The electronic transport properties of single layer graphene having a dilute coating of indium adatoms has been investigated. Our studies establish that isolated indium atoms donate electrons to graphene and become a source of charged impurity scattering, affecting the conductivity as well as magnetotransport properties of the pristine graphene. Notably, a positive magnetoresistance is observed over a wide density range after In doping. The low field magnetoresistance carries signatures of quantum interference effects which are significantly altered by the adatoms.
Enhancement of the spin-orbit coupling in graphene may lead to various topological phenomena and also find applications in spintronics. Adatom absorption has been proposed as an effective way to achieve the goal. In particular, great hope has been held for indium in strengthening the spin-orbit coupling and realizing the quantum spin Hall effect. To search for evidence of the spin-orbit coupling in graphene absorbed with indium adatoms, we carry out extensive transport measurements, i.e., weak localization magnetoresistance, quantum Hall effect and non-local spin Hall effect. No signature of t…
Graphene decorated with 5d transitional metal atoms is predicted to exhibit many intriguing properties; for example iridium adatoms are proposed to induce a substantial topological gap in graphene. We extensively investigated the conductivity of single-layer graphene decorated with iridium deposited in ultra-high vacuum at low temperature (7 K) as a function of Ir concentration, carrier density, temperature, and annealing conditions. Our results are consistent with the formation of Ir clusters of ~100 atoms at low temperature, with each cluster donating a single electronic charge to graphene. …
We theoretically study absorption by an undoped graphene layer decorated with arrays of small particles. We discuss periodic and random arrays within a common formalism, which predicts a maximum absorption of $50\%$ for suspended graphene in both cases. The limits of weak and strong scatterers are investigated and an unusual dependence on particle-graphene separation is found and explained in terms of the effective number of contributing evanescent diffraction orders of the array. Our results can be important to boost absorption by single layer graphene due to its simple setup with potential a…
Liquid-based applications of biomolecule-decorated field-effect transistors (FETs) range from biosensors to in vivo implants. A critical scientific challenge is to develop a quantitative understanding of the gating effect of charged biomolecules in ionic solution and how this influences the readout of the FETs. To address this issue, we fabricated protein-decorated graphene FETs and measured their electrical properties, specifically the shift in Dirac voltage, in solutions of varying ionic strength. We found excellent quantitative agreement with a model that accounts for both the graphene pola…
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 electronic transport properties of monolayer graphene have been studied before and after the deposition of a dilute coating of tungsten adatoms on the surface. For coverages up to 2.5\% of a monolayer, we find tungsten adatoms simultaneously donate electrons to graphene and reduce the carrier mobility, impacting the zero- and finite-field transport properties. Two independent transport analyses suggest the adatoms lie nearly 1 nm above the surface. The presence of adatoms is also seen to impact the low field magnetoresistance, altering the signatures of weak localization.
