We develop a first-principles theory of resonant impurities in graphene and show that a broad range of typical realistic impurities leads to the characteristic sublinear dependence of the conductivity on the carrier concentration. By means of density functional calculations various organic groups as well as ad-atoms like H absorbed to graphene are shown to create midgap states within +-0.03eV around the neutrality point. A low energy tight-binding description is mapped out. Boltzmann transport theory as well as a numerically exact Kubo formula approach yield the conductivity of graphene contaminated with these realistic impurities in accordance with recent experiments.
Inherent symmetries of a system lead to multiple degeneracies of its energy spectra. Introducing individual atomic impurities can locally break these symmetries, which is expected to lift the degenerate degrees of freedom around the impurities. Although central to our understanding of the fundamental properties of solids, the broken-symmetry states induced by individual atomic impurities have so far eluded observation. Here, we report nanoscale probing of the broken-symmetry states in graphene induced by two types of individual atomic impurities, i.e., isolated nitrogen dopants and isolated hy…
Carbon Impurities on Graphene Synthesized by Chemical Vapor Deposition on Platinum
我们报告了纳米晶碳杂质与通过化学气相沉积（CVD）在铂上合成的石墨烯共存。我们观察到微米尺寸的岛状杂质层，其在光学显微镜或次级电子显微镜（SEM）中容易被误认为第二石墨烯层。岛的取向取决于Pt的结晶取向，如电子背散射衍射（EBSD）所示，表明石墨烯下方的无定形碳的生长。暗场TEM表明，除了均匀的单晶石墨烯之外，我们的样品还装饰有空间不均匀分布的纳米晶碳杂质。拉曼光谱显示出大的D峰，然而电特性显示出高迁移率（~ 6，000 cm 2/Vs），表明拉曼光谱在表征石墨烯的电子质量方面的局限性。
We theoretically study the atomic structure and energetics of silicon and silicon-nitrogen impurities in graphene. Using density-functional theory, we get insight into the atomic structures of the impurities, evaluate their formation energies and assess their abundance in realistic samples. We find that nitrogen, as well as oxygen and hydrogen, are trapped at silicon impurities, considerably altering the electronic properties of the system. Furthermore, we show that nitrogen doping can induce local magnetic moments resulting in spin-dependent transport properties, even though neither silicon n…
Ground-state of graphene in the presence of random charged impurities
我们计算的载流子密度依赖的基态性能的石墨烯在衬底中的随机带电杂质的存在下，考虑到无序和相互作用的影响，在一个自洽的理论形式主义的平等的基础上非微扰。我们提供了详细的定量结果上的依赖性的无序引起的空间不均匀的二维载流子密度分布的外部栅极偏置，杂质密度，和杂质的位置。我们发现，无序和相互作用之间的相互作用是强烈的，特别是在较低的杂质密度。我们表明，对于目前可用的典型石墨烯样品，在低（$\lesssim 10^{12}$ cm $^{-2}$）载流子密度下，不均匀性主导石墨烯物理，密度波动变得大于平均密度。
While imaging individual atoms can routinely be achieved in high resolution transmission electron microscopy, visualizing the potential distribution of individually charged adsorbates leading to a phase shift of the probing electron wave is still a challenging task. Low-energy electrons (30 - 250 eV) are sensitive to localized potential gradients. We employed low-energy electron holography to acquire in-line holograms of individual charged impurities on free-standing graphene. By applying an iterative phase retrieval reconstruction routine we recover the potential distribution of the localized…
Interaction between adsorbed atoms in graphene is studied using a combination of DFT and the path integral formalism. Our results reveal a complex non-monotonic interaction profile. We show that the strength and sign of the interaction are dictated by the arrangement of impurities, as well as the system doping. These findings can be used to interpret the complex behavior of impurities in experimentally realized systems, as well as other classes of impurities, such as C substitutions in graphene.
Experimentally produced graphene sheets exhibit a wide range of mobility values. Both extrinsic charged impurities and intrinsic ripples (corrugations) have been suggested to induce long-range disorder in graphene and could be a candidate for the dominant source of disorder. Here, using large-scale molecular dynamics and quantum transport simulations, we find that the hopping disorder and the gauge and scalar potentials induced by the ripples are short-ranged, in strong contrast with predictions by continuous models, and the transport fingerprints of the ripple disorder are very different from…
We study the interaction between two magnetic adatom impurities in graphene using the Anderson model. The two-impurity Anderson Hamiltonian is solved numerically by using the quantum Monte Carlo technique. We find that the inter-impurity spin susceptibility is strongly enhanced at low temperatures, significantly diverging from the well-known Ruderman-Kittel-Kasuya-Yoshida (RKKY) result which decays as $R^{-3}$.
We study the spin relaxation of charge carriers in graphene in the presence of spin-polarized charged impurities by calculating the time evolution of initially polarized state. The spin relaxation time shows completely different energy behaviour for short-ranged and long-ranged spin scatterers and can be used to identify the dominant source of spin scattering. Our results agree well with recent experimental findings and indicate that their spin relaxation is likely caused by long-ranged scatterers.
