We study the effects of metallic doping on the electronic properties of graphene using density functional theory in the local density approximation in the presence of a local charging energy (LDA+U). The electronic properties are sensitive to whether graphene is doped with alkali or transition metals. We estimate the the charge transfer from a single layer of Potassium on top of graphene in terms of the local charging energy of the graphene sheet. The coating of graphene with a non-magnetic layer of Palladium, on the other hand, can lead to a magnetic instability in coated graphene due to the hybridization between the transition-metal and the carbon orbitals.
The synthesis, physical, photocatalytic, and antibacterial properties of MgO and graphene nanoplatelets (GNPs) nanocomposites are reported. The crystallinity, phase, morphology, chemical bonding, and vibrational modes of prepared nanomaterials are studied. The conductive nature of GNPs is tailored via photocatalysis and enhanced antibacterial activity. It is interestingly observed that the MgO/GNPs nanocomposite with optimized GNPs content show a significant photocatalytic activity (97.23% degradation) as compared to bare MgO (43%) which makes it the potential photocatalyst for purification of…
In two-dimensional van der Waals (vdWs) materials, the relative twist angle between adjacent layers not only controls their electronic properties, but also determines their stacking energy. This effect makes it much easier to realize energetically favorable configurations of the vdWs materials, for example, Bernal-stacked structure of bilayer graphene. Here we demonstrate that we can controllably tailor adhesive energy landscape of graphene nanostructures on graphene and stabilize the system with tunable twist angle by using a one-dimensional tilt grain boundary (GB). The area ratio with diffe…
Contrary to most materials, graphene exhibits a negative thermal expansion coefficient (TEC), i.e it contracts when heated. This contraction is due to the thermal excitation of low energy out-of-plane vibration modes. These flexural modes have been reported to govern the electronic transport and the mechanical response of suspended graphene. In this work, we systematically investigate the influence of defects in the TEC of suspended graphene membranes. Controlled introduction of low densities of mono-vacancies reduces the graphene TEC, up to one order of magnitude for a defect density of $5\ti…
We investigate the growth of the graphene buffer layer and the involved step bunching behavior of the silicon carbide substrate surface using atomic force microscopy. The formation of local buffer layer domains are identified to be the origin of undesirably high step edges in excellent agreement with the predictions of a general model of step dynamics. The applied polymer-assisted sublimation growth method demonstrates that the key principle to suppress this behavior is the uniform nucleation of the buffer layer. In this way, the silicon carbide surface is stabilized such that ultra-flat surfa…
We propose a theoretical approach to quantitatively determine the photothermally driven enhancement of molecular mobility of graphene-indomethacin mixtures under infrared laser irradiation. Graphene plasmons absorb incident electromagnetic energy and dissipate them into heat. The absorbed energy depends on optical properties of graphene plasmons, which are sensitive to structural parameters, and concentration of plasmonic nanostructures. By using theoretical model, we calculate temperature gradients of the bulk drug with different concentrations of graphene plasmons. From these, we determine t…
Integration of two-dimensional (2D) van der Waals (vdWs) materials with non-2D materials to realize mixed-dimensional heterostructures has potential for creating functional devices beyond the reach of existing materials and has long been a pursuit of the material science community. Here we report the patterning of monolayer/bilayer transition metal dichalcogenide (TMD) nanostructures with nanometer-precision, tunable sizes and sites at interfaces of graphene/TMD heterostructures. Our experiments demonstrate that the TMD nanostructures can be created at selected positions of the interface using…
Graphene offers a possibility for actively controlling plasmon confinement and propagation by tailoring its spatial conductivity pattern. However, implementation of this concept has been hampered because uncontrollable plasmon reflection is easily induced by inhomogeneous dielectric environment. In this work, we demonstrate full electrical control of plasmon reflection/transmission at electronic boundaries induced by a zinc-oxide-based dual gate, which is designed to minimize the dielectric modulation. Using Fourier-transform infrared spectroscopy, we show that the plasmon reflection can be va…
