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In the presence of high magnetic field, quantum Hall systems usually host both even- and odd-integer quantized states because of lifted band degeneracies. Selective control of these quantized states is challenging but essential to understand the exotic ground states and manipulate the spin textures. Here, we study the quantum Hall effect in Bi2O2Se thin films. In magnetic fields as high as 50 T, we observe only even-integer quantum Hall states, but no sign of odd-integer states. However, when reducing the thickness of the epitaxial Bi2O2Se film to one unit cell, we observe both odd- and even-integer states in this Janus (asymmetric) film grown on SrTiO3. By means of a Rashba bilayer model based on ab initio band structures of Bi2O2Se thin films, we can ascribe the absence of odd-integer states in thicker films to the hidden Rasbha effect, where the local inversion symmetry breaking in two sectors of the [Bi2O2]2+ layer yields opposite Rashba spin polarizations, which compensate with each other. In the one unit cell Bi2O2Se film grown on SrTiO3, the asymmetry introduced by top surface and bottom interface induces a net polar field. The resulting global Rashba effect lifts the band degeneracies present in the symmetric case of thicker films., Comment: 6 Figures, 23 pages

Moir\'e superlattices have emerged as a new platform for studying strongly correlated quantum phenomena, but these systems have been largely limited to van der Waals layer two-dimensional (2D) materials. Here we introduce moir\'e superlattices leveraging ultra-thin, ligand-free halide perovskites, facilitated by ionic interactions. Square moir\'e superlattices with varying periodic lengths are clearly visualized through high-resolution transmission electron microscopy. Twist-angle-dependent transient photoluminescence microscopy and electrical characterizations indicate the emergence of localized bright excitons and trapped charge carriers near a twist angle of ~10{\deg}. The localized excitons are accompanied by enhanced exciton emission, attributed to an increased oscillator strength by a theoretically forecasted flat band. This work illustrates the potential of extended ionic interaction in realizing moir\'e physics at room temperature, broadening the horizon for future investigations.

We thank G.P. Mikitik and Yu.V. Sharlai for contributing this note and the cordial exchange about it. First and foremost, we note that the aim of our paper is to report a methodology to diagnose topological (semi)metals using magnetic quantum oscillations. Thus far, such diagnosis has been based on the phase offset of quantum oscillations, which is extracted from a "Landau fan plot". A thorough analysis of the Onsager-Lifshitz-Roth quantization rules has shown that the famous $\pi$-phase shift can equally well arise from orbital- or spin magnetic moments in topologically trivial systems with strong spin-orbit coupling or small effective masses. Therefore, the "Landau fan plot" does not by itself constitute a proof of a topologically nontrivial Fermi surface. In the paper at hand, we report an improved analysis method that exploits the strong energy-dependence of the effective mass in linearly dispersing bands. This leads to a characteristic temperature dependence of the oscillation frequency which is a strong indicator of nontrivial topology, even for multi-band metals with complex Fermi surfaces. Three materials, Cd$_3$As$_2$, Bi$_2$O$_2$Se and LaRhIn$_5$ served as test cases for this method. Linear band dispersions were detected for Cd$_3$As$_2$, as well as the $F$ $\approx$ 7 T pocket in LaRhIn$_5$., Comment: Response to Matter arising for Nature Communications 12, 6213 (2021)

Hydrogen isotope separation has been effectively achieved using gaseous H2/D2 filtered through graphene/Nafion composite membranes. Nevertheless, deuteron nearly does not exist in the form of gaseous D2 in nature but in liquid water. Thus, it is a more feasible way to separate and enrich deuterium from water. Herein we have successfully transferred monolayer graphene to a rigid and porous polymer substrate PITEM (polyimide tracked film), which could avoid the swelling problem of the Nafion substrate, as well as keep the integrity of graphene. Meanwhile, defects in large area of CVD graphene could be successfully repaired by interfacial polymerization resulting in high separation factor. Moreover, a new model was proposed for the proton transport mechanism through monolayer graphene based on the kinetic isotope effect (KIE). In this model, graphene plays the significant role in the H/D separation process by completely breaking the O-H/O-D bond, which can maximize the KIE leading to prompted H/D separation performance. This work suggests a promising application of using monolayer graphene in industry and proposes a pronounced understanding of proton transport in graphene, Comment: 10 pages, 4 figures (6pages, 6figures for SI)

