Spin-orbit coupling (SOC) can provide essential tools to manipulate electron spins in two-dimensional materials like graphene, which is of great interest for both fundamental physics and spintronics application. In this paper, we report the low-field magnetotransport of in situ hydrogenated graphene where hydrogen atoms are attached to the graphene surface in continuous low temperature and vacuum environment. Transition from weak localization to weak antilocalization with increasing hydrogen adatom density is observed, indicating enhancing Bychkov-Rashba-type SOC in a mirror symmetry broken system. From the low-temperature saturation of phase breaking scattering rate, the existence of spin-flip scattering is identified, which corroborates the existence of magnetic moments in hydrogenated graphene.
We calculate the spin transport of hydrogenated graphene using the Landauer-Büttiker formalism with a spin-dependent tight-binding Hamiltonian. The advantages of using this method is that it simultaneously gives information on sheet resistance and localization length as well as spin relaxation length. Furthermore, the Landauer-Büttiker formula can be computed very efficiently using the recursive Green's function technique. Previous theoretical results on spin relaxation time in hydrogenated graphene have not been in agreement with experiments. Here, we study magnetic defects in graphene with r…
In this work we present a fully atomistic reactive (ReaxFF force field) molecular dynamics study of the structural and dynamical aspects of the one-side hydrogenation of graphene membranes, leading to the formation of the so-called graphone structure. We have considered different substrates: graphene, few-layers graphene, graphite and platinum at different temperatures. Our results showed that the hydrogenation rates are very dependent on the substrate and thermal effects. Our results also showed that, similarly to graphane, large hydrogenated domains are unlikely to be formed. These hydrogena…
Conventional in-gap Yu-Shiba-Rusinov states require two ingredients: magnetic atoms and a superconducting host that, in the normal phase, has a finite density of states at the Fermi energy. Here we show that hydrogenated graphene can host Yu-Shiba-Rusinov states without any of those two ingredients. Atomic hydrogen chemisorbed in graphene is known to act as paramagnetic center with a weakly localized magnetic moment. Our calculations for hydrogenated graphene in proximity to a superconductor show that individual adatoms induce in-gap Yu-Shiba-Rusinov states with an exotic spectrum whereas chai…
The weak spin-orbit interaction in graphene was predicted to be increased, e.g., by hydrogenation. This should result in a sizable spin Hall effect (SHE). We employ two different methods to examine the spin Hall effect in weakly hydrogenated graphene. For hydrogenation we expose graphene to a hydrogen plasma and use Raman spectroscopy to characterize this method. We then investigate the SHE of hydrogenated graphene in the H-bar method and by direct measurements of the inverse SHE. Although a large nonlocal resistance can be observed in the H-bar structure, comparison with the results of the ot…
We report the observation of a giant positive magnetoresistance in millimetre scale hydrogenated graphene with magnetic field oriented in the plane of the graphene sheet. A positive magnetoresistance in excess of 200\% at a temperature of 300 mK was observed in this configuration, reverting to negative magnetoresistance with the magnetic field oriented normal to the graphene plane. We attribute the observed positive, in-plane, magnetoresistance to Pauli-blockade of hopping conduction induced by spin polarization. Our work shows that spin polarization in concert with electron-electron interacti…
We calculate the spin-dependent zero-bias conductance $G_{σσ'}$ in armchair graphene nanoribbons with hydrogen adsorbates employing a DFT-based ab initio transport formalism including spin-orbit interaction. We find that the spin-flip conductance $G_{σ\barσ}$ can reach the same order of magnitude as the spin-conserving one, $G_{σσ}$, due to exchange-mediated spin scattering. In contrast, the genuine spin-orbit interaction appears to play a secondary role, only.