The possibility to make 10 nm scale, and low-disorder, suspended graphene devices would open up many possibilities to study and make use of strongly coupled quantum electronics, quantum mechanics, and optics. We present a versatile method, based on the electromigration of gold-on-graphene bow-tie bridges, to fabricate low-disorder suspended graphene junctions and quantum dots with lengths ranging from 6 nm up to 55 nm. We control the length of the junctions, and shape of their gold contacts by adjusting the power at which the electromigration process is allowed to avalanche. Using carefully en…
The long spin-diffusion length, spin-lifetimes and excellent optical absorption coefficient of graphene provide an excellent platform for building opto-electronic devices as well as spin-based logic in a nanometer regime. In this study, by employing density functional theory and its time-dependent version, we provide a detailed analysis of how the size and shape of graphene nanoflakes can be used to alter their magnetic structure and optical properties. As the edges of zigzag graphene nanoribbons are known to align anti-ferromagnetically and armchair nanoribbons are typically non-magnetic, a c…
A variety of novel quantum phases have been achieved in twist bilayer graphene (tBLG) and other moire superlattices recently, including correlated insulators, superconductivity, magnetism, and topological states. These phenomena are very sensitive to the moire superlattices, which can hardly be changed rapidly or intensely. Here, we report the experimental realization of a high-order moire pattern (a high-order interference pattern) in graphene-monolayer xenon heterostructure (G/mXe), with moire period in-situ tuned from few nanometers to infinity by changing the lattice constant of Xe through…
We report a systematic first-principles investigation of the influence of different magnetic insulators on the magnetic proximity effect induced in graphene. Four different magnetic insulators are considered: two ferromagnetic europium chalcogenides namely EuO and EuS and two ferrimagnetic insulators yttrium iron garnet (YIG) and cobalt ferrite (CFO). The obtained exchange-splitting varies from tens to hundreds of meV. We also find an electron doping induced by YIG and europium chalcogenides substrates, that shift the Fermi level up to 0.78 eV and 1.3 eV respectively, whereas hole doping up to…
Graphene-based materials (GBMs) constitute a large family of materials which has attracted great interest for potential applications. In this work, we apply first-principles calculations based on density functional theory (DFT) and fully atomistic reactive molecular dynamics (MD) simulations to study the structural and electronic effects of hydrogenation in Me-graphene, a non-zero bandgap GBM composed of both $sp^2$ and $sp^3$-hybridized carbon. Our DFT results show a substantial tuning of the electronic properties of Me-graphene by hydrogenation, with the bandgap varying from $0.64$ eV to $2.…
There are a number of theoretical proposals based on strain engineering of graphene and other two-dimensional materials, however purely mechanical control of strain fields in these systems has remained a major challenge. The two approaches mostly used so far either couple the electrical and mechanical properties of the system simultaneously or introduce some unwanted disturbances due to the substrate. Here, we report on silicon micro-machined comb-drive actuators to controllably and reproducibly induce strain in a suspended graphene sheet, in an entirely mechanical way. We use spatially resolv…
Our First-principles Full-Potential Density Functional Theory (DFT) calculations show that a monolayer of ZnS (ML-ZnS), which is predicted to adopt a graphene-like planar honeycomb structure with a direct band gap, undergoes strain-induced modifications in its structure and band gap when subjected to in-plane homogeneous biaxial strain ($δ$). ML-ZnS gets buckled for compressive strain greater than 0.92%; the buckling parameter $Δ$ (= 0.00 Å\, for planar ML-ZnS) linearly increases with increasing compressive strain ($Δ= 0.435$ Å\,at $δ= - 5.25$%). A tensile strain of 2.91% turns the direct band…
High quality epitaxial graphene films can be applied as templates for tailoring graphene-substrate interfaces that allow for precise control of the charge carrier behavior in graphene through doping and many-body effects. By combining scanning tunneling microscopy, angle-resolved photoemission spectroscopy and density functional theory we demonstrate that oxygen intercalated epitaxial graphene on Ir(111) has high structural quality, is quasi free-standing, and shows signatures of many-body interactions. Using this system as a template, we show that tunable pn-junctions can be patterned by adso…
Three dimensional topological insulator crystals consist of an insulating bulk enclosed by metallic surfaces, and detailed theoretical predictions about the surface state band topology and spin texture are available. While several topological insulator materials are currently known, the existence and topology of these metallic states have only ever been probed for one particular surface orientation of a given material. For most topological insulators, such as Bi$_{1-x}$Sb$_{x}$ and Bi$_2$Se$_3$, this surface is the closed-packed (111) surface and it supports one topologically guaranteed surfac…
