Brillouin zones of graphene systems possess Dirac points, where band degeneracies occur. We study the variety of (and large magnitude) phases that the electronic states can acquire when a uniform time-dependent electric field carries the electrons around one or more Dirac points in a non-concentric fashion. An experimentally accessible determination of excess Berry phases is proposed involving the Zitterbewegung of electronic current near an orthogonality point in adiabatic motion.
Since its discovery, Berry phase has been demonstrated to play an important role in many quantum systems. In gapped Bernal bilayer graphene, the Berry phase can be continuously tuned from zero to 2pi, which offers a unique opportunity to explore the tunable Berry phase on the physical phenomena. Here, we report experimental observation of Berry phases-induced valley splitting and crossing in moveable bilayer graphene p-n junction resonators. In our experiment, the bilayer graphene resonators are generated by combining the electric field of scanning tunneling microscope tip with the gap of bila…
Ever since the novel quantum Hall effect in bilayer graphene was discovered, and explained by a Berry phase of 2pi [K. S. Novoselov et al., "Unconventional quantum Hall effect and Berry's phase of 2pi in bilayer graphene", Nature Phys. 2, 177 (2006)], it has been widely accepted that the low-energy electronic wavefunction in this system is described by a non-trivial Berry phase of 2pi, different from the zero phase of a conventional two-dimensional electron gas. Here, we show that (i) the relevant Berry phase for bilayer graphene is not different from that for a conventional two-dimensional el…
Berry phase plays an important role in determining many physical properties of quantum systems. However, a Berry phase altering energy spectrum of a quantum system is comparatively rare. Here, we report an unusual tunable valley polarized energy spectra induced by continuously tunable Berry phase in Bernal-stacked bilayer graphene quantum dots. In our experiment, the Berry phase of electron orbital states is continuously tuned from about pi to 2pi by perpendicular magnetic fields. When the Berry phase equals pi or 2pi, the electron states in the two inequivalent valleys are energetically degen…
When a gap of tunable size opens at the conic band intersections of graphene, the Berry phase does not vanish abruptly, but progressively decreases as the gap increases. The phase depends on the reciprocal-space path radius, i.e., for a doped system, the Fermi wave vector. The phase and its observable consequences can thus be tuned continuously via gap opening --by a modulating potential induced by strain, epitaxy, or nanostructuration-- and doping adjustment.
Klein tunneling in gapless bilayer graphene, perfect reflection of electrons injecting normal to a pn junction, is expected to disappear in the presence of energy band gap induced by external gates. We theoretically show that the Klein effect still exists in gapped bilayer graphene, provided that the gaps in the n and p regions are balanced such that the polarization of electron pseudospin has the same normal component to the bilayer plane in the regions. We attribute the Klein effect to Berry phase $π$ (rather than the conventional value $2 π$ of bilayer graphene) and to electron-hole and tim…
We have found that the Berry phase of bilayer graphene becomes from 2$π$ estimated by Shubnikov-de Haas oscillations when the A-B stacked pristine bilayer graphene experiences the Li-intercalation and sequential Li-desorption process in ultrahigh vacuum. Furthermore, the mobility of such processed bilayer graphene increases around four times larger, ~ 8,000 cm2/V$\cdot$s, than that of the pristine bilayer graphene. This is mainly due to increment of the scattering time and decrement of the cyclotron mass, which can be interpreted as a result of the change of the stacking structure of bilayer g…
Standing waves near the zigzag and armchair edges, and their Berry's phases are investigated. It is suggested that the Berry's phase for the standing wave near the zigzag edge is trivial, while that near the armchair edge is non-trivial. A non-trivial Berry's phase implies the presence of a singularity in parameter space. We have confirmed that the Dirac singularity is absent (present) in the parameter space for the standing wave near the zigzag (armchair) edge. The absence of the Dirac singularity has a direct consequence in the local density of states near the zigzag edge. The transport prop…
Chiral quasiparticles in Bernal-stacked bilayer graphene have valley-contrasting Berry phases of 2π. This nontrival topological structure, associated with the pseudospin winding along a closed Fermi surface, is responsible for various novel electronic properties, such as anti-Klein tunneling, unconventional quantum Hall effect, and valley Hall effect1-6. Here we show that the quantum interference due to intervalley scattering induced by atomic defects/impurities provides further insights into the topological nature of the bilayer graphene. The scattered chiral quasiparticles between distinct v…