A lot of efforts have been devoted to understanding the origin and effects of magnetic moments induced in graphene with carbon atom vacancy, or light adatoms like hydrogen or fluorine. At the meantime, the large negative magnetoresistance (MR) widely observed in these systems is not well understood, nor had it been associated with the presence of magnetic moments. In this paper, we study the systematic evolution of the large negative MR of in-situ hydrogenated graphene in ultra-high vacuum (UHV) environment. We find for most combination of electron density ($n_e$) and hydrogen density ($n_H$),…
We show that the $d^{0}$ ferromagnetism with high Curie temperature ($T_c$) can be achieved in the electron doped hydrogenated epitaxial graphene on some certain SiC substrates through first-principles calculations. The pristine systems are found to be a Mott insulator independent of SiC polytypes (2$H$, 4$H$ or 6$H$) which, however, play a significant role in the modulation of magnetic interaction. Carrier doping enhances the ferromagnetic coupling due to the double exchange mechanism and thus realizes the phase transition from antiferromagnetism to ferromagnetism. A $T_c$ of around 400 K is …
Geometry, stability, and thermal transport of graphene nanoquilts folded by hydrogenation are studied using molecular dynamics simulations. The hydrogenated graphene nanoquilts show increased thermodynamic stability and better transport properties than folded graphene structures without hydrogenation. For the two-fold graphene nanoquilt, both geometry and thermal conductivity are very sensitive to the adsorbed hydrogen chains, which is interpreted by the red-shift of PDOS. For the multi-fold nanoquilts, their thermal conductivities can be tuned from 100% to 15% of pristine graphene, by varying…
We present a theoretical study of spin-velocity injection (SVI) of a pure spin current (PSC) induced by a linearly polarized light that impinges normally on the surface of two 50\% hydrogenated noncentrosymmetric two-dimensional (2D) graphene structures. The first structure, hydrogenated at only one side, labeled Up, also known as graphone, and the second, labelled Alt, is 25\% hydrogenated at both sides. The hydrogenation opens an energy gap in both structures. We analyze two possibilities: in the first, the spin is fixed along a chosen direction, and the resulting SVI is calculated; in the s…
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 …
Charge doping induced phase transitions in hydrogenated and fluorinated graphene
我们发现，电荷掺杂可以诱导氢化和氟化石墨烯中三种不同的吸附物相之间的转变。通过结合从头算，近似密度泛函理论和紧束缚计算，我们确定了过渡从岛的C $_8$ H $_2$和C $_8$ F $_2$的随机吸附分布周围的掺杂水平$\pm 0.05$ e/C-原子。此外，在具有随机吸附物覆盖的情况下，电荷掺杂被示出为触发有序转变，其中当掺杂水平超过吸附物浓度时，亚晶格对称性自发地被破坏。再杂化能和晶格畸变能使得仅从一侧共价官能化的石墨烯最容易发生这两种相变。与聚集和有序转变相关的能量增益超过室温热能。
Motivated by recent experimental and calculational investigations of bilayer, hydrogenated and fluorinated graphene, we apply the formalisms of U(1) QED (quantum electrodynamics) and SU(2) QCD (quantum chromodynamics) theories of strongly correlated state. Unlike non-bipartite triangular lattice, on bipartite honeycomb lattice there always exists a monopole that transforms trivially under all the microscopic symmetries, destabilizing the Dirac spin liquid (DSL), so that one can continuously tune the DSL state to the state with parent SU(2) instead of U(1) gauge group. The SU(2) theory describe…
We describe a mechanism that explains the formation of hydrocarbons and hydrocarbyls from hydrogenated graphene/graphite; hard C-C bonds are weakened and broken by the synergistic effect of chemisorbed hydrogen and high temperature vibrations. Total energies, optimized structures, and transition states are obtained from Density Functional Theory simulations. These values have been used to determine the Boltzman probability for a thermal fluctuation to overcome the kinetic barriers, yielding the time scale for an event to occur. This mechanism can be used to rationalize the possible routes for …
Using helium-3 atom scattering, we have studied the adsorption kinetics, the structure and the diffusional dynamics of atomic hydrogen on the surface of a graphene monolayer on Ni(111). Diffraction measurements reveal a 4$^\circ$ rotated rectangular hydrogen overstructure. Hydrogen adsorption and desorption exhibit activation barriers of $E_a=(89\pm7)\,$meV and $E_d=(1.8\pm0.2)\,$eV, respectively. Helium-3 spin-echo measurements showed no decay of the spatial correlation function (or intermediate scattering function) within the time range of the spectrometer. Hence, we are able to set lower li…
Electron correlation effects caused by the topological zero mode of a hydrogenated graphene vacancy, $V_{111}$, with three adsorbed hydrogen atoms is discussed theoretically. A Kondo model is derived from the multi-reference representation of the density functional theory, where exchange scattering processes between the zero mode and low-energy modes in the Dirac cones are estimated. Even when the Dirac cone is slightly off from the charge neutral point, a finite on-site correlation energy, $U_0$, for the zero mode of an isolated $V_{111}$ allows the half-filling of the localized level giving …