Using typical experimental techniques it is difficult to separate the effects of carrier density and disorder on the superconducting transition in two dimensions. Using a simple fabrication procedure based on metal layer dewetting, we have produced graphene sheets decorated with a non-percolating network of nanoscale tin clusters. These metal clusters both efficiently dope the graphene substrate and induce long-range superconducting correlations. This allows us to study the superconducting transition at fixed disorder and variable carrier concentration. We find that despite structural inhomoge…
Recent experiments reporting unexpectedly large spin Hall effect (SHE) in graphene decorated with adatoms have raised a fierce controversy. We apply numerically exact Kubo and Landauer- Buttiker formulas to realistic models of gold-decorated disordered graphene (including adatom clustering) to obtain the spin Hall conductivity and spin Hall angle, as well as the nonlocal resistance as a quantity accessible to experiments. Large spin Hall angles of 0.1 are obtained at zero-temperature, but their dependence on adatom clustering differs from the predictions of semiclassical transport theories. F…
Realization of the quantum-spin-Hall effect in graphene devices has remained an outstanding challenge dating back to the inception of the field of topological insulators. Graphene's exceptionally weak spin-orbit coupling -stemming from carbon's low mass- poses the primary obstacle. We experimentally and theoretically study artificially enhanced spin-orbit coupling in graphene via random decoration with dilute Bi2Te3 nanoparticles. Remarkably, multi-terminal resistance measurements suggest the presence of helical edge states characteristic of a quantum-spin-Hall phase; the magnetic-field and te…
We showed in past work that nanopatterned monolayer graphene (NPG) enables spectrally selective thermal emission in the mid-infrared (mid-IR) from 3 to 12 $μ$m. In that case the spectral selection is realized by means of the localized surface plasmon (LSP) resonances inside graphene. Here we show that graphene decorated with metallic nanoparticles, such as Ag nanocubes or nanospheres, also realize spectrally selective thermal emission, but in this case by means of acoustic graphene plasmons (AGPs) localized between graphene and the Ag nanoparticle inside a dielectric material. Our finite-diffe…
Interactions of magnetic elements with graphene may lead to various electronic states that have potential applications. We report an in-situ experiment in which the quantum transport properties of graphene are measured with increasing cobalt coverage in continuous ultra-high vacuum environment. The results show that e-beam deposited cobalt forms clusters on the surface of graphene, even at low sample temperatures. Scattering of charge carriers by the absorbed cobalt clusters results in the disappearance of the Shubnikov-de Haas (SdH) oscillations and the appearance of negative magnetoresistanc…
Theoretical predictions and recent experimental results suggest one can engineer spin Hall effect in graphene by enhancing the spin-orbit coupling in the vicinity of an impurity. We use a Chebyshev expansion of the Kubo-Bastin formula to compute the spin conductivity tensor for a tight-binding model of graphene with randomly distributed impurities absorbed on top of carbon atoms. We model the impurity-induced spin-orbit coupling with a graphene-only Hamiltonian that takes into account three different contributions~\cite{Gmitra2013} and show how the spin Hall and longitudinal conductivities dep…
The interplay between electron-electron interaction and electron-phonon coupling has been one of the key issues in graphene as it can provide information on the origin of enhanced electron-phonon coupling in graphene by foreign atoms. In ytterbium-decorated graphene on SiC substrate, electron-phonon coupling exhibits strong enhancement compared to that of as-grown graphene. Based on angle-resolved photoemission study, the presence of ytterbium is also found to result in the decrease of Fermi velocity, revealing the enhancement of electron-electron interaction within the Fermi liquid theory. Ou…
The introduction of spin-orbit interactions (SOIs) and the subsequent appearance of a two-dimensional (2D) topological phase are crucial for voltage-controlled and zero-emission energy spintronic devices. In contrast, graphene basically lacks SOIs due to the small mass of the carbon atom, and appropriate experimental reports for SOIs are rare. Here, we control small-amount (cover ratios < 8%) random decoration of heavy nanoparticles [platinum (Pt) or bismuth telluride (Bi2Te3)] onto mono-layer graphene by developing an original nanoneedle method. X-ray photoelectron spectra support low-damage …
Graphene is a true two dimensional material with exceptional electronic properties and enormous potential for practical applications. Graphene's promise as a chemical sensor material has been noted but there has been relatively little work on practical chemical sensing using graphene, and in particular how chemical functionalization may be used to sensitize graphene to chemical vapors. Here we show one route towards improving the ability of graphene to work as a chemical sensor by using single stranded DNA as a sensitizing agent. The resulting broad response devices show fast response times, c…
We investigate the role of the substrate for the strength of the electon phonon coupling in Li-decorated graphene. We find that the interaction with a $h$-BN substrate leads to a significant enhancement from $λ_0=0.62$ to $λ_1=0.67$, which corresponds to a $25\%$ increase of the transition temperature from $T_{c0}=10.33$ K to $T_{c1}=12.98$ K. The superconducting gaps amount to 1.56 meV (suspended) and 1.98 meV (supported). These findings open up a new route to enhanced superconducting transition temperatures in graphene-based materials by substrate engineering.