Systematic electrical transport characterizations were performed on high-quality Bi2O2Se nanowires to illustrate its great transport properties and further application potentials in spintronics. Bi2O2Se nanowires synthesized by chemical vapor deposition method presented a high field-effect mobility up to 1.34*104 cm2V-1s-1, and exhibited ballistic transport in the low back-gate voltage (Vg) regime where conductance plateaus were observed. When further increasing the electron density by increasing Vg, we entered the phase coherent regime and weak antilocalization (WAL) was observed. The spin relaxation length extracted from the WAL was found to be gate tunable, ranging from ~100 nm to ~250 nm and reaching a stronger spin-obit coupling (SOC) than the two-dimensional counterpart (flakes). We attribute the strong SOC and the gate tunability to the presence of a surface accumulation layer which induces a strong inversion asymmetry on the surface. Such scenario was supported by the observation of two Shubnikov-de Haas oscillation frequencies that correspond to two types of carriers, one on the surface, and the other in the bulk. The high-quality Bi2O2Se nanowires with a high mobility and a strong SOC can act as a very prospective material in future spintronics., Comment: 22 pages, 7 figures

We report on an experimental study of the effect of coherent surface-bulk electron scattering on quantum transport in a three-dimensional topological insulator Bi$_2$Te$_3$ nanoplate. The nanoplate is grown via van der Waals epitaxy on a mica substrate and a top-gated Hall-bar device is fabricated from the nanoplate directly on the growth substrate. Top-gate voltage dependent measurements of the sheet resistance of the device reveal that the transport carriers in the nanoplate are of n-type and that, with decreasing top gate voltage, the carrier density in the nanoplate is decreased. However, the mobility is increased with decreasing top-gate voltage. This mobility increase with decreasing carrier density in the nanoplate is demonstrated to arise from a decrease in bulk-to-surface electron scattering rate. Low-field magnetotransport measurements are performed at low temperatures. The measured magnetoconductivity of the nanoplate shows typical weak anti-localization (WAL) characteristics. We analyze the measurements by taking surface-bulk inter-channel electron scattering into account and extract dephasing times ${\tau}_{\phi}$, diffusion coefficients $D$ of electrons at the top surface and in the bulk, and the surface-bulk scattering times ${\tau}_{SB}$ as a function of top-gate voltage and temperature. It is found that the dephasing in the nanoplate arises dominantly from electron-electron scattering with small energy transfers. It is also found that the ratio of ${\tau}_{\phi}$/${\tau}_{SB}$ (a measure of the surface-bulk electron coherent coupling) is decreased with decreasing gate voltage or increasing temperature. We demonstrate that taking the surface-bulk coherent electron scattering in our Bi$_2$Te$_3$ nanoplate into account is essential to understand quantum transport measurements at low temperatures., Comment: 15 pages, 3 figures, Supplementary Materials

Many promising optoelectronic devices, such as broadband photodetectors, nonlinear frequency converters, and building blocks for data communication systems, exploit photoexcited charge carriers in graphene. For these systems, it is essential to understand, and eventually control, the cooling dynamics of the photoinduced hot-carrier distribution. There is, however, still an active debate on the different mechanisms that contribute to hot-carrier cooling. In particular, the intrinsic cooling mechanism that ultimately limits the cooling dynamics remains an open question. Here, we address this question by studying two technologically relevant systems, consisting of high-quality graphene with a mobility >10,000 cm$^2$V$^{-1}$s$^{-1}$ and environments that do not efficiently take up electronic heat from graphene: WSe$_2$-encapsulated graphene and suspended graphene. We study the cooling dynamics of these two high-quality graphene systems using ultrafast pump-probe spectroscopy at room temperature. Cooling via disorder-assisted acoustic phonon scattering and out-of-plane heat transfer to the environment is relatively inefficient in these systems, predicting a cooling time of tens of picoseconds. However, we observe much faster cooling, on a timescale of a few picoseconds. We attribute this to an intrinsic cooling mechanism, where carriers in the hot-carrier distribution with enough kinetic energy emit optical phonons. During phonon emission, the electronic system continuously re-thermalizes, re-creating carriers with enough energy to emit optical phonons. We develop an analytical model that explains the observed dynamics, where cooling is eventually limited by optical-to-acoustic phonon coupling. These fundamental insights into the intrinsic cooling mechanism of hot carriers in graphene will play a key role in guiding the development of graphene-based optoelectronic devices.

