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The origin of superconductivity in magic-angle twisted bilayer graphene has been a subject of intense debate. While some experimental evidence indicated an unconventional pairing mechanism, efforts to tune the critical temperature by screening the Coulomb interactions have been unsuccessful, possibly indicating a conventional phonon-mediated pairing. Here we study a double-layer electronic system consisting of two twisted graphene bilayers in immediate proximity of each other but remaining electronically decoupled. By increasing the carrier density in one bilayer, we completely suppressed both the superconductivity and the correlated-insulator state in the adjacent magic-angle graphene. The observation of such a screening effect offers strong support for an unconventional mechanism of Cooper pairing in magic-angle twisted bilayer graphene, shedding new light on the underlying physics governing their properties., Comment: 25 pages, 9 figures

Two-dimensional (2D) materials with remarkable second-harmonic generation (SHG) hold promise for future on-chip nonlinear optics. Relevant materials with both giant SHG response and environmental stability are long-sought targets. Here, we demonstrate the enormous SHG from the phase engineering of a high-performance semiconductor, Bi$_2$O$_2$Se (BOS), under uniaxial strain. SHG signals captured in strained 20 nm-BOS films exceed those of NbOI$_2$ and NbOCl$_2$ of similar thickness by a factor of 10, and are four orders of magnitude higher than monolayer-MoS$_2$, resulting in a significant second-order nonlinear susceptibility on the order of 1 nm V$^{-1}$. Intriguingly, the strain enables continuous adjustment of the ferroelectric phase transition across room temperature. Consequently, an exceptionally large tunability of SHG, approximately six orders of magnitude, is achieved through strain or thermal modulation. This colossal SHG, originating from the geometric phase of Bloch wave functions and coupled with sensitive tunability through multiple approaches in this air-stable 2D semiconductor, opens new possibilities for designing chip-scale, switchable nonlinear optical devices.

Chern insulators host topologically protected chiral edge currents with quantized conductance characterized by their Chern number. Switching the chirality of a Chern insulator, namely, the direction of the edge current, is highly challenging due to topologically forbidden backscattering but is of considerable importance for the design of topological devices. Nevertheless, this can be achieved by reversing the sign of the Chern number through a topological phase transition. Here, we report electrically switchable chirality in rhombohedral multilayer graphene-based Chern insulators. By introducing moire superlattices in rhombohedral heptalayer graphene, we observed a cascade of topological phase transitions at quarter electron filling of a moire band with the Chern number tunable from -1, 1 to 2. Furthermore, integrating monolayer tungsten diselenide at the moireless interface of rhombohedral decalayer graphene/h-BN superlattices stabilizes the Chern insulators, enabling quantized anomalous Hall resistance of h/2e^2. Remarkably, the Chern number can be switched from -1 to 2 using displacement fields. Our work establishes rhombohedral multilayer graphene moire superlattices as a versatile platform for topological engineering, with switchable chirality offering significant promise for integrating chiral edge currents into topological electronic circuits., Comment: Include the data from 10L graphene devices. To appear in Physical Review X

The stacking order and twist angle provide abundant opportunities for engineering band structures of two-dimensional materials, including the formation of moire bands, flat bands, and topologically nontrivial bands. The inversion symmetry breaking in rhombohedral-stacked transitional metal dichalcogenides (TMDCs) endows them with an interfacial ferroelectricity associated with an out-of-plane electric polarization. By utilizing twist angle as a knob to construct rhombohedral-stacked TMDCs, antiferroelectric domain networks with alternating out-of-plane polarization can be generated. Here, we demonstrate that such spatially periodic ferroelectric polarizations in parallel-stacked twisted WSe2 can imprint their moire potential onto a remote bilayer graphene. This remote moire potential gives rise to pronounced satellite resistance peaks besides the charge-neutrality point in graphene, which are tunable by the twist angle of WSe2. Our observations of ferroelectric hysteresis at finite displacement fields suggest the moire is delivered by a long-range electrostatic potential. The constructed superlattices by moire ferroelectricity represent a highly flexible approach, as they involve the separation of the moire construction layer from the electronic transport layer. This remote moire is identified as a weak potential and can coexist with conventional moire. Our results offer a comprehensive strategy for engineering band structures and properties of two-dimensional materials by utilizing moire ferroelectricity.

