The discovery of superconductivity and correlated electronic states in the flat bands of twisted bilayer graphene has raised a lot of excitement. Flat bands also occur in multilayer graphene flakes that present rhombohedral (ABC) stacking order on many consecutive layers. Although Bernal-stacked (AB) graphene is more stable, long-range ABC-ordered flakes involving up to 50 layers have been surprisingly observed in natural samples. Here we present a microscopic atomistic model, based on first-principles density functional theory calculations, that demonstrates how shear stress can produce long-range ABC order. A stress-angle phase diagram shows under which conditions ABC-stacked graphene can be obtained, providing an experimental guide for its synthesis.
In rhombohedral-stacked few-layer graphene, the very flat energy bands near the charge neutrality point are unstable to electronic interactions, giving rise to states with spontaneous broken symmetries. Using transport measurements on suspended rhombohedral-stacked tetralayer graphene, we observe an insulating ground state with a large interaction-induced gap up to 80 meV. This gapped state can be enhanced by a perpendicular magnetic field, and suppressed by an interlayer potential, carrier density, or a critical temperature of ~ 40 K.
Horizontal shifts in the top layer of highly oriented pyrolytic graphite, induced by a scanning tunneling microscope (STM) tip, are presented. Excellent agreement is found between STM images and those simulated using density functional theory. First-principle calculations identify that the low-energy barrier direction of the top layer displacement is toward a structure where none of the carbon pz orbitals overlap, while the high-energy barrier direction is toward AA stacking. Each directional shift yields a real-space surface charge density similar to graphene; however the low-energy barrier d…
Van der Waals (vdW) materials have greatly expanded our design space of heterostructures by allowing individual layers to be stacked at non-equilibrium configurations, for example via control of the twist angle. Such heterostructures not only combine characteristics of the individual building blocks, but can also exhibit emergent physical properties absent in the parent compounds through interlayer interactions. Here we report on a new family of emergent, nanometer-thick, semiconductor 2D ferroelectrics, where the individual constituents are well-studied non-ferroelectric monolayer transition …
The band structure of ABC-stacked N-layer graphene comprises topologically corresponding flat surface and gapped bulk subbands, as a consequence of the unique stacking configuration. In this paper, the bulk subbands are for the first times ever obtained for arbitrary N. A non-perturbative effective Hamiltonian closed in the bulk subspace is derived and used. The gapped bulk subbands are shown to evolve towards the zero energy with increasing N and in the infinite limit, they touch linearly along a circle. This outcome is a manifestation of the dimensional crossover to a three-dimensional Dirac…
Three-dimensional topological semimetals can support band crossings along one-dimensional curves in the momentum space (nodal lines or Dirac lines) protected by structural symmetries and topology. We consider rhombohedrally (ABC) stacked honeycomb lattices supporting Dirac lines protected by time-reversal, inversion and spin rotation symmetries. For typical band structure parameters there exists a pair of nodal lines in the momentum space extending through the whole Brillouin zone in the stacking direction. We show that these Dirac lines are topologically distinct from the usual Dirac lines wh…
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 …
The interlayer coupling is emerging as a new parameter for tuning the physical properties of two-dimensional (2D) van der Waals materials. When two identical semiconductor monolayers are stacked with a twist angle, the periodic interlayer coupling modulation due to the moiré superlattice may endow exotic physical phenomena, such as moiré excitons and correlated electronic phases. To gain insight into these new phenomena, it is crucial to unveil the underlying coupling between atomic layers. Recently, the rhombohedral-stacked transition metal dichalcogenide (TMD) bilayer has attracted significa…
