A single graphene layer placed between two parallel Ni(111) surfaces screens the strong attractive force and results in a significant reduction of adhesion and sliding friction. When two graphene layers are inserted, each graphene is attached to one of the metal surfaces with a significant binding and reduces the adhesion further. In the sliding motion of these surfaces the transition from stick-slip to continuous sliding is attained, whereby non-equilibrium phonon generation through sudden processes is suppressed. The adhesion and corrugation strength continues to decrease upon insertion of the third graphene layer and eventually saturates at a constant value with increasing number of graphene layers. In the absence of Ni surfaces, the corrugation strength of multilayered graphene is relatively higher and practically independent of the number of layers. Present first-principles calculations reveal the superlubricant feature of graphene layers placed between pseudomorphic Ni(111) surfaces, which is achieved through the coupling of Ni-3d and graphene-$π$ orbitals. The effect of graphene layers inserted between a pair of parallel Cu(111) and Al(111) surfaces are also discussed. The treatment of sliding friction under the constant loading force, by taking into account the deformations corresponding to any relative positions of sliding slabs, is the unique feature of our study.
The state of vanishing friction known as superlubricity has important applications for energy saving and increasing the lifetime of devices. Superlubricity detected with atomic force microscopy appears in examples like sliding large graphite flakes or gold nanoclusters across surfaces. However, the origin of the behavior is poorly understood due to the lack of a controllable nano-contact. We demonstrate graphene nanoribbons superlubricity when sliding on gold with a joint experimental and computational approach. The atomically well-defined contact allows us to trace the origin of superlubricit…
The potential energy surface (PES) of interlayer interaction of twisted bilayer graphene with vacancies in one of the layers is investigated via density functional theory (DFT) calculations with van der Waals corrections. These calculations give a non-negligible magnitude of PES corrugation of 28 meV per vacancy and barriers for relative sliding of the layers of 7 - 8 meV per vacancy for the moiré pattern with coprime indices (2,1) (twist angle 21.8$^\circ$). At the same time, using the semiempirical potential fitted to the DFT results, we confirm that twisted bilayer graphene without defects …
In light of the race towards macroscale superlubricity of graphitic contacts, the effect of grain boundaries on their frictional properties becomes of central importance. Here, we elucidate the unique frictional mechanisms characterizing topological defects along typical grain boundaries that can vary from being nearly flat to highly corrugated, depending on the boundary misfit angle. We find that frictional energy dissipation over grain boundaries can originate from variations of compressibility along the surface, heat produced during defect (un)buckling events, and elastic energy storage in …
Robust structural superlubricity of twisted graphene bilayer and domain walls between commensurate moiré pattern domains from first-principles calculations
Quantifying superlubricity of bilayer graphene from the mobility of interface dislocations
University of Illinois at Urbana-Champaign（伊利诺伊大学厄巴纳-香槟分校）；Material Research Laboratory, University of Illinois at Urbana-Champaign（伊利诺伊大学厄巴纳-香槟分校材料研究实验室）
We address the atomistic nature of the longitudinal static friction against sliding of graphene nanoribbons (GNRs) deposited on gold, a system whose structural and mechanical properties have been recently the subject of intense experimental investigation. By means of numerical simulations and modeling we show that the GNR interior is structurally lubric ("superlubric") so that the static friction is dominated by the front/tail regions of the GNR, where the residual uncompensated lateral forces arising from the interaction with the underneath gold surface opposes the free sliding. As a result o…
In this paper we review thermal properties of graphene and multilayer graphene and discuss the optothermal technique developed for the thermal conductivity measurements. We also outline different theoretical approaches used for the description of phonon transport in graphene and provide comparison with available experimental thermal conductivity data.