Ferroelectricity is intriguing for its spontaneous electric polarization, which is switchable by an external electric field. Expanding ferroelectric materials to two-dimensional limit will provide versatile applications for the development of next-generation nonvolatile devices. Conventional ferroelectricity requires the materials consisting of at least two constituent elements associated with polar crystalline structures. Monolayer graphene as an elementary two-dimensional material unlikely exhibits ferroelectric order due to its highly centrosymmetric hexagonal lattices. Nevertheless, two-dimensional moire superlattices offer a powerful way to engineer diverse electronic orders in non-polar materials. Here, we report the observations of electronic ferroelectricity in monolayer graphene by introducing asymmetric moire superlattice at the graphene/h-BN interface. Utilizing Hall measurements, the electric polarization is identified to stem from electron-hole dipoles, suggesting the electronic dynamics of the observed ferroelectricity. Standard polarization-electric field hysteresis loops, as well as unconventional multiple switchable polarization states, have been achieved. By in-situ comparing with control devices, we found that the electronic ferroelectricity in graphene moire systems is independent of layer number of graphene and the corresponding fine band structures. Furthermore, we demonstrate the applications of this ferroelectric moire structures in multi-state non-volatile data storage and the emulation of versatile synaptic behaviors, including short-term plasticity, long-term potentiation and long-term depression. This work not only enriches the fundamental understanding of ferroelectricity, but also demonstrates the promising applications of graphene in multi-state memories and neuromorphic computing.

Symmetry breaking governs most fascinating phenomena in crystals, such as ferroelectricity, nonlinear optics, piezoelectricity, ferromagnetism, and superconductivity. In two-dimensional materials, a wide variety of tuning knobs presents extraordinary opportunities for engineering symmetry breaking, leading to the emergence and manipulation of novel physical properties. Recently, tetralayer graphene with ABCB stacking order is predicted to possess atypical elemental ferroelectricity arising from the symmetry breaking induced by its specific stacking configuration. Experimentally unveiling the stacking-order dependent symmetry in tetralayer graphene is crucial to understand the intricate properties in the emergent graphene allotropes. Here, we observe pronounced nonlinear optical second harmonic generation (SHG) in ABCB-stacked tetralayer graphene, but absent in both ABAB- and ABCA-stacked allotropes. Our results provide direct evidence of symmetry breaking in ABCB-stacked tetralayer graphene. The remarkable contrast in the SHG spectra of tetralayer graphene allows straightforward identification of ABCB domains from the other two kinds of stacking order and facilitates the characterization of their crystalline orientation. The employed SHG technique serves as a convenient tool for exploring the intriguing physics and novel nonlinear optics in ABCB-stacked graphene, where spontaneous polarization and intrinsic gapped flat bands coexist. Our results establish ABCB-stacked graphene as a unique platform for studying the rare ferroelectricity in non-centrosymmetric elemental structures.

Van der Waals assembly enables exquisite design of electronic states in two-dimensional (2D) materials, often by superimposing a long-wavelength periodic potential on a crystal lattice using moir\'e superlattices. Here we show that electronic states in three-dimensional (3D) crystals such as graphite can also be tuned by the superlattice potential arising at the interface with another crystal, namely, crystallographically aligned hexagonal boron nitride. Such alignment is found to result in a multitude of Lifshitz transitions and Brown-Zak oscillations for near-surface 2D states whereas, in high magnetic fields, fractal states of Hofstadter's butterfly extend deep into graphite's bulk. Our work shows a venue to control 3D spectra by using the approach of 2D twistronics.

Twisted heterostructures of two-dimensional crystals offer almost unlimited scope for the design of novel metamaterials. Here we demonstrate a room-temperature ferroelectric semiconductor that is assembled using mono- or few- layer MoS2. These van der Waals heterostructures feature broken inversion symmetry, which, together with the asymmetry of atomic arrangement at the interface of two 2D crystals, enables ferroelectric domains with alternating out-of-plane polarisation arranged into a twist-controlled network. The latter can be moved by applying out-of-plane electrical fields, as visualized in situ using channelling contrast electron microscopy. The interfacial charge transfer for the observed ferroelectric domains is quantified using Kelvin probe force microscopy and agrees well with theoretical calculations. The movement of domain walls and their bending rigidity also agrees well with our modelling results. Furthermore, we demonstrate proof-of-principle field-effect transistors, where the channel resistance exhibits a pronounced hysteresis governed by pinning of ferroelectric domain walls. Our results show a potential venue towards room temperature electronic and optoelectronic semiconductor devices with built-in ferroelectric memory functions., Comment: 15 pages, 3 figures

