Guorui Chen

Epitaxial growth of single-domain graphene on hexagonal boron nitride

Hexagonal boron nitride (h-BN) has recently emerged as an excellent substrate for graphene nanodevices, owing to its atomically flat surface and its potential to engineer graphenes electronic structure. Thus far, graphene/h-BN heterostructures have been obtained only through a transfer process, which introduces structural uncertainties due to the random stacking between graphene and h-BN substrate. Here we report the epitaxial growth of single-domain graphene on h-BN by a plasma-assisted deposition method. Large-area graphene single crystals were successfully grown for the first time on h-BN with a fixed stacking orientation. A two-dimensional (2D) superlattice of trigonal moiré pattern was observed on graphene by atomic force microscopy. Extra sets of Dirac points are produced as a result of the trigonal superlattice potential and the quantum Hall effect is observed with the 2D-superlattice-related feature developed in the fan diagram of longitudinal and Hall resistance, and the Dirac fermion physics near the original Dirac point is unperturbed. The macroscopic epitaxial graphene is in principle limited only by the size of the h-BN substrate and our synthesis method is potentially applicable on other flat surfaces. Our growth approach could thus open new ways of graphene band engineering through epitaxy on different substrates.

Quantum oscillations in a two-dimensional electron gas in black phosphorus thin films

For decades, two-dimensional electron gases (2DEG) have allowed important experimental discoveries and conceptual developments in condensed-matter physics. When combined with the unique electronic properties of two-dimensional crystals, they allow rich physical phenomena to be probed at the quantum level. Here, we create a 2DEG in black phosphorus--a recently added member of the two-dimensional atomic crystal family--using a gate electric field. The black phosphorus film hosting the 2DEG is placed on a hexagonal boron nitride substrate. The resulting high carrier mobility in the 2DEG allows the observation of quantum oscillations. The temperature and magnetic field dependence of these oscillations yields crucial information about the system, such as cyclotron mass and lifetime of its charge carriers. Our results, coupled with the fact that black phosphorus possesses anisotropic energy bands with a tunable, direct bandgap, distinguish black phosphorus 2DEG as a system with unique electronic and optoelectronic properties.

Gate-tunable topological valley transport in bilayer graphene

Bilayer graphene can host topological currents that are robust against defects and are associated with the electron valleys. It is now shown that electric fields can tune this topological valley transport over long distances at room temperature. Valley pseudospin, the quantum degree of freedom characterizing the degenerate valleys in energy bands1, is a distinct feature of two-dimensional Dirac materials1,2,3,4,5. Similar to spin, the valley pseudospin is spanned by a time-reversal pair of states, although the two valley pseudospin states transform to each other under spatial inversion. The breaking of inversion symmetry induces various valley-contrasted physical properties; for instance, valley-dependent topological transport is of both scientific and technological interest2,3,4,5. Bilayer graphene is a unique system whose intrinsic inversion symmetry can be controllably broken by a perpendicular electric field, offering a rare possibility for continuously tunable topological valley transport. We used a perpendicular gate electric field to break the inversion symmetry in bilayer graphene, and a giant nonlocal response was observed as a result of the topological transport of the valley pseudospin. We further showed that the valley transport is fully tunable by external gates, and that the nonlocal signal persists up to room temperature and over long distances. These observations challenge the current understanding of topological valley transport in a gapped system, and the robust topological transport may lead to future valleytronic applications.

Gaps induced by inversion symmetry breaking and second-generation Dirac cones in graphene/hexagonal boron nitride

Graphene/h-BN has emerged as a model van der Waals heterostructure [1], and the band structure engineering by the superlattice potential has led to various novel quantum phenomena including the self-similar Hofstadter butterfly states [2–5]. Although newly generated second generation Dirac cones (SDCs) are believed to be crucial for understanding such intriguing phenomena, so far fundamental knowledge of SDCs in such heterostructure, e.g. locations and dispersion of SDCs, the effect of inversion symmetry breaking on the gap opening, still remains highly debated due to the lack of direct experimental results. Here we report first direct experimental results on the dispersion of SDCs in 0◦ aligned graphene/h-BN heterostructure using angle-resolved photoemission spectroscopy. Our data reveal unambiguously SDCs at the corners of the superlattice Brillouin zone, and at only one of the two superlattice valleys. Moreover, gaps of ≈ 100 meV and ≈ 160 meV are observed at the SDCs and the original graphene Dirac cone respectively. Our work highlights the important role of a strong inversion symmetry breaking perturbation potential in the physics of graphene/h-BN, and fills critical knowledge gaps in the band structure engineering of Dirac fermions by a superlattice potential. ∗These authors contribute equally to this work. †Correspondence should be sent to syzhou@mail.tsinghua.edu.cn

Thermally Induced Graphene Rotation on Hexagonal Boron Nitride.