Intervalley charged-impurity scattering processes are examined. It is found that the scattering probability is enhanced due to the Coulomb interaction with the impurity by the Sommerfield factor $F_Z\propto ε^{2\sqrt{1-4g^2}-2}$, where $ε$ is the electron energy and $g$ is the dimensionless constant of the Coulomb interaction.
The effective spin exchange coupling between impurities (adatoms) on graphene mediated by conduction electrons is studied as a function of the strength of the potential part of the on-site energy $U$ of the electron-adatom interaction. With increasing $U$, the exchange coupling becomes long-range, determined largely by the impurity levels with energies close to the Dirac points. When adatoms reside on opposite sublattices, their exchange coupling, normally antiferromagnetic, becomes ferromagnetic and resonantly enhanced at a specific distance where an impurity level crosses the Dirac point.
In graphene, charged defects break the electron-hole symmetry and can even give rise to exotic collapse states when the defect charge exceeds a critical value which is proportional to the Fermi velocity. In this work, we investigate the electronic properties of twisted bilayer graphene (tBLG) with charged defects using tight-binding calculations. Like monolayer graphene, tBLG exhibits linear bands near the Fermi level but with a dramatically reduced Fermi velocity near the magic angle (approximately 1.1°). This suggests that the critical value of the defect charge in magic-angle tBLG should al…
The effective interaction between resonant magnetic Anderson impurities in graphene, mediated by conduction electrons, is studied as a function of the strength of the onsite energy level of the impurities and the amplitude of coupling to conduction electrons. The sign and character of the interaction depend on whether the impurities reside on the same or opposite sublattices. For the same (opposite) sublattice, the potential interaction is attractive (repulsive) in the weak coupling limit with $1/R^3$ dependence on the distance; the interaction reverses sign and becomes repulsive (attractive) …
We analyze the electronic properties of bilayer graphene with Bernal stacking and a low concentration of adatoms. Assuming that the host bilayer lies on top of a substrate, we consider the case where impurities are adsorbed only on the upper layer. We describe non-magnetic impurities as a single orbital hybridized with carbon's pz states. The effect of impurity doping on the local density of states with and without a gated electric field perpendicular to the layers is analyzed. We look for Anderson localization in the different regimes and estimate the localization length. In the biased system…
We propose that the observed spin-relaxation in bilayer graphene is due to resonant scattering by magnetic impurities. We analyze a resonant scattering model due to adatoms on both dimer and non-dimer sites, finding that only the former give narrow resonances at the charge neutrality point. Opposite to single-layer graphene, the measured spin-relaxation rate in graphene bilayer increases with carrier density. Although it has been commonly argued that a different mechanism must be at play for the two structures, our model explains this behavior rather naturally in terms of different broadening …
In contrast to monolayer graphene, in bilayer graphene (BLG) one can induce a tunable bandgap by applying an external electric field, which makes it suitable for field effect applications. Extrinsic doping of BLGs enriches the electronic properties of the graphene-based family, as their behavior can be switched from an intrinsic small-gap semiconductor to a degenerate semiconductor. In the framework of density functional theory (DFT) calculations, we investigate the electronic and thermoelectric properties of BLGs doped with extrinsic impurities from groups III (B, Al, Ga), IV (Si, Ge) and V (…
This work analyses how impurities and vacancies on the surface of a graphene sample affect its optical conductivity and plasmon excitations. The disorder is analysed in the self-consistent Green's function formulation and nonlocal effects are fully taken into account. It is shown that impurities modify the linear spectrum and give rise to an impurity band whose position and width depend on the two parameters of our model, the density and the strength of impurities. The presence of the impurity band strongly influences the electromagnetic response and the plasmon losses. Furthermore, we discuss…
We study the effect of a dilute homogeneous spatial distribution of non-magnetic impurities on the equilibrium supercurrent sustained by a ballistic graphene Josephson junction in the short junction limit. Within the Dirac-Bogoliubov-de Gennes approach and modeling impurities by the Anderson model we derive the supercurrent and its equilibrium power spectrum. We find a modification of the current-phase relation with a reduction of the skewness induced by disorder, and a nonmonotonic temperature dependence of the critical current. The potentialities of the supercurrent power spectrum for accura…
We calculate the temperature dependent long-range magnetic coupling in the presence of dilute concentrations of random magnetic impurities in chiral multilayer two-dimensional semimetals, i.e., undoped intrinsic multilayer graphene. Assuming a carrier-mediated indirect RKKY exchange interaction among the well-separated magnetic impurities with the itinerant carriers mediating the magnetic interaction between the impurities, we investigate the magnetic properties of intrinsic multilayer graphene using an effective chiral Hamiltonian model. We find that due to the enhanced density of states in t…
We study the electronic and structural properties of substitutional impurities of graphenelike nanoporous materials C$_2$N, $tg$-, and $hg$-C$_3$N$_4$ by means of density functional theory calculations. We consider four types of impurities; boron substitution on carbon sites (B(C)), carbon substitution on nitrogen sites (C(N)), nitrogen substitution on carbon sites (N(C)), and sulfur substitution on nitrogen sites (S(N)). From cohesive energy calculations, we find that the C(N) and B(C) substitutions are the most energetically favorable and induce small bond modifications in the vicinity of th…