Electrically interfacing atomically thin transition metal dichalcogenide semiconductors (TMDSCs) with metal leads is challenging because of undesired interface barriers, which have drastically constrained the electrical performance of TMDSC devices for exploring their unconventional physical properties and realizing potential electronic applications. Here we demonstrate a strategy to achieve nearly barrier-free electrical contacts with few-layer TMDSCs by engineering interfacial bonding distortion. The carrier-injection efficiency of such electrical junction is substantially increased with robust ohmic behaviors from room to cryogenic temperatures. The performance enhancements of TMDSC field-effect transistors are well reflected by the ultralow contact resistance (down to 90 Ohm um in MoS2, towards the quantum limit), the ultrahigh field-effect mobility (up to 358,000 cm2V-1s-1 in WSe2) and the prominent transport characteristics at cryogenic temperatures. This method also offers new possibilities of the local manipulation of structures and electronic properties for TMDSC device design.

In thermodynamic equilibrium, current in metallic systems is carried by electronic states near the Fermi energy whereas the filled bands underneath contribute little to conduction. Here we describe a very different regime in which carrier distribution in graphene and its superlattices is shifted so far from equilibrium that the filled bands start playing an essential role, leading to a critical-current behavior. The criticalities develop upon the velocity of electron flow reaching the Fermi velocity. Key signatures of the out-of-equilibrium state are current-voltage characteristics resembling those of superconductors, sharp peaks in differential resistance, sign reversal of the Hall effect, and a marked anomaly caused by the Schwinger-like production of hot electron-hole plasma. The observed behavior is expected to be common for all graphene-based superlattices., Comment: 22 pages, 11 figures

In van der Waals heterostructures, electronic bands of two-dimensional (2D) materials, their nontrivial topology, and electron-electron interactions can be dramatically changed by a moire pattern induced by twist angles between different layers. Such process is referred to as twistronics, where the tuning of twist angle can be realized through mechanical manipulation of 2D materials. Here we demonstrate an experimental technique that can achieve in situ dynamical rotation and manipulation of 2D materials in van der Waals heterostructures. Using this technique we fabricated heterostructures where graphene is perfectly aligned with both top and bottom encapsulating layers of hexagonal boron nitride. Our technique enables twisted 2D material systems in one single stack with dynamically tunable optical, mechanical, and electronic properties.

The rectification of electromagnetic waves to direct currents is a crucial process for energy harvesting, beyond-5G wireless communications, ultra-fast science, and observational astronomy. As the radiation frequency is raised to the sub-terahertz (THz) domain, ac-to-dc conversion by conventional electronics becomes challenging and requires alternative rectification protocols. Here we address this challenge by tunnel field-effect transistors made of bilayer graphene (BLG). Taking advantage of BLG's electrically tunable band structure, we create a lateral tunnel junction and couple it to an antenna exposed to THz radiation. The incoming radiation is then down-converted by the tunnel junction nonlinearity, resulting in high-responsivity (> 4 kV/W) and low-noise (0.2 pW/$\sqrt{\mathrm{Hz}}$}) detection. We demonstrate how switching from intraband Ohmic to interband tunneling regime can raise detectors' responsivity by few orders of magnitude, in agreement with the developed theory. Our work demonstrates a potential application of tunnel transistors for THz detection and reveals BLG as a promising platform therefor.