The effects of tensile strain on the current-voltage (I-V) characteristics of hydrogenated-edge armchair graphene nanoribbons (HAGNRs) are investigated by using DFT theory. The strain is introduced in two different ways related to the two types of systems studied in this work: in-plane strained systems (A), and out-of-plane strained systems due to bending (B). These two kinds of strain lead to make a distinction among three cases: in-plane strained systems with strained electrodes (A1) and with unstrained electrodes (A2), and out-of-plane homogeneously strained systems with unstrained, fixed e…
Graphene nanoribbons' electronic transport properties strongly depend on the type of edge, armchair, zigzag or other, and on edge functionalization that can be used for band-gap engineering. For only partly hydrogenated edges interesting magnetic properties are predicted. Electric charge accumulates at edges and corners. Scanning force microscopy has so far shown the centre of graphene nanoribbons with atomic resolution using a quartz crystal tuning fork sensor of high stiffness. Weak long-range electrostatic forces related to the charge accumulation on the edges of graphene nanoribbons could …
In the paper a theoretical study of critical (Curie) temperature of diluted ferromagnet based on multilayer graphene (or graphite) with hydrogen adatoms deposited over carbon atoms belonging to single sublattice is presented. The calculations are performed within Pair Approximation (PA) for diluted ferromagnetic system with long-range interactions. The method is able to take into account the spin-space anisotropy of coupling. The results obtained within Mean Field Approximation (MFA) are also presented for comparison. The assumed interaction between hydrogen adatom spins is inversely proportio…
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…
We report on theoretical investigations of the spin-orbit coupling effects in fluorinated graphene. First-principles density functional calculations are performed for the dense and dilute adatom coverage limits. The dense limit is represented by the single-side semifluorinated graphene, which is a metal with spin-orbit splittings of about 10 meV. To simulate the effects of a single adatom, we also calculate the electronic structure of a $10 \times 10$ supercell, with one fluorine atom in the top position. Since this dilute limit is useful to study spin transport and spin relaxation, we also in…
Graphene functionalization by hydrogen and fluorine has been proposed as a route to modulate its reactivity and electronic properties. However, until now, proposed systems present degradation and limited hydrogen adsorption capacity. In this study, combining first-principles calculations based on density functional theory (DFT) and reactive molecular dynamics, we analyze the tuning of hydrogen adsorption and electronic properties in fluorinated and hydrogenated monolayer graphenes. Our results indicate that fluorine adsorption promotes stronger carbon$-$hydrogen bonds. By changing the concentr…
We study the band gap of finite $N_A=7$ armchair graphene nanoribbons (7-AGNRs) on Au(111) through scanning tunneling microscopy/spectroscopy combined with density functional theory calculations. The band gap of 7-AGNRs with lengths of 6 nm and more is converged to within 0.1 eV of its bulk value of 2.3 eV, while the band gap opens by several hundred meV in very short 7-AGNRs. The termination has a significant effect on the band gap, doubly hydrogenated termini yielding a lower band gap than singly hydrogenated ones.
A method of regulating spin dynamics of the so-called magnetic graphene is analyzed. Magnetic moments can be incorporated into graphene flakes and graphene ribbons through defects, such as adatoms and vacancies. Local spins can also be attached to graphene at hydrogenated zigzag edges. Spin flips can be produced by transverse pulses and by connecting the sample to a resonance electric coil. The action of the resonator feedback field strongly accelerates spin reversal. The possibility of fast spin reversal is important for spintronics and for quantum information processing allowing for an effic…
We perform a comparative study of the spin relaxation by spin-orbit coupling induced from adatoms (hydrogen and fluorine) in graphene. Two methods are applied, giving consistent results: a full quantum transport simulation of a graphene nanoribbon, and a T-matrix calculation using Green's functions for a single adatom in graphene. For hydrogenated graphene the dominant spin-orbit term for spin relaxation is PIA, the hitherto neglected interaction due to pseudospin inversion asymmetry. In contrast, in fluorinated graphene PIA and Rashba couplings destructively interfere, reducing the total spin…