We study the optical transmittance of multilayer graphene films up to 65 layers thick. By combing large-scale tight-binding simulation and optical measurement on CVD multilayer graphene, the optical transmission through graphene films in the visible region is found to be solely determined by the number of graphene layers. We argue that the optical transmittance measurement is more reliable in the determination of the number of layers than the commonly used Raman Spectroscopy. Moreover, optical transmittance measurement can be applied also to other 2D materials with weak van der Waals interlaye…
We address the intrinsic polarisation and screening of external electric field in a broad range of ordered and twisted configurations of multilayer graphene, using an ab initio approach combining density functional theory and the Wannier function formalism. We show that multilayer graphene is intrinsically polarized due to the crystal field effect, an effect that is often neglected in tight-binding models of twisted bilayer graphene and similar systems. This intrinsic polarization of the order of up to few tens of meVs has different out-of-plane alignments in ordered and twisted graphene multi…
We discuss the chiral decomposition of non-symmetric stacking structures. It is shown that the low-energy electronic structure of Bernal stacked graphene multilayer deposited on h-BN consists of chiral pseudospin doublets. N-layer graphene stocks on h-BN layer have N/2 effective bilayer graphene systems and one effective h-BN layer if N is even or (N-1)/2 effective graphene bilayers plus one graphene monolayer modified by h-BN layer if N is odd. We present the decomposition procedure and we derive the recurrence relations for the effective parameters characterizing the chiral subsystems. The e…
Rhombohedral stacked multilayer graphene displays the occurrence of a magnetic surface state at low temperatures. Recent angular resolved photoemission experiments demonstrate the robustness of the magnetic state in long sequences of ABC graphene. Here, by using first-principles calculations, we show that field-effect doping of these graphene multilayers induces a perfect half-metallic behaviour with 100% of spin current polarization already at dopings attainable in conventional field effect transistors with solid state dielectrics. Our work demonstrates the realisability of a new kind of spin…
Edges naturally exist in a single-layer graphene sample. Similarly, individual graphene layers in a multilayer graphene sample contribute their own edges. We study the Raman spectrum at the edge of a graphene layer laid on n layer graphene (nLG). We found that the D band observed from the edge of the top graphene layer exhibits an identical line shape to that of disordered (n+1)LG induced by ion-implantation. Based on the spectral features of the D and 2D bands, we identified two types of alignment configurations at the edges of mechanically-exfoliated bilayer and trilayer graphenes, whose edg…
We propose a generalized Peierls substitution method in conjunction with the tight-binding model to explore the magnetic quantization and quantum Hall effect in twisted multilayer graphene under a magnetic field. The Bloch-basis tight-binding Hamiltonian is constructed for large twist angle while a simplified tight-binding model is employed for the magic angle. We investigate extensively the band structures, Landau levels (LLs), and quantum Hall conductivity (QHC) of twisted bilayer graphene and twisted double bilayer graphene, as well as their dependence on the twist angle. Comparison between…
The presence of twist angles between layers of two-dimensional materials has a profound impact on their physical properties. Turbostratic multilayer graphene is a system containing a distribution of rotational stacking faults, and these interfaces also have variable twist angles. In this work, we examine the influence of turbostratic single-layer graphene content on the in-plane thermal conductivity of a defect free multilayer graphene system with low defect density. Detailed Raman mode analysis is used to quantify the content of turbostratic single-layer graphene in the system while complemen…
We present a theoretical study on the electron transmission through the AB-BA stacking boundary in multilayer graphene. Using the tight-binding model and the transfer matrix method, we calculate the electron transmission probability through the boundary as a function of electron Fermi energy in multilayers from bilayer to five-layer. We find that the transmission is strongly suppressed particularly near the band touching point, suggesting that the electronic conductivity in general multilayer graphenes is significantly interfered by stacking fault. The conductivity suppression by stacking faul…
We demonstrate electrical spin injection into multilayer graphene (MLG) in a lateral spin valve device from a highly spin-polarized Co2FeSi (CFS) Huesler electrode. Exfoliated MLG was transferred onto pre-patterned epitaxial CFS wires grown on an Si(111) substrate by a polymer-based transfer method. This method enabled us to fabricate multiple single-crystal CFS electrodes in contact with MLG. Electrical spin injection from CFS to MLG was detected through non-local magnetoresistance (MR) measurement. A non-local spin signal of 430 ohm was observed; this is the largest value among all reported …
There has been a lot of excitement around the observation of superconductivity in twisted bilayer graphene, associated to flat bands close to the Fermi level. Such correlated electronic states also occur in multilayer rhombohedral stacked graphene (RG), which has been receiving increasing attention in the last years. In both natural and artificial samples however, multilayer stacked Bernal graphene (BG) occurs more frequently, making it desirable to determine what is their relative stability and under which conditions RG might be favored. Here, we study the energetics of BG and RG in bulk and …
In this work, we study structural and vibrational properties of multilayer graphene using density-functional theory (DFT) with van der Waals (vdW) functionals. Initially, we analyze how different vdW functionals compare by evaluating the lattice parameters, elastic constants and vibrational frequencies of low energy optical modes of graphite. Our results indicate that the vdW-DF1-optB88 functional has the best overall performance on the description of vibrational properties. Next, we use this functional to study the influence of the vdW interactions on the structural and vibrational properties…