The naturally weak spin-orbit coupling in Graphene can be largely enhanced by adatom deposition (e.g. Weeks et al. Phys. Rev. X 1, 021001 (2011)). However, the dynamics of the adatoms also induces a coupling between phonons and the electron spin. Using group theory and a tight-binding model, we systematically investigate the coupling between the low-energy in-plane phonons and the electron spin in single-layer graphene uniformly decorated with heavy adatoms. Our results provide the foundation for future investigations of spin transport and superconductivity in this system. In order to quantify…
Based on first principles calculation, the electronic properties of graphene on metal (Ti, Ca, Ni, Mn, Co, Fe, Cr, K) modified SiO2 substrate have been studied. The results of binding energies supported graphene indicate that the metal atoms are adsorbed more stably on O surface than on Si surface of SiO2 substrate, and graphene is adsorbed very stably on metal modified substrate. The band structures of supported graphene are similar with that of suspending graphene when deposited on Co modified SiO2 surface, but change obviously with the effect of decorated Fe atoms. Interesting, a semi-metal…
We present here the results on superconducting properties in tantalum thin films (100nm thick) deposited on three-dimensional graphene (3DG) and carbon structures. A superconducting transition is observed in both composite thin films with a superconducting transition temperature of 1.2K and 1.0K, respectively. We have further measured the magnetoresistance at various temperatures and differential resistance dV/dI at different magnetic fields in these two composite thin films. In both samples, a much large critical magnetic field (~ 2 Tesla) is observed and this critical magnetic field shows li…
We present a two-band model based on periodic Hückel theory, which is capable of predicting the existence and position of Dirac cones in the first Brillouin zone of an infinite class of two-dimensional periodic carbon networks, obtained by systematic perturbation of the graphene connectivity by bond decoration, that is by inclusion of arbitrary $π$-electron Hückel networks into each of the three carbon-carbon $π$-bonds within the graphene unit cell. The bond decoration process can fundamentally modify the graphene unit cell and honeycomb connectivity, representing a simple and general way to d…
The phase diagram of graphene decorated with magnetic adatoms distributed either on a single sublattice, or evenly over the two sublattices, is computed for adatom concentrations as low as $\sim1\%$. Within the framework of the $s$-$d$ interaction, we take into account disorder effects due to the random positioning of the adatoms and/or to the thermal fluctuations in the direction of magnetic moments. Despite the presence of disorder, the magnetic phases are shown to be stable down to the lowest concentration accessed here. This result agrees with several experimental observations where adatom…
Guanine-quadruplex, consisting of several stacked guanine-quartets (GQs), has emerged as an important category of novel molecular targets with applications from nanoelectronic devices to anticancer drugs. Incorporation of metal cations into GQ structure is utilized to form stable G-quadruplexes, while no other passage has been reported yet. Here we report the room temperature (RT) molecular self-assembly of extensive metal-free GQ networks on Au(111) surface. Surface defect induced by an implanted molybdenum atom within Au(111) surface is used to nucleate and stabilize the cation-free GQ netwo…
Here, we examine the influence of surface chemical reactivity toward ambient gases on the performance of nanodevices based on two-dimensional materials "beyond graphene" and novel topological phases of matter. While surface oxidation in ambient conditions was observed for silicene and phosphorene with subsequent reduction of the mobility of charge carriers, nanodevices with active channels of indium selenide, bismuth chalcogenides and transition-metal dichalcogenides are stable in air. However, air-exposed indium selenide suffers of p-type doping due to water decomposition on Se vacancies, whe…
Wrinkles in monolayer graphene (GN) affect the GN electronic and transport properties. Defined network of wrinkles can be reached by placing the GN on the substrate decorated with the nanoparticles (NPs). In order to explain mechanism behind the topographically induced changes of the GN electronic structure and to correlate it with the wrinkling, correct description of the GN morphology is of high demand. We demonstrate here how to determine from the atomic force microscopy (AFM) images whether the GN is in the contact with the substrate or it is delaminated, how is the wrinkling of the layer …