Low-energy electronic properties of ABC-stacked graphite are studied by the tight-binding model. There are linear and parabolic bands with and without degeneracy. They show strongly anisotropic dispersions. ABC-stacked grahite is a semimetal due to slight overlapping near the Fermi level beween conduction and valence bands. The interlayer interactions could change the energy dispersion, state degeneracy, and positions of band-crossing and band-edge state. Density of states exhibit a shoulder structure, owing to band-edge states near or at high symmetric points. Low-frequency Coulomb excitation…
Trilayer graphene (TLG) exhibits rich novel electronic properties and extraordinary quantum Hall phenomena owning to enhanced electronic interactions and tunable chirality of its quasiparticles. Here, we report direct observation of chirality transition of quasiparticles at stacking solitons of TLG via spatial-resolved Landau level spectroscopy. The one-dimensional stacking solitons with width of the order of 10 nm separate adjacent Bernal-stacked TLG and rhombohedral-stacked TLG. By using high field tunneling spectra of scanning tunneling microscopy, we measured Landau quantization in both th…
Stacking order in van der Waals materials determines the coupling between atomic layers and is therefore key to the materials' properties. By exploring different stacking orders, many novel physical phenomena have been realized in artificial vdW stacks. Recently, 2D ferroelectricity has been observed in zero-degree aligned hBN and graphene-hBN heterostructures, holding promise in a range of electronic applications. In those artificial stacks, however, the single domain size is limited by the stacking-angle misalignment to about 0.1 to 1 $μ$m, which is incompatible with most optical or optoelec…
Due to their unique electron dispersion and lack of a Fermi surface, Coulomb interactions in undoped two-dimensional Dirac systems, such as single, bi- and tri-layer graphene, can be marginal or relevant. Relevant interactions can result in spontaneous symmetry breaking, which is responsible for a large class of physical phenomena ranging from mass generation in high energy physics to correlated states such as superconductivity and magnetism in condensed matter. Here, using transport measurements, we show that rhombohedral-stacked trilayer graphene (r-TLG) offers a simple, yet novel and tunabl…
Tunneling atomic force microscopy (TUNA) was used at ambient conditions to measure the current-voltage ($I$-$V$) characteristics at clean surfaces of highly oriented graphite samples with Bernal and rhombohedral stacking orders. The characteristic curves measured on Bernal-stacked graphite surfaces can be understood with an ordinary self-consistent semiconductor modeling and quantum mechanical tunneling current derivations. We show that the absence of a voltage region without measurable current in the $I$-$V$ spectra is not a proof of the lack of an energy band gap. It can be induced by a surf…
Charge carriers in single and multilayered graphene systems behave as chiral particles due to the particular lattice symmetry of the crystal. We show that the interplay between the meta-material properties of graphene multilayers and the pseudospinorial properties of the charge carriers result in the occurrence of Klein and anti-Klein tunneling for rhombohedral stacked multilayers. We derive an algebraic formula predicting the angles at which these phenomena occur and support this with numerical calculations for systems up to four layers. We present a decomposition of an arbitrarily stacked mu…
Motivated by the observation of two distinct superconducting phases in the moiréless ABC-stacked rhombohedral trilayer graphene, we investigate the electron-acoustic-phonon coupling as a possible pairing mechanism. We predict the existence of superconductivity with the highest $T_c\sim 3$K near the Van Hove singularity. Away from the Van Hove singularity, $T_c$ remains finite in a wide range of doping. In our model, the $s$-wave spin-singlet and $f$-wave spin-triplet pairings yield the same $T_c$, while other pairing states have negligible $T_c$. Our theory provides a simple explanation for th…
Enrichment of rhombohedral stacking by mechanical exfoliation of graphite
Hungarian Research Network, Centre for Energy Research（匈牙利研究网络能源研究中心）；MTA - HUN-REN EK Lendület “Momentum” Topology in Nanomaterials Research Group（MTA-HUN-REN EK Lendulet“动量”纳米材料拓扑研究组）；Óbuda University（奥比乌斯大学）；Budapest University of Technology and Economics（布达佩斯技术与经济大学）；ELTE Eötvös Loránd University（罗兰大学）
In recent times, trilayer graphene has attracted wide attention owing to its stacking and electric field dependent electronic properties. However, a direct and well-resolved experimental visualization of its band structure has not yet been reported. In this work, we present angle resolved photoemission spectroscopy (ARPES) data which show with high resolution the electronic band structure of trilayer graphene obtained on α-SiC(0001) and β-SiC(111) via hydrogen intercalation. Electronic bands obtained from tight-binding calculations are fitted to the experimental data to extract the interatomic…