The capture of photoexcited deep-band hot carriers, excited by photons with energies far above the bandgap, is of significant importance for photovoltaic and photoelectronic applications since it is directly related to the quantum efficiency of photon-to-electron conversion. By employing time-resolved photoluminescence and state-of-the-art time-domain density functional theory, we reveal that photoexcited hot carriers in organic-inorganic hybrid perovskites prefer a zigzag interfacial charge-transfer pathway, i.e., the hot carriers transfer back and forth between CH3NH3PbI3 and graphene, before they reach a charge separated state. Driven by quantum coherence and interlayer vibrational modes, this pathway at the semiconductor-graphene interface takes about 400 femtoseconds, much faster than the relaxation process within CH3NH3PbI3 (in several picoseconds). We further demonstrate that the transfer rate of the pathway can be further enhanced by interfacial defects. Our work provides a new insight for the fundamental understanding and precise manipulation of hot-carrier dynamics at the complex semiconductor-graphene interfaces, paving the way for highly efficient photovoltaic and photoelectric device optimization.

We report on realization and quantum transport study of a twisted bilayer graphene (tBLG) Josephson junction device. High-quality tBLG employed in the device fabrication is obtained via chemical vapour deposition and the device is fabricated by contacting a piece of tBLG by two closely spaced Al electrodes in an Al-tBLG-Al Josephson junction configuration. Low-temperature transport measurements show that below the critical temperature of the Al electrodes ($T_c\approx1.1$ K), the device exhibits sizable supercurrents at zero magnetic field, arising from the superconducting proximity effect with high contact transparency in the device. In the measurements of the critical supercurrent as a function of perpendicularly applied magnetic field, a standard Fraunhofer-like pattern of oscillations is observed, indicating a uniform supercurrent distribution inside the junction. Multiple Andreev reflection characteristics are also observed in the spectroscopy measurements of the device, and their magnetic field and temperature dependencies are found to be well described by the Bardeen$-$Cooper$-$Schrieffer theory., Comment: 14 pages, 4 figures

We report on low-temperature transport study of a single layer graphene (SLG)-twisted bilayer graphene (tBLG) junction device. The SLG-tBLG junction in the device is grown by chemical vapor deposition and the device is fabricated in a Hall-bar configuration on Si/SiO$_2$ substrate. The longitudinal resistances across the SLG-tBLG junction (cross-junction resistances) on the two sides of the Hall bar and the Hall resistances of SLG and tBLG in the device are measured. In the quantum Hall regime, the measurements show that the measured cross-junction resistances exhibit a series of new quantized plateaus and the appearance of these resistance plateaus can be attributed to the presence of the well-defined edge-channel transport along the SLG-tBLG junction interface. The measurements also show that the difference between the cross-junction resistances measured on the two sides of the Hall-bar provides a sensitive measure to the edge channel transport characteristics in the two graphene layers that constitute the SLG-tBLG junction and to degeneracy lifting of the Landau levels in the tBLG layer. Temperature dependent measurements of the cross-junction resistance in the quantum Hall regime are also carried out and the influence of the transverse transport of the bulk Landau levels on the edge channel transport along the SLG-tBLG junction interface are extracted. These results enrich the understanding of the charge transport across interfaces in graphene hybrid structures and open up new opportunities for probing exotic quantum phenomena in graphene devices., Comment: 20 pages, 4 figures