Electronic band structures dictate the mechanical, optical and electrical properties of crystalline solids. Their experimental determination is therefore of crucial importance for technological applications. While the spectral distribution in energy bands is routinely measured by various techniques, it is more difficult to access the topological properties of band structures such as the Berry phase γ. It is usually thought that measuring the Berry phase requires applying external electromagnetic forces because these allow realizing the adiabatic transport on closed trajectories along which qua…
We consider the anomalous thermoelectric transport in gapped single and bilayer graphene where the gap may be due to broken inversion symmetry. In the presence of the gap, non-trivial Berry phase effects can be shown to mediate a transverse thermoelectric voltage in response to an applied temperature gradient even in the absence of a perpendicular magnetic field. This spontaneous, anomalous Nernst effect is nonzero for non-uniform chemical potential in the two inequivalent valleys in the graphene band structure. Conversely, the Nernst response can be used to create a valley-index polarization …
The electronic dispersion of a graphene bilayer is highly dependent on rotational mismatch between layers and can be further manipulated by electrical gating. This allows for an unprecedented control over electronic properties and opens up the possibility of flexible band structure engineering. Here we present novel magnetotransport data in a twisted bilayer, crossing the energetic border between decoupled monolayers and coupled bilayer. In addition a transition in Berry phase between pi and 2pi is observed at intermediate magnetic fields. Analysis of Fermi velocities and gate induced charge c…
We study the energy spectrum of a graphene bilayer in the presence of transverse electric and magnetic fields. We find that the resulting Landau levels exhibit a nonmonotonic dependence on the electric field, as well as numerous level crossings. This behavior is explained using quasiclassical quantization rules that properly take into account the pseudospin of the quasiparticles. The pseudospin generates the Berry phase, which leads to a shift in energy quantization and results in a pseudo-Zeeman effect. The latter depends on the electric field, alternates in sign among the two valleys, and al…
Single-layer carbon, or graphene, demonstrates amazing transport properties, such as the minimum conductivity near $\frac{4e^2}{h}$ independent of shapes and mobility of samples. This indicates there exist some unusual effects due to specific Dirac dispersion relation of fermion in two dimensions. By deriving fermion-lattice interaction Hamiltonian we show that Berry phases can be produced in fermion states around two Dirac points by relative rotations of two sublattices. The Berry phases in turn remove the degeneracies of energies for states near the Fermi surface, leading to a dynamical inst…
The phase of a quantum state may not return to its original value after the system's parameters cycle around a closed path; instead, the wavefunction may acquire a measurable phase difference called the Berry phase. Berry phases typically have been accessed through interference experiments. Here, we demonstrate an unusual Berry-phase-induced spectroscopic feature: a sudden and large increase in the energy of angular-momentum states in circular graphene p-n junction resonators when a small critical magnetic field is reached. This behavior results from turning on a $π$-Berry phase associated wit…
The electronic band structure of ABC-stacked multilayer graphene is studied within an effective mass approximation. The electron and hole bands touching at zero energy support chiral quasiparticles characterized by Berry's phase N pi for N-layers, generalizing the low-energy band structure of monolayer and bilayer graphene. We investigate the trigonal-warping deformation of the energy bands and show that the Lifshitz transition, in which the Fermi circle breaks up into separate parts at low energy, reflects Berry's phase N pi. It is particularly prominent in trilayers, N=3, with the Fermi circ…
Single-crystalline transition metal films are ideal playing fields for the epitaxial growth of graphene and graphene-base materials. Graphene-silicon layered structures were successfully constructed on Ir(111) thin film on Si substrate with an yttria-stabilized zirconia buffer layer via intercalation approach. Such hetero-layered structures are compatible with current Si-based microelectronic technique, showing high promise for applications in future micro- and nano-electronic devices.