Scanning tunneling microscopy (STM) images are obtained for the first time on few layer and twisted multilayer epitaxial graphene states synthesized on n+ 6H-SiC a-plane non-polar surface. The twisted graphene is determined to have a rotation angle of 5.4° between the top two layers, by comparing moiré patterns from stick and ball models of bilayer graphene to experimentally obtained images. Furthermore, the experimental moiré pattern shows dynamic behavior, continuously shuffling between two stable surface arrangements one bond length apart. The moiré pattern shifts by more than 1 nm, making …
When electrons are confined in a two dimensional (2D) system, typical quantum mechanical phenomena such as Landau quantization can be detected. Graphene systems, including the single atomic layer and few-layer stacked crystals, are ideal 2D materials for studying a variety of quantum mechanical problems. In this article, we review the experimental progress in the unusual Landau quantized behaviors of Dirac fermions in monolayer and multilayer graphene by using scanning tunneling microscopy(STM) and scanning tunneling spectroscopy(STS). Through STS measurement of the strong magnetic fields, dis…
In the context of graphene-based composite applications, a complete understanding of charge conduction in multilayer reduced graphene oxides (rGO) is highly desirable. However, these rGO compounds are characterized by multiple and different sources of disorder depending on the chemical method used for their synthesis. Most importantly the precise role of interlayer interaction in promoting or jeopardizing electronic flow remains unclear. Here, thanks to the development of a multiscale computational approach combining first-principles calculations with large scale transport simulations, the tra…
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…
Turbostratic graphitic microstructures: electronically decoupled multilayer graphene devices with robust high charge carrier mobility
碳纳米材料由于其特殊的物理性质继续令科学家感到惊讶。最近已经有理论预测和石墨烯多层膜的第一次报告，其中，由于堆叠层的旋转，保持了出色的电子性能，同时由于多层性质，对降解和机械应力的敏感性大大降低。在这里，我们表明，完全乱层多层石墨微结构结合了先进的电子和自旋电子器件所需的高载流子迁移率与石墨结构的鲁棒性。使用拉曼光谱和透射电子显微镜（TEM）的盘形石墨微结构的结构表征揭示了莫尔和衍射图案证实其乱层性质。电子输运特性产生了可重复的高迁移率，> 105 cm ^2（Vs）^（-1），与盘的厚度无关，这是乱层堆积引起的电子去耦的直接结果。
We report on spatial measurements of the superconducting proximity effect in epitaxial graphene induced by a graphene-superconductor interface. Superconducting aluminum films were grown on epitaxial multilayer graphene on SiC. The aluminum films were discontinuous with networks of trenches in the film morphology reaching down to exposed graphene terraces. Scanning tunneling spectra measured on the graphene terraces show a clear decay of the superconducting energy gap with increasing separation from the graphene-aluminum edges. The spectra were well described by Bardeen-Cooper-Schrieffer (BCS) …
Circular polarization resolved magneto-infrared studies of multilayer epitaxial graphene (MEG) are performed using tunable quantum cascade lasers in high magnetic fields up to 17.5 T. Landau level (LL) transitions in the monolayer and bilayer graphene inclusions of MEG are resolved, and considerable electron-hole asymmetry is observed in the extracted electronic band structure. For monolayer graphene, a four-fold splitting of the $n=0$ to $n=1$ LL transition is evidenced and attributed to the lifting of the valley and spin degeneracy of the zeroth LL and the broken electron-hole symmetry. The …
Using the low-energy effective Hamiltonian of the ABC-stacked multilayer graphene, pseudo spin coupling to real orbital angular momentum of electron in multilayer graphene is investigated. We show that electron wave function in N-layer graphene mimics behavior of particle with spin of N/2. It is said that for N greater than 1 the low-energy effective Hamiltonian for ABC-stacked graphene is no longer used to describe pseudo spin 1/2-particle wave function. The wave function of electron in multilayer graphene may behave like fermionic (or bosonic) particle when N is odd (or even). This work prop…
Bilayer graphene has been a subject of intense study in recent years. We extend a structural phase field crystal method to include an external potential from adjacent layer(s), which is generated by the corresponding phase field and changes over time. Moreover, multiple layers can be added into the structure. Using the thickness of the boundaries between different stacking variants of the bilayer structure as the key parameter, we quantify the strength of the adjacent layer potential by comparing with atomistic simulation results. We then test the multiple graphene structures, including bilaye…
We calculate the transport properties of multilayer graphene, considering the effect of multisubband scattering in a high density regime, where higher subbands are occupied by charge carriers. To calculate the conductivity of multilayer graphene, we use the coupled multiband Boltzmann transport theory while fully incorporating the multiband scattering effects. We show that the allowed scattering channels, screening effects, chiral nature of the electronic structure, and type of impurity scatterings determine the transport behavior of multilayer graphene. We find that the conductivity of multil…
We investigate the competition between acoustic-phonon-mediated superconductivity and the long-range Coulomb interaction in moiréless graphene multilayers, specifically, Bernal bilayer graphene, rhombohedral trilayer graphene, and ABCA-stacked tetralayer graphene. In these graphene multilayers, the acoustic phonons can realize, through electron-phonon coupling, both spin-singlet and spin-triplet pairings, and the intra-sublattice pairings ($s$-wave spin-singlet and $f$-wave spin-triplet) are the dominant channels. Our theory naturally explains the distinct recent experimental findings in Berna…
The intrinsic resistance peak (ridge) structures were recently found to appear in the carrier density dependence plot of the resistance of the AB-stacked multilayer graphene with even numbers of layers.The ridges are due to topological changes in the Fermi surface. Here, these structures were studied in AB-stacked multilayer graphene with odd numbers of layers (5 and 7 layers) by performing experiments using encapsulated high-quality graphene samples equipped with top and bottom gate electrodes.The intrinsic resistance peaks that appeared on maps plotted with respect to the carrier density and…