Stacking order has strong influence on the coupling between the two layers of twisted bilayer graphene (BLG), which in turn determines its physical properties. Here, we report the investigation of the interlayer coupling of the epitaxially grown single-crystal 30{\deg} twisted BLG on Cu(111) at the atomic scale. The stacking order and morphology of BLG is controlled by a rationally designed two-step growth process, that is, the thermodynamically controlled nucleation and kinetically controlled growth. The crystal structure of the 30{\deg}-twisted bilayer graphene (30{\deg}-tBLG) is determined to have the quasicrystal like symmetry. The electronic properties and interlayer coupling of the 30{\deg}-tBLG is investigated using scanning tunneling microscopy (STM) and spectroscopy (STS). The energy-dependent local density of states (DOS) with in-situ electrostatic doping shows that the electronic states in two graphene layers are decoupled near the Dirac point. A linear dispersion originated from the constituent graphene monolayers is discovered with doubled degeneracy. This study contributes to controlled growth of twist-angle-defined BLG, and provides insights of the electronic properties and interlayer coupling in this intriguing system., Comment: 26 pages, 4 figures

The phase offset of quantum oscillations is commonly used to experimentally diagnose topologically non-trivial Fermi surfaces. This methodology, however, is inconclusive for spin-orbit-coupled metals where $\pi$-phase-shifts can also arise from non-topological origins. Here, we show that the linear dispersion in topological metals leads to a $T^2$-temperature correction to the oscillation frequency that is absent for parabolic dispersions. We confirm this effect experimentally in the Dirac semi-metal Cd$_3$As$_2$ and the multiband Dirac metal LaRhIn$_5$. Both materials match a tuning-parameter-free theoretical prediction, emphasizing their unified origin. For topologically trivial Bi$_2$O$_2$Se, no frequency shift associated to linear bands is observed as expected. However, the $\pi$-phase shift in Bi$_2$O$_2$Se would lead to a false positive in a Landau-fan plot analysis. Our frequency-focused methodology does not require any input from ab-initio calculations, and hence is promising for identifying correlated topological materials.

Quantum confined devices of three-dimensional topological insulators have been proposed to be promising and of great importance for studies of confined topological states and for applications in low energy-dissipative spintronics and quantum information processing. The absence of energy gap on the TI surface limits the experimental realization of a quantum confined system in three-dimensional topological insulators. This communication reports on the successful realization of single-electron transistor devices in Bi$_2$Te$_3$ nanoplates by state of the art nanofabrication techniques. Each device consists of a confined central island, two narrow constrictions that connect the central island to the source and drain, and surrounding gates. Low-temperature transport measurements demonstrate that the two narrow constrictions function as tunneling junctions and the device shows well-defined Coulomb current oscillations and Coulomb diamond shaped charge stability diagrams. This work provides a controllable and reproducible way to form quantum confined systems in three-dimensional topological insulators, which should greatly stimulate research towards confined topological states, low energy-dissipative devices and quantum information processing., Comment: 13 pages, 3 figures, Supporting Information

We report on phase-coherent transport studies of a Bi$_2$O$_2$Se nanoplate and on observation of universal conductance fluctuations and spin-orbit interaction induced reduction in fluctuation amplitude in the nanoplate. Thin-layered Bi$_2$O$_2$Se nanoplates are grown by chemical vapor deposition (CVD) and transport measurements are made on a Hall-bar device fabricated from a CVD-grown nanoplate. The measurements show weak antilocalization at low magnetic fields at low temperatures, as a result of spin-orbit interaction, and a crossover toward weak localization with increasing temperature. Temperature dependences of characteristic transport lengths, such as spin relaxation length, phase coherence length, and mean free path, are extracted from the low-field measurement data. Universal conductance fluctuations are visible in the low-temperature magnetoconductance over a large range of magnetic fields and the phase coherence length extracted from the autocorrelation function is in consistence with the result obtained from the weak localization analysis. More importantly, we find a strong reduction in amplitude of the universal conductance fluctuations and show that the results agree with the analysis assuming strong spin-orbit interaction in the Bi$_2$O$_2$Se nanoplate., Comment: 11 pages, 4 figures, supplementary materials