Novel systems of layered graphene are attracting interest for theories and applications. The stability, band structures of few-layer graphite films, and their dependence on electric field applied along the c-axis are examined within the density functional theory. We predict that those of Bernal type and also rhombohedral type tri- and tetra-layer graphite films exhibit stability. The rhombohedral-type systems including AB-bilayer, show variable band gap induced by perpendicular electric field, whereas the other systems such as the Bernal-type films stay semi-metallic.
Berry curvature induced giant anomalous and spin texture driven Hall responses in the layered kagome antiferromagnet GdTi3Bi4
Indian Institute of Technology Delhi（印度德里理工学院）；Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences（中国科学院金属研究所沈阳材料科学国家研究中心）；Institute for Materials Research, Tohoku University（东北大学物质材料研究所学部）；Center for Science and Innovation in Spintronics, Tohoku University（东北大学自旋电子学科学与创新中心）
We investigated the electronic and optoelectronic properties of vertical van der Waals heterostructure photodetectors using layered p type GaSe and n type InSe, with graphene as the transparent electrodes. Not only the photocurrent peaks from the layered GaSe and InSe themselves were observed, also the interlayer optical transition peak was observed, which is consistent with the first-principles calculation. The built-in electric field between p-n heterojunction and the advantage of the graphene electrodes can effectively separate the photo-induced electron-hole pairs, and thus lead to the res…
The Lennard-Jones potential is widely used to describe the interlayer interactions within layered materials like graphene. However, it is also widely known that this potential strongly underestimates the frictional properties for layered materials. Here we propose to supplement the Lennard-Jones potential by a Gaussian-type potential, which enables more accurate calculations of the frictional properties of two-dimensional layered materials. Furthermore, the Gaussian potential is computationally simple as it introduces only one additional potential parameter that is determined by the interlayer…
We calculated the optical properties of an $N$-layer graphene by formulating the dynamical conductivity of each layer. This is the conductivity when an electromagnetic field is localized at a particular layer and differs from the standard conductivity calculated assuming a uniform field throughout all layers. By combining these conductivities with a transfer matrix method, we took into account the spatial variation of the electromagnetic field caused by internal reflections. The results obtained from the two conductivities show that similar peak structures originating from the interlayer elect…
We theoretically study the phase of the reflection amplitude of an electron (massive Dirac fermion) at a lateral potential step in Bernal-stacked bilayer graphene. The phase shows anomalous jump of $π$, as the electron incidence angle (relative to the normal direction to the step) varies to pass $\pm π/4$. The jump is attributed to the Berry phase associated with the pseudospin-1/2 of the electron. This Berry-phase effect is robust against the band gap opening due to the external electric gates generating the step. We propose an interferometry setup in which collimated waves can be generated a…
Layered electrides, as typified by Ca$_2$N, are a new class of quasi-two-dimensional materials with low work functions. Using first-principles calculations, we have shown that a graphene layer deposited on Ca$_2$N is doped to $n=5\times 10^{14}$ cm$^{-2}$ with its Fermi level aligned with the logarithmically divergent van Hove singularity in the graphene $π^*$ band. For bilayer graphene on Ca$_2$N, the inner graphene layer is doped to the same level, while the doping of the outer graphene layer is much more modest. This finding opens an interesting possibility of using layered electrides for t…
Nanoscale engineered materials combined with wearable wireless technologies can deliver a new level of health monitoring. A reduced graphene oxide-nylon composite material is developed and tested, demonstrating its usefulness as a material for sensors in wearable, long-term electrocardiogram (ECG) monitoring via a comparison to one of the widely used ECG sensors. The structural analysis by scanning electron (SEM) and atomic force microscopy (AFM) shows a limited number of defects on a macroscopic scale. Fourier Transform Infrared (FTIR) and Raman spectroscopy confirm the presence of rGOx, and …
Full experimental control of local spin-charge interconversion is of primary interest for spintronics. Heterostructures combining graphene with a strongly spin-orbit coupled two-dimensional (2D) material enable such functionality by design. Electric spin valve experiments have provided so far global information on such devices, while leaving the local interplay between symmetry breaking, charge flow across the heterointerface and aspects of topology unexplored. Here, we utilize magneto-optical Kerr microscopy to resolve the gate-tunable, local current-induced spin polarisation in graphene/WTe$…