Trilayer graphene is receiving an increasing level of attention due to its stacking--dependent magnetoelectric and optoelectric properties, and its more robust ferromagnetism relative to monolayer and bilayer variants. Additionally, rhombohedral stacked trilayer graphene presents the possibility of easily opening a gap via either an external electric field perpendicular to the layers, or via the application of external strain. In this paper, we consider an external electric field to open a bandgap in rhombohedral trilayer graphene and study the excitonic optical response of the system. This is…
Few layer graphene (FLG) has been recently intensively investigated for its variable electronic properties defined by a local atomic arrangement. While the most natural layers arrangement in FLG is ABA (Bernal) stacking, a metastable ABC (rhombohedral) stacking characterized by a relatively high energy barrier can also occur. When both stacking occur in the same FLG device this results in in-plane heterostructure with a domain wall (DW). We show that ABC stacking in FLG can be controllably and locally turned into ABA stacking by two following approaches. In the first approach, Joule heating wa…
The low-energy physics of rhombohedral $N$-layer graphene mainly arises on the external layers, where most of the π electrons are located. Their Bloch band structure defines a two-band semimetal; the dispersion relation scales as $\pm q^{N}$ with the momentum norm $q$ in the vicinity of two nonequivalent valleys. In this paper, we address the problem of elastic scattering through a localized impurity located either on the surface of the material or within the bulk, and focus on the quantum interferences it induces on the two external layers. It is apprehended in the framework of a $T$-matrix a…
Magnetism is a prototypical phenomenon of quantum collective state, and has found ubiquitous applications in semiconductor technologies such as dynamic random access memory (DRAM). In conventional materials, it typically arises from the strong exchange interaction among the magnetic moments of d- or f-shell electrons. Magnetism, however, can also emerge in perfect lattices from non-magnetic elements. For instance, flat band systems with high density of states (DOS) may develop spontaneous magnetic ordering, as exemplified by the Stoner criterion. Here we report tunable magnetism in rhombohedra…
In the continuum low energy model, we calculate the one-loop dynamical polarization functions in ABC-stacked (rhombohedral) $n$-layer graphene in a magnetic field. Neglecting the trigonal warping effects, they are derived as functions of wavevector and frequency at finite chemical potential, temperature, band gap, and the width of Landau levels. The analytic results are given in terms of digamma functions and generalized Laguerre polynomials and have the form of double sums over Landau levels. Various particular limits for polarization functions (static, clean, etc.) are discussed. The intrala…
Graphene layers are known to stack in two stable configurations, namely ABA or ABC stacking, with drastically distinct electronic properties. Unlike the ABA stacking, little has been done to experimentally investigate the electronic properties of ABC graphene multilayers. Here, we report the first magneto optical study of a large ABC domain in a graphene multilayers flake, with ABC sequences exceeding 17 graphene sheets. The ABC-stacked multilayers can be fingerprinted with a characteristic electronic Raman scattering response, which persists even at room temperatures. Tracing the magnetic fie…
Graphene and other two-dimensional crystals can be combined to form various hybrids and heterostructures, creating materials on demand, in which the interlayer coupling at the interface leads to modified physical properties as compared to their constituents. Here, by measuring Raman spectra of shear modes, we probe the coupling at the interface between two artificially-stacked few-layer graphenes rotated with respect to each other. The strength of interlayer coupling between the two interface layers is found to be only 20% of that between Bernal-stacked layers. Nevertheless, this weak coupling…