Graphene is considered a promising candidate to replace conventional transparent conductors due to its low opacity, high carrier mobility and flexible structure. Multi-layer graphene or stacked single layer graphenes have been investigated in the past but both have their drawbacks. The uniformity of multi-layer graphene is still questionable, and single layer graphene stacks require many transfer processes to achieve sufficiently low sheet resistance. In this work, bilayer graphene film grown with low pressure chemical vapor deposition was used as a transparent conductor for the first time. Th…
We have performed density functional theory calculations of graphene decorated with carbon adatoms, which bind at the bridge site of a C--C bond. Earlier studies have shown that the C adatoms have magnetic moments and have suggested the possibility of ferromagnetism with high Curie temperature. Here we propose to use a gate voltage to fine tune the magnetic moments from zero to 1$μ_B$ while changing the magnetic coupling from antiferromagnetism to ferromagnetism and again to antiferromagnetism. These results are rationalized within the Stoner and RKKY models. When the SCAN meta-GGA correction …
Adatom-decorated graphene offers a promising new path towards spintronics in the ultrathin limit. We combine experiment and theory to investigate the electronic properties of dilutely fluorinated bilayer graphene, where the fluorine adatoms covalently bond to the top graphene layer. We show that fluorine adatoms give rise to resonant impurity states near the charge neutrality point of the bilayer, leading to strong scattering of charge carriers and hopping conduction inside a field-induced band gap. Remarkably, the application of an electric field across the layers is shown to tune the resonan…
We study the charge and spin transport in a two terminal graphene nanoribbon (GNR) decorated with random Gold (Au) adatoms using a Kane-Mele model. Two commonly used GNRs, that is, the armchair graphene nanoribbon (AGNR) and the zigzag graphene nanoribbon (ZGNR) are compared and contrasted, which shows that in presence of Au adatoms, a somewhat robust $2e^2/h$ conductance plateau occurs in the case of AGNR around the zero of the Fermi energy, while in ZGNR this plateau is fragile. We show that this flat plateau, having a conductance value $2e^2/h$, is not a hallmark signature of a topologicall…
Following the recent proposal by Weeks et al., which suggested that indium (or thallium) adatoms deposited on the surface of graphene should turn the latter into a quantum spin Hall (QSH) insulator characterized by a sizeable gap, we perform a systematic study of the transport properties of this system as a function of the density of randomly distributed adatoms. While the samples are, by construction, very disordered, we find that they exhibit an extremely stable QSH phase with no signature of the spatial inhomogeneities of the adatom configuration. We find that a simple rescaling of the spin…
The decoration of graphene samples with adatoms or nanoparticles leads to the enhancement of spin-orbit interactions as well as to the introduction of symmetry-breaking effects that could have drastic effects on spin and electronic transport phenomena. We present an analysis based on symmetry considerations and examine the impact on the scattering matrix for graphene systems containing defects that enhance spin-orbit interactions, while conserving the electronic total angular momentum. We show that the appearance and dominance of skew scattering, and the related observation of valley and/or sp…
The two inequivalent valleys in graphene preclude the protection against inter-valley scattering offered by an odd-number of Dirac cones characteristic of Z2 topological insulator phases. Here we propose a way to engineer a chiral single-valley metallic phase with quadratic crossover in a honeycomb lattice through tailored \sqrt{3}N *\sqrt{3}N or 3N *3N superlattices. The possibility of tuning valley-polarization via pseudo-Zeeman field and the emergence of Dresselhaus-type valley-orbit coupling are proposed in adatom decorated graphene superlattices. Such valley manipulation mechanisms and me…