We report on the electronic structure of $α$-Sn films in the very low thickness regime grown on InSb(111)A. High-resolution low photon energies angle-resolved photoemission (ARPES) allows for the direct observation of the linearly dispersing 2D topological surface states (TSSs) that exist between the second valence band and the conduction band. The Dirac point of this TSS was found to be 200meV below the Fermi level in 10-nm-thick $α$-Sn films, which enables the observation of the hybridization gap opening at the Dirac point of the TSS for thinner films. The crossover to a quasi-2D electronic …
Kirigami structure, from the macro- to the nanoscale, exhibits distinct and tunable properties from original 2-dimensional sheet by tailoring. In present work, the extreme reduction of the thermal conductivity by tailoring sizes in graphene nanoribbon kirigami (GNR-k) is demonstrated using nonequilibrium molecular dynamics simulations. The results show that the thermal conductivity of GNR-k (around 5.1 Wm-1K-1) is about two orders of magnitude lower than that of the pristine graphene nanoribbon (GNR) (around 151.6 Wm-1K-1), while the minimum value is expected to be approaching zero in extreme …
Polaritons in polar biaxial crystals with extreme anisotropy offer a promising route to manipulate nanoscale light-matter interactions. The dynamical modulation of their dispersion is great significance for future integrated nano-optics but remains challenging. Here, we report a momentum-directed strategy, a coupling between the modes with extra momentum supported by the interface and in-plane hyperbolic polaritons, to tailor topological transitions of anisotropic polaritons in biaxial crystals. We experimentally demonstrate such tailored polaritons at the interface of heterostructures between…
We have demonstrated that the island nucleation in the initial stage of epitaxial thin film growth can be tuned by substrate surface charge doping. This charge effect was investigated using spin density functional theory calculation in Fe-deposition on graphene substrate as an example. It was found that hole-doping can apparently increase both Fe-adatom diffusion barrier and Fe inter-adatom repulsion energy occurring at intermediate separation, whereas electron-doping can decrease Fe-adatom diffusion barrier but only slightly modify inter-adatom repulsion energy. Further kinetic Monte Carlo si…
The electronic and optical properties of graphene can be precisely tuned by generating deterministic arrangements of strain features. In this paper, we report the formation of widespread and controlled buckling delamination of monolayer graphene deposited on hexagonal boron-nitride promoted by a significant squeezing of the graphene flake and induced by polymeric micro-actuators. The flexibility of this method offers a promising technique to create arbitrary buckling geometries and arrays of wrinkles which could also be subjected to iterative folding-unfolding cycles. Further development of th…
Topological band theory provides a conceptual framework to predict or even engineer robust metallic states at the boundaries of topologically distinct phases. The bulk-boundary correspondence requires that a topological electronic phase transition between two insulators must proceed via closing of the electronic gap. Therefore, it can provide a conceptual solution to the instability of metallic phases in π-conjugated 1D polymers. In this work we predict and demonstrate that a clever design and on-surface synthesis of polymers consisting of 1D linearly bridged polyacene moieties, can position t…
Control of nucleation sites is an important goal in materials growth: nuclei in regular arrays may show emergent photonic or electronic behavior, and once the nuclei coalesce into thin films, the nucleation density influences parameters such as surface roughness, stress, and grain boundary structure. Tailoring substrate properties to control nucleation is therefore a powerful tool for designing functional thin films and nanomaterials. Here, we examine nucleation control for metals deposited on two-dimensional (2D) materials in a situation where substrate effects are absent and heterogeneous nu…
Controlling magnetism of transition metal atoms by pairing with $π$ electronic states of graphene is intriguing. Herein, through first - principle computation we explore the possibility of switching magnetization by forming the tetrahedral $sp^3$ - metallic $d$ hybrid bonds. Graphene multilayers capped by single - layer cobalt atoms can transform into the $sp^3$ - bonded diamond films upon the hydrogenation of the bottom surface. While the conversion is favored by hybridization between the $sp^3$ dangling bonds and metallic $d_{z^2}$ states, such a strong hybridization can lead to the reorient…