Understanding and tuning correlated states is of great interest and significance to modern condensed matter physics. The recent discovery of unconventional superconductivity and Mott-like insulating states in magic-angle twisted bilayer graphene (tBLG) presents a unique platform to study correlation phenomena, in which the Coulomb energy dominates over the quenched kinetic energy as a result of hybridized flat bands. Extending this approach to the case of twisted multilayer graphene would allow even higher control over the band structure because of the reduced symmetry of the system. Here, we study electronic transport properties in twisted trilayer graphene (tTLG, bilayer on top of monolayer graphene heterostructure). We observed the formation of van Hove singularities which are highly tunable by twist angle and displacement field and can cause strong correlation effects under optimum conditions, including superconducting states. We provide basic theoretical interpretation of the observed electronic structure., Comment: 16 pages, 9 figures

When two-dimensional atomic crystals are brought into close proximity to form a van der Waals heterostructure, neighbouring crystals can start influencing each others electronic properties. Of particular interest is the situation when the periodicity of the two crystals closely match and a moir\'e pattern forms, which results in specific electron scattering, reconstruction of electronic and excitonic spectra, crystal reconstruction, and many other effects. Thus, formation of moir\'e patterns is a viable tool of controlling the electronic properties of 2D materials. At the same time, the difference in the interatomic distances for the two crystals combined, determines the range in which the electronic spectrum is reconstructed, and thus is a barrier to the low energy regime. Here we present a way which allows spectrum reconstruction at all energies. By using graphene which is aligned simultaneously to two hexagonal boron nitride layers, one can make electrons scatter in the differential moir\'e pattern, which can have arbitrarily small wavevector and, thus results in spectrum reconstruction at arbitrarily low energies. We demonstrate that the strength of such a potential relies crucially on the atomic reconstruction of graphene within the differential moir\'e super-cell. Such structures offer further opportunity in tuning the electronic spectra of two-dimensional materials., Comment: 35 pages, 15 figures

Of the two stable forms of graphite, hexagonal (HG) and rhombohedral (RG), the former is more common and has been studied extensively. RG is less stable, which so far precluded its detailed investigation, despite many theoretical predictions about the abundance of exotic interaction-induced physics. Advances in van der Waals heterostructure technology have now allowed us to make high-quality RG films up to 50 graphene layers thick and study their transport properties. We find that the bulk electronic states in such RG are gapped and, at low temperatures, electron transport is dominated by surface states. Because of topological protection, the surface states are robust and of high quality, allowing the observation of the quantum Hall effect, where RG exhibits phase transitions between gapless semimetallic phase and gapped quantum spin Hall phase with giant Berry curvature. An energy gap can also be opened in the surface states by breaking their inversion symmetry via applying a perpendicular electric field. Moreover, in RG films thinner than 4 nm, a gap is present even without an external electric field. This spontaneous gap opening shows pronounced hysteresis and other signatures characteristic of electronic phase separation, which we attribute to emergence of strongly-correlated electronic surface states., Comment: 18 pages, 12 figures

In graphite crystals, layers of graphene reside in three equivalent, but distinct, stacking positions typically referred to as A, B, and C projections. The order in which the layers are stacked defines the electronic structure of the crystal, providing an exciting degree of freedom which can be exploited for designing graphitic materials with unusual properties including predicted high-temperature superconductivity and ferromagnetism. However, the lack of control of the stacking sequence limits most research to the stable ABA form of graphite. Here we demonstrate a strategy to control the stacking order using van der Waals technology. To this end, we first visualise the distribution of stacking domains in graphite films and then perform directional encapsulation of ABC-rich graphite crystallites with hexagonal boron nitride (hBN). We found that hBN-encapsulation which is introduced parallel to the graphite zigzag edges preserves ABC stacking, while encapsulation along the armchair edges transforms the stacking to ABA. The technique presented here should facilitate new research on the important properties of ABC graphite.

Electrons hopping in two-dimensional honeycomb lattices possess a valley degree of freedom in addition to charge and spin. In the absence of inversion symmetry, these systems were predicted to exhibit opposite Hall effects for electrons from different valleys. Such valley Hall effects have been achieved only by extrinsic means, such as substrate coupling, dual gating, and light illuminating. Here, we report the first observation of intrinsic valley Hall transport without any extrinsic symmetry breaking in the non-centrosymmetric monolayer and trilayer MoS2, evidenced by considerable nonlocal resistance that scales cubically with local resistance. Such a hallmark survives even at room temperature with a valley diffusion length at micron scale. By contrast, no valley Hall signal is observed in the centrosymmetric bilayer MoS2. Our work elucidates the topological quantum origin of valley Hall effects and marks a significant step towards the purely electrical control of valley degree of freedom in topological valleytronics., Comment: 22 pages, 4 figures