Orchestration of diverse synaptic plasticity mechanisms across different timescales produces complex cognitive processes. To achieve comparable cognitive complexity in memristive neuromorphic systems, devices that are capable to emulate short- and long-term plasticity (STP and LTP, respectively) concomitantly are essential. However, this fundamental bionic trait has not been reported in any existing memristors where STP and LTP can only be induced selectively because of the inability to be decoupled using different loci and mechanisms. In this work, we report the first demonstration of truly concomitant STP and LTP in a three-terminal memristor that uses independent physical phenomena to represent each form of plasticity. The emerging layered material Bi2O2Se is used in memristor for the first time, opening up the prospects for ultra-thin, high-speed and low-power neuromorphic devices. The concerted action of STP and LTP in our memristor allows full-range modulation of the transient synaptic efficacy, from depression to facilitation, by stimulus frequency or intensity, providing a versatile device platform for neuromorphic function implementation. A recurrent neural circuitry model is developed to simulate the intricate "sleep-wake cycle autoregulation" process, in which the concomitance of STP and LTP is posited as a key factor in enabling this neural homeostasis. This work sheds new light on the highly sophisticated computational capabilities of memristors and their prospects for realization of advanced neuromorphic functions.

We study a relativistic quantum cavity system realized by etching out from a graphene sheet by quantum transport measurements and theoretical calculations. The conductance of the graphene cavity has been measured as a function of the back gate voltage (or the Fermi energy) and the magnetic field applied perpendicular to the graphene sheet, and characteristic conductance contour patterns are observed in the measurements. In particular, two types of high conductance contour lines, i.e., straight and parabolic-like high conductance contour lines, are found in the measurements. The theoretical calculations are performed within the framework of tight-binding approach and Green's function formalism. Similar characteristic high conductance contour features as in the experiments are found in the calculations. The wave functions calculated at points selected along a straight conductance contour line are found to be dominated by a chain of scars of high probability distributions arranged as a necklace following the shape of cavity and the current density distributions calculated at these point are dominated by an overall vortex in the cavity. These characteristics are found to be insensitive to increasing magnetic field. However, the wave function probability distributions and the current density distributions calculated at points selected along a parabolic-like contour line show a clear dependence on increasing magnetic field, and the current density distributions at these points are characterized by the complex formation of several localized vortices in the cavity. Our work brings a new insight into quantum chaos in relativistic particle systems and would greatly stimulate experimental and theoretical efforts towards this still emerging field., Comment: 20 pages, 6 figures

A new type of two-dimensional layered semiconductor with weak electrostatic but not van der Waals interlayer interactions, Bi2O2Se, has been recently synthesized, which shown excellent air stability and ultrahigh carrier mobility. Herein, we combined theoretical and experimental approaches to study the Raman spectra of Bi2O2Se and related bismuth oxychalcogenides (Bi2O2Te and Bi2O2S). The experimental peaks were fully consistent with the calculated results, and were successfully assigned. Bi2O2S was predicted to have more Raman-active modes due to its lower symmetry. The shift of the predicted frequencies of Raman active modes was also found to get softened as the interlayer interaction decreases from bulk to monolayer Bi2O2Se and Bi2O2Te. To reveal the strain effects on the Raman shifts, a universal theoretical equation was established based on the symmetry of Bi2O2Se and Bi2O2Te. It was predicted that the doubly degenerate modes split under in-plane uniaxial/shear strains. Under a rotated uniaxial strain, the changes of Raman shifts are anisotropic for degenerate modes although Bi2O2Se and Bi2O2Te were usually regarded as isotropic systems similar to graphene. This implies a novel method to identify the crystallographic orientation from Raman spectra under strain. These results have important consequences for the incorporation of 2D Bismuth oxychalcogenides into nanoelectronic devices., Comment: 40 Pages, 18 figures

Recently an air-stable layered semiconductor Bi2O2Se was discovered to exhibit an ultrahigh mobility in transistors fabricated with its thin layers. In this work, we explored the mechanism that induces the high mobility and distinguishes Bi2O2Se from other semiconductors. We found that the electron donor states lie above the lowest conduction band. Thus, electrons get spontaneously ionized from donor sites (e.g., Se vacancies) without involving the thermal activation, different from the donor ionization in conventional semiconductors. Consequently, the resistance decreases as reducing the temperature as observed in our measurement, which is similar to a metal but contrasts to a usual semiconductor. Furthermore, the electron conduction channels locate spatially away from ionized donor defects (Se vacancies) in different van der Waals layers. Such a spatial separation can strongly suppress the scattering caused by donor sites and subsequently increase the electron mobility, especially at the low temperature. We call this high-mobility mechanism self-modulation doping, i.e. the modulation doping spontaneously happening in a single-phase material without requiring a heterojunction. Our work paves a way to design novel high-mobility semiconductors with layered materials.