Lateral heterostructures of two-dimensional materials may exhibit various intriguing emergent properties. Yet when specified to the orientationally aligned heterojunctions of zigzag graphene and hexagonal boron nitride (hBN) nanoribbons, realizations of the high expectations on their properties encounter two standing hurtles. First, the rapid accumulation of strain energy prevents large- scale fabrication. Secondly, the pronounced half-metallicity predicted for freestanding graphene nanoribbons is severely suppressed. By properly tailoring orientational misalignment between zigzag graphene and…
Proximity-induced fine features and spin-textures of the electronic bands in graphene-based van der Waals heterostructures can be explored from the point of tailoring a twist angle. Here we study spin-orbit coupling and exchange coupling engineering of graphene states in the proximity of 1T-TaS$_2$ not triggering the twist, but a charge density wave in 1T-TaS$_2$-a realistic low-temperature phase. Using density functional theory and effective model we found that the emergence of the charge density wave in 1T-TaS$_2$ significantly enhances Rashba spin-orbit splitting in graphene and tilts the s…
Combining atomically-thin van der Waals materials into heterostructures provides a powerful path towards the creation of designer electronic devices. The interaction strength between neighboring layers, most easily controlled through their interlayer separation, can have significant influence on the electronic properties of these composite materials. Here, we demonstrate unprecedented control over interlayer interactions by locally modifying the interlayer separation between graphene and boron nitride, which we achieve by applying pressure with a scanning tunneling microscopy tip. For the spec…
We report on the magnetic and structural properties of ferromagnetic-insulating La$_2$CoMnO$_6$ thin films grown on top of (001) STO substrates by means of RF sputtering technique. Careful structural analysis, by using synchrotron X-ray diffraction, allows identifying two different crystallographic orientations that are closely related to oxygen stoichiometry and to the features (coercive fields and remanence) of the hysteresis loops. Both Curie temperature and magnetic hysteresis turn out to be dependent on the oxygen stoichiometry. In situ annealing conditions allow tailoring the oxygen cont…
Intercalation is an established technique for tailoring the electronic structure of epitaxial graphene. Moreover, it enables the synthesis of otherwise unstable two-dimensional (2D) layers of elements with unique physical properties compared to their bulk versions due to interfacial quantum confinement. In this work, we present uniformly Pb-intercalated quasi-freestanding monolayer graphene on SiC, which turns out to be essentially charge neutral with an unprecedented $p$-type carrier density of only $(5.5\pm2.5)\times10^9$ cm$^{-2}$. Probing the low-energy electronic structure throughout the …
The electronic implications of strain in graphene can be captured at low energies by means of pseudovector potentials which can give rise to pseudomagnetic fields. These strain-induced vector potentials arise from the local perturbation to the electronic hopping amplitudes in a tight-binding framework. Here we complete the standard description of the strain-induced vector potential, which accounts only for the hopping perturbation, with the explicit inclusion of the lattice deformations or, equivalently, the deformation of the Brillouin zone. These corrections are linear in strain and are diff…
The Diels-Alder surface modified top epitaxial graphene layer, with newly created pair of sp3 carbon centres, results in abrupt minimization of interlayer van der Waals interactions between two stacked graphene planes, and escapes the wafer during post-reaction manipulation stage, leaving the layer under it almost pristine-like. Above picture shows Diels-Alder functionalized sp2/sp3 graphene adduct leaves the parent wafer. In this communication we systematically address several fundamental questions in graphene surface chemistry, which are of extreme importance for device fabrication, and in s…
Large holes in graphene membranes were recently shown to heal, either at room temperature during a low energy STEM experiment, or by annealing at high temperatures. However, the details of the healing mechanism remain unclear. We carried out fully atomistic reactive molecular dynamics simulations in order to address these mechanisms under different experimental conditions. Our results show that, if a carbon atom source is present, high temperatures can provide enough energy for the carbon atoms to overcome the potential energy barrier and to produce perfect reconstruction of the graphene hexag…