Monolayer transition metal dichalcogenides are recently emerged 2D electronic systems with various novel properties, such as spin-valley locking, circular dichroism, valley Hall effects, Ising superconductivity. The reduced dimensionality and large effective masses further produce unconventional many-body interaction effects. Although recent hole transport measurements in WSe$_2$ indicate strong interactions in the valence bands, many-body interaction effects, particularly in the conduction bands, remain elusive to date. Here, for the first time, we perform transport measurements up to a magnetic field of $29$T to study the massive Dirac electron Landau levels (LL) in layer-polarized MoS$_2$ samples with mobilities of $22000$cm$^2$/(V$\cdot$s) at $1.5$K and densities of $\sim10^{12}$cm$^{-2}$. With decreasing the density, we observe LL crossing induced valley ferrimagnet-to-ferromagnet transitions, as a result of the interaction enhancement of the g-factor from $5.64$ to $21.82$. Near integer ratios of Zeeman-to-cyclotron energies, we discover LL anticrossings due to the formation of quantum Hall Ising ferromagnets, the valley polarizations of which appear to be reversible by tuning the density or an in-plane magnetic field. Our results provide compelling evidence for many-body interaction effects in the conduction bands of monolayer MoS$_2$ and establish a fertile ground for exploring strongly correlated phenomena of massive Dirac electrons., Comment: 21 pages, 4 figures

This work reports an experimental study on an antiferromagnetic honeycomb lattice of MnPS$_3$ that couples the valley degree of freedom to a macroscopic antiferromagnetic order. The crystal structure of MnPS$_3$ is identified by high resolution scanning transmission electron microscopy. Layer dependent angle resolved polarized Raman fingerprints of the MnPS$_3$ crystal are obtained and the Raman peak at 383 cm$^{-1}$ exhibits 100% polarity. Temperature dependences of anisotropic magnetic susceptibility of MnPS$_3$ crystal are measured in superconducting quantum interference device. Magnetic parameters like effective magnetic moment, and exchange interaction are extracted from the mean field approximation mode. Ambipolar electronic transport channels in MnPS$_3$ are realized by the liquid gating technique. The conducting channel of MnPS$_3$ offers a unique platform for exploring the spin/valleytronics and magnetic orders in 2D limitation., Comment: 16 pages, 6 figures

Atomically thin transition metal dichalcogenides (TMDCs) such as MoS$_2$ and WSe$_2$ are emerging as a new platform for exploring many-body effects. Coulomb interactions are markedly enhanced in these materials because of the reduced screening and the large Wigner-Seitz radii. Although many-body excitonic effects in TMDCs have been extensively studied by optical means, not until recently did probing their strongly correlated electronic effects become possible in transport. Here, in p-type few-layer WSe$_2$ we observe highly density-dependent quantum Hall states of {\Gamma} valley holes below 12 T, whose predominant sequences alternate between odd- and even-integers. By tilting the magnetic field to induce Landau level crossings, we show that the strong Coulomb interaction enhances the Zeeman-to-cyclotron energy ratio from 2.67 to 3.55 as the density is reduced from 5.7 to 4.0$\times$10$^{12}$ cm$^{-2}$, giving rise to the even-odd alternation. Unprecedentedly, this indicates a 4.8 times enhancement of the g-factor over its band theory value at a density as high as 4.0$\times$10$^{12}$ cm$^{-2}$. Our findings unambiguously demonstrate that p-type few-layer WSe$_2$ is a superior platform for exploring strongly correlated electronic phenomena, opening a new perspective for realizing the elusive Wigner crystallization at a moderate density., Comment: 13 pages, 4 figures. Main text and figures are updated

Few-layer black phosphorus possesses unique electronic properties giving rise to distinct quantum phenomena and thus offers a fertile platform to explore the emergent correlation phenomena in low dimensions. A great progress has been demonstrated in improving the quality of hole-doped few-layer black phosphorus and its quantum transport studies, whereas the same achievements are rather modest for electron-doped few-layer black phosphorus. Here, we report the ambipolar quantum transport in few-layer black phosphorus exhibiting undoubtedly the quantum Hall effect for hole transport and showing clear signatures of the quantum Hall effect for electron transport. By bringing the spin-resolved Landau levels of the electron-doped black phosphorus to the coincidence, we measure the spin susceptibility $\chi_s=m^\ast g^\ast=1.1\pm0.03$. This value is larger than for hole-doped black phosphorus and illustrates an energetically equidistant arrangement of spin-resolved Landau levels. Evidently, the n-type black phosphorus offers a unique platform with equidistant sequence of spin-up and spin-down states for exploring the quantum spintronic.