We introduce an approach to derive realistic Coulomb interaction terms in free standing layered materials and vertical heterostructures from ab-initio modelling of the corresponding bulk materials. To this end, we establish a combination of calculations within the framework of the constrained random phase approximation, Wannier function representation of Coulomb matrix elements within some low energy Hilbert space and continuum medium electrostatics, which we call Wannier function continuum electrostatics (WFCE). For monolayer and bilayer graphene we reproduce full ab-initio calculations of th…
A model for the formation of carbon nanotubes (CNTs) and layered graphene in an arc discharge method is developed on the basis of observed erosion of graphite anode under various experimental conditions and analyses of the morphology of the eroded anode-surface, concerned cathode deposits and their constituents. It is predicted that, cold thermal shock, triggered by the rapid movement of the anode-spot, leads to crack microbranching at some selected locations on the anode-surface. These crack-microbranches cleave and fragment the basal planes of pairs of adjacent crystallites into curved graph…
Two-dimensional materials are popular in design of nanodevices. To improve bending stiffness of few-layered graphene ribbon, the relative sliding between neighboring layers should be avoided by method such as bonding them together. In this study, the new bonds between the graphene layers in ribbon are formed by ballistic C60 fullerenes from both surfaces of the ribbon. Collision effects are evaluated through molecular dynamics simulations. The formation of the new two dimensional carbon material is demonstrated by breakage and generation of bonds between atoms from graphene and/or fullerenes. …
The concept of hyperlens, as a novel transformation optics device, is a promising real-time super-resolution lens that can effectively transform evanescent waves into propagating waves and thus break the diffraction limit. However, previous hyperlens implementations usually adopted metal which would absorb most energy during light transmission and thus deteriorate imaging efficiency. Here we propose a novel hyperlens design based on dielectric layered graphene and h-boron nitride (h-BN) whose performance can surpass the counterpart design with metal. Our first-principle and Kramers-Kronig rela…
Nanostructured materials have emerged as an alternative to enhance the figure of merit (ZT) of thermoelectric (TE) devices. Graphene exhibits a high electrical conductivity (in-plane) that is necessary for a high ZT; however, this effect is countered by its impressive thermal conductivity. In this work TE layered devices composed of electrochemically exfoliated graphene (EEG) and a phonon blocking material such as poly (3,4-ethylenedioxythiophene)polystyrene sulfonate (PEDOT:PSS), polyaniline (PANI) and gold nanoparticles (AuNPs) at the interface were prepared. The figure of merit, ZT, of each…
Layering two-dimensional van der Waals materials provides unprecedented control over atomic placement, which could enable tailoring of vibrational spectra and heat flow at the sub-nanometer scale. Here, using spatially-resolved ultrafast thermoreflectance and spectroscopy, we uncover the design rules governing cross-plane heat transport in superlattices assembled from monolayers of graphene (G) and MoS2 (M). Using a combinatorial experimental approach, we probe nine different stacking sequences: G, GG, MG, GGG, GMG, GGMG, GMGG, GMMG, GMGMG and identify the effects of vibrational mismatch, inte…
The photo-excitation of multi-layered potassium doped black phosphorus that exists as a gapped semi-Dirac two-dimensional normal insulator (NI), transforms it into a time-reversal symmetry broken Chern insulator (CI). This transition from an NI to CI happens under a high-frequency radiation corresponding to the off-resonant regime of the Floquet theory of periodic perturbations, which here is the impinging light beam. This photo-induced topological CI phase manifests as a finite Berry curvature and forms the basis of anomalous transverse heat flow in presence of a longitudinal temperature grad…
We present a comprehensive study of the band structure of two- and three-dimensional hexagonal layered materials using Landau Level optical Hall effect spectroscopy investigations, employing graphene and graphite as model systems. We study inter-Landau-level transitions in highly oriented pyrolytic graphite and a stack of multilayer graphene on C-face 6\textit{H}-SiC, using data from reflection-type optical Hall effect measurements in the mid-infrared spectral range at sample temperatures of $T=1.5$~K and magnetic fields up to $B=8$~T. We describe a comprehensive dielectric polarizability mode…