With reduced degrees of freedom, structural defects are expected to play a greater role in two-dimensional materials in comparison to their bulk counterparts. In particular, mechanical strength, electronic properties, and chemical reactivity are strongly affected by crystal imperfections in the atomically thin limit. Here, ultra-high vacuum (UHV) scanning tunneling microscopy (STM) and spectroscopy (STS) are employed to interrogate point and line defects in monolayer MoS2 grown on epitaxial graphene (EG) at the atomic scale. Five types of point defects are observed with the majority species sh…
Van der Waals heterostructures obtained by artificially stacking two-dimensional crystals represent the frontier of material engineering, demonstrating properties superior to those of the starting materials. Fine control of the interlayer twist angle has opened new possibilities for tailoring the optoelectronic properties of these heterostructures. Twisted bilayer graphene with a strong interlayer coupling is a prototype of twisted heterostructure inheriting the intriguing electronic properties of graphene. Understanding the effects of the twist angle on its out-of-equilibrium optical properti…
We demonstrate a considerable suppression of the low-field leakage through a Y2O3 topgate insulator on graphene by applying high-pressure O2 at 100 atm during post-deposition annealing (HP-PDA). Consequently, the quantum capacitance measurement for the monolayer graphene reveals the largest Fermi energy modulation (EF = ~0.52 eV, i.e., the carrier density of ~2*10^13 cm^-2) in the solid-state topgate insulators reported so far. HP-PDA is the robust method to improve the electrical quality of high-k insulators on graphene.
Thermoelectrics as a way to use waste heat, is essential in electronic industries, but its low performance at operational temperatures makes it inappropriate in practical applications. Tailoring graphene can change its properties. In this work, we are interested in studying the transport properties of S-shape graphene structures with the single vacancy (SV) and double vacancy (DV) models. The structures are composed of a chiral part, which is an armchair graphene nanoribbon, and two zigzag graphene ribbons. We investigate the changes in the figure of merit by means of the Seebeck coefficient, …
Due to their graphene-like properties after oxygen reduction, incorporation of graphene oxide (GO) sheets into correlated-electron materials offers a new pathway for tailoring their properties. Fabricating GO nanocomposites with polycrystalline MgB2 superconductors leads to an order of magnitude enhancement of the supercurrent at 5 K/8 T and 20 K/4 T. Herein, we introduce a novel experimental approach to overcome the formidable challenge of performing quantitative microscopy and microanalysis of such composites, so as to unveil how GO doping influences the structure and hence the material prop…
A quantitative understanding of the electromagnetic response of materials is essential for the precise engineering of maximal, versatile, and controllable light--matter interactions. Material surfaces, in particular, are prominent platforms for enhancing electromagnetic interactions and for tailoring chemical processes. However, at the deep nanoscale, the electromagnetic response of electron systems is significantly impacted by quantum surface-response at material interfaces, which is challenging to probe using standard optical techniques. Here, we show how ultra-confined acoustic graphene pla…
Understanding the origin of hysteresis in the channel resistance from top gated graphene transistors is important for transistor applications. Capacitance - voltage measurements across the gate oxide on top gated bilayer graphene show hysteresis with a charging and discharging time constant of ~100 μs. However, the measured capacitance across the graphene channel does not show any hysteresis, but shows an abrupt jump at a high channel voltage due to the emergence of an order, indicating that the origin of hysteresis between gate and source is due to charge traps present in the gate oxide and g…
We report results of experimental investigation of the low-frequency noise in the top-gate graphene transistors. The back-gate graphene devices were modified via addition of the top gate separated by 20 nm of HfO2 from the single-layer graphene channels. The measurements revealed low flicker noise levels with the normalized noise spectral density close to 1/f (f is the frequency) and Hooge parameter below 2 x 10^-3. The analysis of the noise spectral density dependence on the top and bottom gate biases helped us to elucidate the noise sources in these devices and develop a strategy for the ele…
Graphene is a unique material to study fundamental limits of plasmonics. Apart from the ultimate single-layer thickness, its carrier concentration can be tuned by chemical doping or applying an electric field. In this manner the electrodynamic properties of graphene can be varied from highly conductive to dielectric. Graphene supports strongly confined, propagating surface plasmon-polaritons (SPPs) in a broad spectral range from terahertz to mid-infrared frequencies. It also possesses a strong magneto-optical response and thus provides complimentary architectures to conventional magneto-plasmo…