Atomically thin black phosphorus (BP) field-effect transistors show strong-weak localization transition which is tunable through gate voltages. Hopping transports through charge impurity induced localized states are measured at low-carrier density regime. Variable-range hopping model is applied to simulate the charge carrier scattering behavior. In the high-carrier concentration regime, a negative magnetoresistance signals the weak localization effect. The extracted phase coherence length is power-law temperature dependent ($\sim T^{-0.48\pm0.03}$) and demonstrates electron-electron interactions in few-layer BP. The competition between the Strong localization length and phase coherence length is proposed and discussed based on the observed gate tunable strong-weak localization transition in few-layer BP.

We fabricate high-mobility p-type few-layer WSe2 field-effect transistors and surprisingly observe a series of quantum Hall (QH) states following an unconventional sequence predominated by odd-integer states under a moderate strength magnetic field. By tilting the magnetic field, we discover Landau level (LL) crossing effects at ultra-low coincident angles, revealing that the Zeeman energy is about three times as large as the cyclotron energy near the valence band top at {\Gamma} valley. This result implies the significant roles played by the exchange interactions in p-type few-layer WSe2, in which itinerant or QH ferromagnetism likely occurs. Evidently, the {\Gamma} valley of few-layer WSe2 offers a unique platform with unusually heavy hole-carriers and a substantially enhanced g-factor for exploring strongly correlated phenomena., Comment: To appear in Physical Review Letters, including the Supplemental Material

Topological states of matter originate from distinct topological electronic structures of materials. As for strong topological insulators (STIs), the topological surface (interface) is a direct consequence of electronic structure transition between materials categorized to different topological genus. Therefore, it is fundamentally interesting if such topological character can be manipulated. Besides tuning the crystal field and the strength of spin-orbital coupling (e.g., by external strain, or chemical doping), there is currently rare report on topological state induced in ordinary insulators (OIs) by the heterostructure of OI/STI. Here we report the observation of a Dirac cone topological surface state (TSS) induced on the Sb2Se3 layer up to 15 nm thick in the OI/STI heterostructure, in sharp contrast with the OI/OI heterostructure where no sign of TSS can be observed. This is evident for an induced topological state in an OI by heterostructure.

We demonstrate that charge density wave (CDW) phase transition occurs on the surface of electronically doped multilayer graphene when the Fermi level approaches the M points (also known as van Hove singularities where the density of states diverge) in the Brillouin zone of graphene band structure. The occurrence of such CDW phase transitions are supported by both the electrical transport measurement and optical measurements in electrostatically doped multilayer graphene. The CDW transition is accompanied with the sudden change of graphene channel resistance at T$_m$= 100K, as well as the splitting of Raman G peak (1580 cm$^{-1}$). The splitting of Raman G peak indicats the lifting of in-plane optical phonon branch degeneracy and the non-degenerate phonon branches are correlated to the lattice reconstructions of graphene -- the CDW phase transition., Comment: 13 Pages, 4 Figures

We demonstrate that encapsulation of atomically thin black phosphorus (BP) by hexagonal boron nitride (h-BN) sheets is very effective for minimizing the interface impurities induced during fabrication of BP channel material for quantum transport nanodevices. Highly stable BP nanodevices with ultrahigh mobility and controllable types are realized through depositing appropriate metal electrodes after conducting a selective etching to the BP encapsulation structure. Chromium and titanium are suitable metal electrodes for BP channels to control the transition from a p-type unipolar property to ambipolar characteristic because of different work functions. Record-high mobilities of 6000 $cm^2V^{-1}s^{-1}$ and 8400 $cm^2V^{-1}s^{-1}$ are respectively obtained for electrons and holes at cryogenic temperatures. High-mobility BP devices enable the investigation of quantum oscillations with an indistinguishable Zeeman effect in laboratory magnetic field., Comment: 14 pages, 3 figures