Stackings in graphene have a pivotal role in properties to be discussed in the future, as seen in the recently found superconductivity of twisted bilayer graphene. Beyond bilayer graphene, the stacking order of multilayer graphene can be rhombohedral, which shows flat bands near the Fermi level that are associated with interesting phenomena, such as tunable conducting surface states expected to exhibit spontaneous quantum Hall effect, surface superconductivity, and even topological order. However, the difficulty in exploring rhombohedral graphenes is that in experiments, the alternative, hexag…
Nanocenter CENN（纳米中心CENN）；Faculty of Mathematics and Physics, University of Ljubljana（卢布尔雅那大学数学物理学院）；Department of Physics, Massachusetts Institute of Technology（麻省理工学院物理系）；Department of Physics and Astronomy, Center for Materials Theory, Rutgers University（罗格斯大学物理与天文学系材料理论中心）；Department of Physics, University of Wisconsin-Madison（威斯康星大学麦迪逊分校物理系）；Max-Planck Institute for Solid State Research（马克斯·普朗克固体研究所）
Motivated by recent experiments on ABC-stacked rhombohedral trilayer graphene (RTG) which observed spin-valley symmetry-breaking and superconductivity, we study instabilities of the RTG metallic state to symmetry breaking orders. We find that interactions select the inter-valley coherent order (IVC) as the preferred ordering channel over a wide range, whose theoretically determined phase boundaries agree well with experiments on both the hole and electron doped sides. The Fermi surfaces near van Hove singularities admit partial nesting between valleys, which promotes both inter-valley supercon…
Electrostatically stabilized surface flat bands in rhombohedral graphite at zero displacement field
Aalto University School of Science（阿尔托大学理学院）；University of California at Santa Barbara（加州大学圣塔芭芭拉分校）；National High Magnetic Field Laboratory（国家高磁场实验室）；Florida State University（佛罗里达州立大学）
The stacking order degree of freedom in trilayer graphene plays a critical role in determining the existence of an electric field tunable band gap. We present spatially-resolved tunneling spectroscopy measurements of dual gated Bernal (ABA) and rhombohedral (ABC) stacked trilayer graphene devices. We demonstrate that while ABA trilayer graphene remains metallic, ABC trilayer graphene exhibits a widely tunable band gap as a function of electric field. However, we find that charged impurities in the underlying substrate cause substantial spatial fluctuation of the gap size. Our work elucidates t…
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…
Chiral superconductivity from parent Chern band and its non-Abelian generalization
University of Maryland, College Park（马里兰大学帕克分校）；University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Johns Hopkins University（约翰斯·霍普金斯大学）；University of Pittsburgh（匹兹堡大学）
The thermodynamic properties of the electron gas in multilayer graphene depend strongly on the number of layers and the type of stacking. Here we analyse how those properties change when we vary the number of layers for rhombohedral stacked multilayer graphene and compare our results with those from a conventional two dimensional electron gas. We show that the highly degenerate zero energy Landau level which is partly filled with electrons and partly with holes has a strong influence on the value of the different thermodynamic quantities.
Multilayer graphene with rhombohedral and Bernal stacking are supposed to be metallic, as predicted by density functional theory calculations using semi-local functionals. However recent angular resolved photoemission and transport data have questioned this point of view. In particular, rhombohedral flakes are suggested to be magnetic insulators. Bernal flakes composed of an even number of layers are insulating, while those composed of an odd number of layers are pseudogapped. Here, by systematically benchmarking with plane waves codes, we develop very accurate all-electron Gaussian basis sets…
Experimental signature of layer skyrmions and implications for band topology in twisted WSe2 bilayers
University of Texas at Austin（德克萨斯大学奥斯汀分校）；The University of Hong Kong（香港大学）；National Yang Ming Chiao Tung University（阳明交通大学）；Pennsylvania State University（宾夕法尼亚州立大学）；National Institute for Materials Science（日本物质材料研究机构）
Trilayer graphene in both ABA (Bernal) and ABC (rhombohedral) stacking sequences is shown to exhibit intense infrared absorption from in-plane optical phonons. The feature, lying at ~1580 cm-1, changes strongly with electrostatic gating. For ABC-stacked graphene trilayers, we observed a large enhancement in phonon absorption amplitude, as well as softening of the phonon mode, as the Fermi level is tuned away from charge neutrality. A similar, but substantially weaker effect is seen in samples with the more common ABA stacking order. The strong infrared response of the optical phonons and the p…