Confinement and edge structures are known to play significant roles in electronic and transport properties of two-dimensional materials. Here, we report on low-temperature magnetotransport measurements of lithographically patterned graphene cavity nanodevices. It is found that the evolution of the low-field magnetoconductance characteristics with varying carrier density exhibits different behaviors in graphene cavity and bulk graphene devices. In the graphene cavity devices, we have observed that intravalley scattering becomes dominant as the Fermi level gets close to the Dirac point. We associate this enhanced intravalley scattering to the effect of charge inhomogeneities and edge disorder in the confined graphene nanostructures. We have also observed that the dephasing rate of carriers in the cavity devices follows a parabolic temperature dependence, indicating that the direct Coulomb interaction scattering mechanism governs the dephasing at low temperatures. Our results demonstrate the importance of confinement in carrier transport in graphene nanostructure devices., Comment: 13 pages, 5 figures

Graphene/hexagonal boron nitride (G/$h$-BN) heterostructures offer an excellent platform for developing nanoelectronic devices and for exploring correlated states in graphene under modulation by a periodic superlattice potential. Here, we report on transport measurements of nearly $0^{\circ}$-twisted G/$h$-BN heterostructures. The heterostructures investigated are prepared by dry transfer and thermally annealing processes and are in the low mobility regime (approximately $3000~\mathrm{cm}^{2}\mathrm{V}^{-1}\mathrm{s}^{-1}$ at 1.9 K). The replica Dirac spectra and Hofstadter butterfly spectra are observed on the hole transport side, but not on the electron transport side, of the heterostructures. We associate the observed electron-hole asymmetry to the presences of a large difference between the opened gaps in the conduction and valence bands and a strong enhancement in the interband contribution to the conductivity on the electron transport side in the low-mobility G/$h$-BN heterostructures. We also show that the gaps opened at the central Dirac point and the hole-branch secondary Dirac point are large, suggesting the presence of strong graphene-substrate interaction and electron-electron interaction in our G/$h$-BN heterostructures. Our results provide additional helpful insight into the transport mechanism in G/$h$-BN heterostructures., Comment: 7 pages, 4 figures

Semiconductor Bi$_2$O$_2$Se nanolayers of high crystal quality have been realized via epitaxial growth. These two-dimensional (2D) materials possess excellent electron transport properties with potential application in nanoelectronics. It is also strongly expected that the 2D Bi$_2$O$_2$Se nanolayers could be of an excellent material platform for developing spintronic and topological quantum devices, if the presence of strong spin-orbit interaction in the 2D materials can be experimentally demonstrated. Here, we report on experimental determination of the strength of spin-orbit interaction in Bi$_2$O$_2$Se nanoplates through magnetotransport measurements. The nanoplates are epitaxially grown by chemical vapor deposition and the magnetotransport measurements are performed at low temperatures. The measured magnetoconductance exhibits a crossover behavior from weak antilocalization to weak localization at low magnetic fields with increasing temperature or decreasing back gate voltage. We have analyzed this transition behavior of the magnetoconductance based on an interference theory which describes the quantum correction to the magnetoconductance of a 2D system in the presence of spin-orbit interaction. Dephasing length and spin relaxation length are extracted from the magnetoconductance measurements. Comparing to other semiconductor nanostructures, the extracted relatively short spin relaxation length of ~150 nm indicates the existence of strong spin-orbit interaction in Bi$_2$O$_2$Se nanolayers., Comment: 14 pages, 4 figures, and 5 pages of Supplementary Materials

Infrared detection and sensing is deeply embedded in modern technology and human society and its development has always been benefitting from the discovery of new photoelectric response materials. The rise of two-dimensional (2D) materials, thanks to their distinct electronic structure, extreme dimensional confinement and strong light-matter interactions, provides new material platform for next-generation infrared photodetection. Ideal infrared detectors should have fast respond, high sensitivity and air-stability, which is rare to meet at the same time for all existing 2D materials, either graphene, transition metal dichalcogenide or black phosphorous. Herein we demonstrate a new infrared photodetector based on 2D Bi2O2Se crystals, whose main characteristics are superb in the whole 2D family: high sensitivity of ~65 A/W at 1200 nm and ultrafast intrinsic photoresponse of ~1 ps at room temperature. Such great performance is attributed to the suitable electronic bandgap and high carrier mobility of 2D oxyselenide. With additional merits of mass production, excellent stability and flexibility, 2D oxyselenide detectors should open new avenues in highly-sensitive, high-speed, low-cost, flexible infrared photodetection and imaging.