Atomically thin black phosphorus (BP) is a promising two-dimensional material for fabricating electronic and optoelectronic nano-devices with high mobility and tunable bandgap structures. However, the charge-carrier mobility in few-layer phosphorene (monolayer BP) is mainly limited by the presence of impurity and disorders. In this study, we demonstrate that vertical BP heterostructure devices offer great advantages in probing the electron states of monolayer and few-layer phosphorene at temperatures down to 2 K through capacitance spectroscopy. Electronic states in the conduction and valence bands of phosphorene are accessible over a wide range of temperature and frequency. Exponential band tails have been determined to be related to disorders. Unusual phenomena such as the large temperature-dependence of the electron state population in few-layer phosphorene have been observed and systematically studied. By combining the first-principles calculation, we identified that the thermal excitation of charge trap states and oxidation-induced defect states were the main reasons for this large temperature dependence of the electron state population and degradation of the on-off ratio in phosphorene field-effect transistors., Comment: 15 pages, 7 figures, 2D Materials, Volume 3, Number 1(2016)

Interfaces between exfoliated topological insulator Bi2Se3 and several transition metals deposited by sputtering were studied by XPS, SIMS, UPS and contact I-V measurements. Chemically clean interfaces can be achieved when coating Bi2Se3 with a transition metal layer as thin as 1 nm, even without capping. Most interestingly, UPS spectra suggest depletion or inversion in the originally n-type topological insulator near the interface. Strong band bending in the topological insulator requires careful material engineering or electric biasing if one desires to make use of the spin locking in surface states in the bulk gap for potential spintronic applications, Comment: 8 pages, 5 figures

In few-layer (FL) transition metal dichalcogenides (TMDC), the conduction bands along the Gamma-K directions shift downward energetically in the presence of interlayer interactions, forming six Q valleys related by three-fold rotational symmetry and time reversal symmetry. In even-layers the extra inversion symmetry requires all states to be Kramers degenerate, whereas in odd-layers the intrinsic inversion asymmetry dictates the Q valleys to be spin-valley coupled. In this Letter, we report the transport characterization of prominent Shubnikov-de Hass (SdH) oscillations for the Q valley electrons in FL transition metal disulfide (TMDs), as well as the first quantum Hall effect (QHE) in TMDCs. Our devices exhibit ultrahigh field-effect mobilities (~16,000 cm2V-1s-1 for FL WS2 and ~10,500 cm2V-1s-1 for FL MoS2) at cryogenic temperatures. Universally in the SdH oscillations, we observe a valley Zeeman effect in all odd-layer TMD devices and a spin Zeeman effect in all even-layer TMD devices., Comment: 20 pages, 4 figures

Negative compressibility generated by many-body effects in 2D electronic systems can enhance gate capacitance. We observe capacitance enhancement in a newly emerged 2D layered material, atomically thin black phosphorus (BP). The encapsulation of BP by hexagonal boron nitride sheets with few-layer graphene as a terminal ensures ultraclean heterostructure interfaces, allowing us to observe negative compressibility at low hole carrier concentrations. We explained the negative compressibility based on the Coulomb correlation among in-plane charges and their image charges in a gate electrode in the framework of Debye screening.

We demonstrate that a field effect transistor (FET) made of few layer black phosphorus (BP) encapsulated in hexagonal boron nitride (h-BN) in vacuum, exhibts the room temperature hole mobility of 5200 $cm^2/Vs$ being limited just by the phonon scattering. At cryogenic tempeature the FET mobility increases up to 45,000 $cm^2/Vs$, which is eight times higher compared with the mobility obtained in earlier reports. The unprecedentedly clean h-BN/BP/h-BN heterostructure exhibits Shubnikov-de Haas oscillations and quantum Hall effect with Landau level (LL) filling factors down to v=2 in conventional laboratory magnetic fields. Moreover, carrier density independent effective mass m=0.26 m_0 is measured, and Lande g-factor g=2.47 is reported. Furthermore, an indication for a distinct hole transport behavior with up and down spin orientation is found., Comment: 30 pages, 12 figures