In this Letter, we report the observation of thermally induced rotation of graphene on hexagonal boron nitride (h-BN). After the rotation, two thermally stable configurations of graphene on h-BN with a relative lattice twisting angle of 0° (most stable) and 30° (metastable), respectively, were found. Graphene on h-BN with a twisting angle below (above) a critical angle of ∼12±2° tends to rotate towards 0° (30°) at a temperature of >100 °C, which is in line with our theoretical simulations. In addition, by manipulating the annealing temperature and the flake sizes of graphene, moiré superlattices with large spatial periods of graphene on h-BN are achieved. Our studies provide a detailed understanding of the thermodynamic properties of graphene on h-BN and a feasible approach to obtaining van der Waals heterostructures with aligned lattices.

Strain-modulated Bandgap and Piezo-resistive Effect in Black Phosphorus Field-effect Transistors

Energy bandgap largely determines the optical and electronic properties of a semiconductor. Variable bandgap therefore makes versatile functionality possible in a single material. In layered material black phosphorus, the bandgap can be modulated by the number of layers; as a result, few-layer black phosphorus has discrete bandgap values that are relevant for optoelectronic applications in the spectral range from red, in monolayer, to mid-infrared in the bulk limit. Here, we further demonstrate continuous bandgap modulation by mechanical strain applied through flexible substrates. The strain-modulated bandgap significantly alters the density of thermally activated carriers; we for the first time observe a large piezo-resistive effect in black phosphorus field-effect transistors (FETs) at room temperature. The effect opens up opportunities for future development of electromechanical transducers based on black phosphorus, and we demonstrate an ultrasensitive strain gauge constructed from black phosphorus thin crystals.

Hofstadter Butterfly and Many-Body Effects in Epitaxial Graphene Superlattice

Graphene placed on hexagonal boron nitride (h-BN) has received a wide range of interest due to the improved electrical performance and rich physics from the interface, especially the emergence of superlattice Dirac points as well as Hofstadter butterfly in high magnetic field. Instead of transferring graphene onto h-BN, epitaxial growth of graphene directly on a single-crystal h-BN provides an alternative and promising way to study these interesting superlattice effects due to their precise lattice alignment. Here we report an electrical transport study on epitaxial graphene superlattice on h-BN with a period of ∼15.6 nm. The epitaxial graphene superlattice is clean, intrinsic, and of high quality with a carrier mobility of ∼27 000 cm(2) V(-1) s(-1), which enables the observation of Hofstadter butterfly features originated from the superlattice at a magnetic field as low as 6.4 T. A metal-insulator transition and magnetic field dependent Fermi velocity were also observed, suggesting prominent electron-electron interaction-induced many-body effects.

Electronic structure of transferred graphene/h-BN van der Waals heterostructures with nonzero stacking angles by nano-ARPES

In van der Waals heterostructures, the periodic potential from the Moiré superlattice can be used as a control knob to modulate the electronic structure of the constituent materials. Here we present a nanoscale angle-resolved photoemission spectroscopy (nano-ARPES) study of transferred graphene/h-BN heterostructures with two different stacking angles of 2.4° and 4.3° respectively. Our measurements reveal six replicas of graphene Dirac cones at the superlattice Brillouin zone (SBZ) centers. The size of the SBZ and its relative rotation angle to the graphene BZ are in good agreement with Moiré superlattice period extracted from atomic force microscopy (AFM) measurements. Comparison to the epitaxial graphene/h-BN with 0° stacking angles suggests that the interaction between graphene and h-BN decreases with increasing stacking angle.

Emergence of Tertiary Dirac Points in Graphene Moiré Superlattices

The electronic structure of a crystalline solid is largely determined by its lattice structure. Recent advances in van der Waals solids, artificial crystals with controlled stacking of two-dimensional (2D) atomic films, have enabled the creation of materials with novel electronic structures. In particular, stacking graphene on hexagonal boron nitride (hBN) introduces a moiré superlattice that fundamentally modifies graphenes band structure and gives rise to secondary Dirac points (SDPs). Here we find that the formation of a moiré superlattice in graphene on hBN yields new, unexpected consequences: a set of tertiary Dirac points (TDPs) emerge, which give rise to additional sets of Landau levels when the sample is subjected to an external magnetic field. Our observations hint at the formation of a hidden Kekulé superstructure on top of the moiré superlattice under appropriate carrier doping and magnetic fields.