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 2007 discovery of quantized conductance in HgTe quantum wells delivered the field of topological insulators (TIs) its first experimental confirmation. While many three-dimensional TIs have since been identified, HgTe remains the only known two-dimensional system in this class. Difficulty fabricating HgTe quantum wells has, moreover, hampered their widespread use. With the goal of breaking this logjam we provide a blueprint for stabilizing a robust TI state in a more readily available two-dimensional material---graphene. Using symmetry arguments, density functional theory, and tight-binding…
We study the charge and spin transport in two and four terminal graphene nanoribbons (GNR) decorated with random distribution of magnetic adatoms. The inclusion of the magnetic adatoms generates only the $z$-component of the spin polarized conductance via an exchange bias in the absence of Rashba spin-orbit interaction (SOI), while in presence of Rashba SOI, one is able to create all the three ($x$, $y$ and $z$) components. This has important consequences for possible spintronic applications. The charge conductance shows interesting behaviour near the zero of the Fermi energy. Where in presenc…
Graphene has been used recently as a replacement for indium tin oxide (ITO) for the transparent electrode of an organic photovoltaic device. Due to its limited supply, ITO is considered as a limiting factor for the commercialization of organic solar cells. We explored the use of large-area graphene grown on copper by chemical vapor deposition (CVD) and then transferred to a glass substrate as an alternative transparent electrode. The transferred film was shown by scanning Raman spectroscopy measurements to consist of >90% single layer graphene. Optical spectroscopy measurements showed that the…
Graphene has recently been shown to be permeable to thermal protons, the nuclei of hydrogen atoms, which sparked interest in its use as a proton-conducting membrane in relevant technologies. However, the influence of light on proton permeation remains unknown. Here we report that proton transport through Pt-nanoparticle-decorated graphene can be enhanced strongly by illuminating it with visible light. Using electrical measurements and mass spectrometry, we find a photoresponsivity of 10^4 A W-1, which translates into a gain of 10^4 protons per photon with response times in the microsecond rang…
'Magic'-angle twisted bilayer graphene has received a lot of interest due to its flat bands with potentially non-trivial topology that lead to intricate correlated phases. A spectrum with flat bands, however, does not require a twist between multiple sheets of van der Waals materials, but rather can be realized with the application of an appropriate periodic potential. Here, we propose the imposition of a tailored periodic potential onto a single graphene layer through local perturbations that could be created via lithography or adatom manipulation, which also results in an energy spectrum fea…
In this work a simple approach to transform MoS$_2$ from its metallic (1T' to semiconductor 2H) character via gold nanoparticle surface decoration of a MoS$_2$ graphene oxide (rGO) nanocomposite is proposed. The possible mechanism to this phase transformation was investigated using different spectroscopy techniques, and supported by density functional theory theoretical calculations. A mixture of the 1T'- and 2H-MoS2 phases was observed from the Raman and Mo 3d High Resolution X-ray photoelectron (HRXPS) spectra analysis in the MoS$_2$-rGO nanocomposite. After surface decoration with gold nano…
We study the spectral function and quasiparticle scattering in Li-decorated graphene (Li@graphene) with an atomistic $T$-matrix formalism and uncover adatom-induced spectral effects which shed light on experimentally observed angle-resolved photoemission spectroscopy (ARPES) features. From transport studies, alkali adatoms are known to introduce charged-impurity scattering limiting the carrier mobility. Here, we demonstrate that Li adatoms furthermore give rise to a low-energy impurity band centered at the $Γ$ point which originates from the hybridization between the atomic 2s state of the Li …
By ab initio calculation, Au, Cu, Fe, Ni and Pt adatoms were proposed for modulating the electronic property of graphdiyne naoribbons (GDNRs). GDNRs of 1~4 nm in width were found to be stable at room temperature, and the thermal rates of Au, Cu, Fe, Ni and Pt adatoms escaping from GDNR are slower than 0.003 atoms per hour even at 900 K. According to the calculation, Au and Cu-decorated GDNRs are metallic with carrier concentrations close to that of graphene at room temperature, while Fe, Ni and Pt-decorated GDNRs are n-type semiconductors with impurity states below Fermi energy. Heterojunction…