2D materials based superlattices have emerged as a promising platform to modulate band structure and its symmetries. In particular, moiré periodicity in twisted graphene systems produces flat Chern bands. The recent observation of anomalous Hall effect (AHE) and orbital magnetism in twisted bilayer graphene has been associated with spontaneous symmetry breaking of such Chern bands. However, the valley Hall state as a precursor of AHE state, when time-reversal symmetry is still protected, has not been observed. Our work probes this precursor state using the valley Hall effect. We show that brok…
The symmetry group analysis is applied to classify the phonon modes of $N$-stacked graphene layers (NSGL's) with AB- and AA-stacking, particularly their infra-red and Raman properties. The dispersions of various phonon modes are calculated in a multi-layer vibrational model, which is generalized from the lattice vibrational potentials of graphene to including the inter-layer interactions in NSGL's. The experimentally reported red shift phenomena in the layer number dependence of the intra-layer optical C-C stretching mode frequencies are interpreted. An interesting low frequency inter-layer op…
It is of keen interest to researchers understanding different approaches to confine massless Dirac fermions in graphene, which is also a central problem in making electronic devices based on graphene. Here, we studied spatial confinement, magnetic localization and their interactions on massless Dirac fermions in an angled graphene wedge formed by two linear graphene p-n boundaries with an angle 34. Using scanning tunneling microscopy, we visualized quasibound states temporarily confined in the studied graphene wedge. Large perpendicular magnetic fields condensed the massless Dirac fermions in …
Graphene-based membranes have been investigated as promising candidates for water filtration and gas separation applications. Experimental evidences have shown that graphene oxide can be impermeable to liquids, vapors and gases, while allowing a fast permeation of water molecules. This phenomenon has been attributed to the formation of a network of nano capillaries that allow nearly frictionless water flow while blocking other molecules by steric hindrance effects. It is supposed that water molecules are transported through the percolated two-dimensional channels formed between graphene-based …
Bilayer graphene and its thicker cousins with Rhombohedral stacking have attracted considerable attention because of their susceptibility to a variety of broken chiral symmetry states. Due to large density-of-states and quantized Berry phases near their gapless band touching points, each spin-valley flavor spontaneously transfers charge between layers to yield opening of energy gaps in quasiparticle spectra and spreading of momentum-space Berry curvatures. In this article we review the development of theories that predicted such chiral symmetry breaking and classified the possible topological …
The ability to engineer the electronic band structure and, more strikingly, to access new exotic phase of matter has been the cornerstone of the advance of science and technology. Twisting van der Waals materials to form moiré superlattice is a powerful paradigm and can drive graphene from a normal metallic state into an insulating, superconducting, or ferromagnetic states. Here, we present a new route to create non-trivial band structure and consequently an exotic phase of matter via lithographically patterned strain (lattice deformation). This method is used to realize an artificially corrug…
The discovery of graphene has spurred vigorous investigation of 2D materials, revealing a wide range of extraordinary properties and functionalities. 2D heterostructural materials have recently been fabricated by assembling isolated planes layer-by-layer in a desired sequence. Unusual properties and novel physical phenomena have been unveiled in such layered heterostructures. For example, Hofstadter's butterfly, an intriguing pattern of the energy states of Bloch electrons, was predicted several decades ago to be observable only under unfeasibly strong magnetic fields in conventional materials…
Properties of many layered materials, including copper- and iron-based superconductors, topological insulators, graphite and epitaxial graphene can be manipulated by inclusion of different atomic and molecular species between the layers via a process known as intercalation. For example, intercalation in graphite can lead to superconductivity and is crucial in the working cycle of modern batteries and supercapacitors. Intercalation involves complex diffusion processes along and across the layers, but the microscopic mechanisms and dynamics of these processes are not well understood. Here we rep…