Piezoelectric and ferroelectric properties in the two dimensional (2D) limit are highly desired for nanoelectronic, electromechanical, and optoelectronic applications. Here we report the first experimental evidence of out-of-plane piezoelectricity and ferroelectricity in van der Waals layered ${\alpha}$-In2Se3 nano-flakes. The non-centrosymmetric R3m symmetry of the ${\alpha}$-In2Se3 samples is confirmed by scanning transmission electron microscopy, second-harmonic generation, and Raman spectroscopy measurements. Domains with opposite polarizations are visualized by piezo-response force microscopy. Single-point poling experiments suggest that the polarization is potentially switchable for ${\alpha}$-In2Se3 nano-flakes with thicknesses down to ~ 10 nm. The piezotronic effect is demonstrated in two-terminal devices, where the Schottky barrier can be modulated by the strain-induced piezopotential. Our work on polar ${\alpha}$-In2Se3, one of the model 2D piezoelectrics and ferroelectrics with simple crystal structures, shows its great potential in electronic and photonic applications., Comment: 17 pages, 5 figures, just accepted by Nano Letters

A foundation of the modern technology that uses single-crystal silicon has been the growth of high-quality single-crystal Si ingots with diameters up to 12 inches or larger. For many applications of graphene, large-area high-quality (ideally of single-crystal) material will be enabling. Since the first growth on copper foil a decade ago, inch-sized single-crystal graphene has been achieved. We present here the growth, in 20 minutes, of a graphene film of 5 x 50 cm2 dimension with > 99% ultra-highly oriented grains. This growth was achieved by: (i) synthesis of sub-metre-sized single-crystal Cu(111) foil as substrate; (ii) epitaxial growth of graphene islands on the Cu(111) surface; (iii) seamless merging of such graphene islands into a graphene film with high single crystallinity and (iv) the ultrafast growth of graphene film. These achievements were realized by a temperature-driven annealing technique to produce single-crystal Cu(111) from industrial polycrystalline Cu foil and the marvellous effects of a continuous oxygen supply from an adjacent oxide. The as-synthesized graphene film, with very few misoriented grains (if any), has a mobility up to ~ 23,000 cm2V-1s-1 at 4 K and room temperature sheet resistance of ~ 230 ohm/square. It is very likely that this approach can be scaled up to achieve exceptionally large and high-quality graphene films with single crystallinity, and thus realize various industrial-level applications at a low cost.

Graphitic nitrogen-doped graphene is an excellent platform to study scattering processes of massless Dirac fermions by charged impurities, in which high mobility can be preserved due to the absence of lattice defects through direct substitution of carbon atoms in the graphene lattice by nitrogen atoms. In this work, we report on electrical and magnetotransport measurements of high-quality graphitic nitrogen-doped graphene. We show that the substitutional nitrogen dopants in graphene introduce atomically sharp scatters for electrons but long-range Coulomb scatters for holes and, thus, graphitic nitrogen-doped graphene exhibits clear electron-hole asymmetry in transport properties. Dominant scattering processes of charge carriers in graphitic nitrogen-doped graphene are analyzed. It is shown that the electron-hole asymmetry originates from a distinct difference in intervalley scattering of electrons and holes. We have also carried out the magnetotransport measurements of graphitic nitrogen-doped graphene at different temperatures and the temperature dependences of intervalley scattering, intravalley scattering and phase coherent scattering rates are extracted and discussed. Our results provide an evidence for the electron-hole asymmetry in the intervalley scattering induced by substitutional nitrogen dopants in graphene and shine a light on versatile and potential applications of graphitic nitrogen-doped graphene in electronic and valleytronic devices., Comment: 35 pages, 5 figures