The transfer-free synthesis of high-quality, large-area graphene on a given dielectric substrate, which is highly desirable for device applications, remains a significant challenge. In this paper, we report on a simple rapid thermal treatment method for the fast and direct growth of high-quality, large-scale monolayer graphene on a SiO2/Si substrate from solid carbon sources. The stack structure of solid carbon layer/copper film/SiO2 is adopted in the RTT process. The inserted copper film does not only act as an active catalyst for the carbon precursor but also serves as a "filter" that prevents premature carbon dissolution, and thus, contributes to monolayer graphene growth on SiO2/Si. The produced monolayer graphene exhibits high carrier mobility of up to 3000 cm2 V-1s-1 at room temperature and standard half-integer quantum oscillations., Comment: 22 pages, 7 figures

Low carrier mobility and high electrical contact resistance are two major obstacles prohibiting explorations of quantum transport in TMDCs. Here, we demonstrate an effective method to establish low-temperature Ohmic contacts in boron nitride encapsulated TMDC devices based on selective etching and conventional electron-beam evaporation of metal electrodes. This method works for most extensively studied TMDCs in recent years, including MoS2, MoSe2, WSe2, WS2, and 2H-MoTe2. Low electrical contact resistance is achieved at 2 K. All of the few-layer TMDC devices studied show excellent performance with remarkably improved field-effect mobilities ranging from 2300 cm2/V s to 16000 cm2/V s, as verified by the high carrier mobilities extracted from Hall effect measurements. Moreover, both high-mobility n-type and p-type TMDC channels can be realized by simply using appropriate contact metals. Prominent Shubnikov-de Haas oscillations have been observed and investigated in these high-quality TMDC devices., Comment: The methods have been applied to p-type WSe2 and other TMDC based devices. Supplementary information is included

Two-dimensional (2D) materials, such as graphene and transition metal dichalcogenides have attracted great attention because of the rich physics and potential applications in next-generation nano-sized electronic devices. Recently, atomically thin black phosphorus (BP) has become a new member of the 2D materials family with high theoretical mobility and tunable bandgap structure. However, degradation of properties under atmospheric conditions and high-density charge traps in BP have largely limited its mobility (~400 cm2/Vs at room temperature) and thus restricted its future applications. Here, we report the fabrication of stable BN-BP-BN heterostructures by encapsulating atomically thin BP between hexagonal boron nitride (BN) layers to realize ultraclean BN-BP interfaces which allow a record-high field-effect mobility ~1350 cm2/Vs at room temperature and on-off ratios over 10^5. At low temperatures, the mobility reaches ~2700 cm2/Vs and quantum oscillations in BP 2D hole gas are observed at low magnetic fields. Importantly, the BN-BP-BN heterostructure can effectively avoid the quality degradation of BP in ambient condition.

We demonstrate that surface relaxation, which is insignificant in trilayer graphene, starts to manifest in Bernal-stacked tetralayer graphene. Bernal-stacked few-layer graphene has been investigated by analyzing its Landau level spectra through quantum capacitance measurements. We find that in trilayer graphene, the interlayer interaction parameters were similar to that of graphite. However, in tetralayer graphene, the hopping parameters between the bulk and surface bilayers are quite different. This shows a direct evidence for the surface relaxation phenomena. In spite of the fact that the Van der Waals interaction between the carbon layers is thought to be insignificant, we suggest that the interlayer interaction is an important factor in explaining the observed results and the symmetry-breaking effects in graphene sublattice are not negligible.

The metal-insulator transition (MIT) is one of the remarkable electrical transport properties of atomically thin molybdenum disulphide (MoS2). Although the theory of electron-electron interactions has been used in modeling the MIT phenomena in MoS2, the underlying mechanism and detailed MIT process still remain largely unexplored. Here, we demonstrate that the vertical metal-insulator-semiconductor (MIS) heterostructures built from atomically thin MoS2 (monolayers and multilayers) are ideal capacitor structures for probing the electron states in MoS2. The vertical configuration of MIS heterostructures offers the added advantage of eliminating the influence of large impedance at the band tails and allows the observation of fully excited electron states near the surface of MoS2 over a wide excitation frequency (100 Hz-1 MHz) and temperature range (2 K- 300 K). By combining capacitance and transport measurements, we have observed a percolation-type MIT, driven by density inhomogeneities of electron states, in the vertical heterostructures built from monolayer and multilayer MoS2. In addition, the valence band of thin MoS2 layers and their intrinsic properties such as thickness-dependence screening abilities and band gap widths can be easily accessed and precisely determined through the vertical heterostructures.