Transport properties of multigraphene layers on 6H-SiC substrates fabricated by thermal graphitization of SiC were studied. The principal result is that these structures were shown to contain a nearly perfect graphene layer situated between the SiC substrate and multgraphene layer. It was found that the curves of magnetoresistance and Shubnikov- de Haas oscillations shown the features, typical for single-layered graphene. The low temperature resistance demonstrated an increase with temperature increase, which also corresponds to a behavior typical for single-layered graphene (antilocalization)…
Electron-phonon scatterings in solid-state systems are pivotal processes in determining many key physical quantities such as charge carrier mobilities and thermal conductivities. Here, we report on the direct probing of phonon mode specific electron-phonon scatterings in layered semiconducting transition metal dichalcogenides WSe2, MoSe2, WS2, and MoS2 through inelastic electron tunneling spectroscopy measurements, quantum transport simulations, and density functional calculation. We experimentally and theoretically characterize momentum-conserving single- and two-phonon electron-phonon scatte…
Surfactants are often used to stabilise two-dimensional (2D) materials in environmentally friendly solvents such as water. Aqueous-surfactant solutions prevent agglomeration of nanosheets through steric and electrostatic repulsion, facilitating the production of high concentration nanomaterial dispersions. Turbulent, shear-assisted liquid exfoliation of layered precursor materials produces defect-free nanosheets by promoting mixing and generating sufficiently high shear rates to overcome out-of-plane van der Waals bonds. In the presence of a liquid-gas interface, a consequence of using surfact…
Compressed hydrogen passes through a series of layered structures in which the layers can be viewed as distorted graphene sheets. The electronic structures of these layered structures can be understood by studying simple model systems- an ideal single hydrogen graphene sheet and three-dimensional model lattices consisting of such sheets. The energetically stable structures result from structural distortions of model graphene-based systems due to electronic instabilities towards Peierls or other distortions associated with the opening of a band gap. Two factors play crucial roles in the metalli…
By using first-principles calculations, we investigated the effects of graphene/boron nitride (BN) encapsulation, surface functionalization by metallic elements (K, Al, Mg and typical transition metals) and molecules (tetracyanoquinodimethane (TCNQ) and tetracyanoethylene (TCNE)) on the electronic properties of layered indium selenide (InSe). It was found that an opposite trend of charge transfer is possible for graphene (donor) and BN (acceptor), which is dramatically different from phosphorene where both graphene and BN play the same role (donor). For InSe/BN heterostructure, a change of the…
The marriage between a two-dimensional layered material (2DLM) and a complex transition metal oxide (TMO) results in a variety of physical and chemical phenomena that would not have been achieved in either material alone. Interesting recent discoveries in systems such as graphene/SrTiO3, graphene/LaAlO3/SrTiO3, graphene/ferroelectric oxide, MoS2/SrTiO3, and FeSe/SrTiO3 heterostructures include voltage scaling in field-effect transistors, charge state coupling across an interface, quantum conductance probing of the electrochemical activity, novel memory functions based on charge traps, and grea…
Van der Waals heterostructure based on layered two-dimensional (2D) materials offers unprecedented opportunities to create materials with atomic precision by design. By combining superior properties of each component, such heterostructure also provides possible solutions to address various challenges of the electronic devices, especially those with vertical multilayered structures. Here, we report the realization of robust memristors for the first time based on van der Waals heterostructure of fully layered 2D materials (graphene/MoS2-xOx/graphene) and demonstrate a good thermal stability lack…
Ultrasonication is widely used to exfoliate two dimensional (2D) van der Waals layered materials such as graphene. Its fundamental mechanism, inertial cavitation, is poorly understood and often ignored in ultrasonication strategies resulting in low exfoliation rates, low material yields and wide flake size distributions, making the graphene dispersions produced by ultrasonication less economically viable. Here we report that few-layer graphene yields of up to 18% in three hours without introduction of basal plane defects can be achieved by optimising inertial cavitation during ultrasonication.…
