edges are magnetic and the time reversal symmetry is broken. In this work we report on the electronic band structure modifications, electrical conductance and thermoelectric properties of narrow zigzag nanoribbons with spontaneously magnetized edges. Theoretical studies based on the Kane-Mele- Hubbard tight-binding mo…
We study the role of non-locality of exchange in a neutral zigzag graphene nanoribbon within the $π$-orbital unrestricted Hartree-Fock approximation. Within this theory we find that the magnetic features are further stabilized for both the intra-edge and inter-edge exchange compared to mean field theories of zigzag ribbon based on local exchange (like the Hubbard model or the ab-initio Local Density Approximation). The inter-edge exchange produces an enhancement of the band-gap of the magnetic ground-state solutions. The effect of this enhanced exchange on the edge states can not be satisfacto…
Graphene is a model system for the study of electrons confined to a strictly two-dimensional layer1 and a large number of electronic phenomena have been demonstrated in graphene, from the fractional2, 3 quantum Hall effect to superconductivity4. However, the coupling of conduction electrons to local magnetic moments5, 6, a central problem of condensed matter physics, has not been realized in graphene, and, given carbon's lack of d or f electrons, magnetism in graphene would seem unlikely. Nonetheless, magnetism in graphitic carbon in the absence of transition-metal elements has been reported7-…
The correlation between structural distortion and emergence of magnetism in graphene containing a single vacancy was investigated using first-principles calculations based on density functional theory (DFT). Our results have shown that a local distortion is formed around the vacancy, with reconstruction of two atomic bonds and with a dangling bond remaining at the third atom adjacent to the vacancy. A systematic investigation of the possible out-of-plane displacement of this third atom was then carried out, in order to ascertain its effects on the magnetic features of the system. The ground st…
We revisit the problem of local moment formation in graphene due to chemisorption of individual atomic hydrogen or other analogous sp$^3$ covalent functionalizations. We describe graphene with the single orbital Hubbard model, so that the H chemisorption is equivalent to a vacancy in the honeycomb lattice. In order to circumvent artefacts related to periodic unit cells, we use either huge simulation cells of up to $8\times10^5$ sites, or an embedding scheme that allows the modelling of a single vacancy in an otherwise pristine infinite honeycomb lattice. We find three results that stress the a…
