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An ideal proton exchange membrane should only permeate protons and be leak tight for fuels. Graphene is impermeable to water and poorly conducting to protons. Here, we chemically functionalized monolayer graphene to install sulfophenylated sp3 dislocations by diazotization. Selective to protons, transmembrane areal conductances are up to ~50 S/cm2, which is ~5000 fold higher than in pristine graphene. Mounted in a direct methanol fuel cell, sulfophenylated graphene resulted in power densities up to 1.6 W/mg or 123 mW/cm under standard cell operation (60 C), a value ~two-fold larger than micron-thick films of Nafion 117. The combination of sp3 dislocations and polar groups, therefore, allow the creation of hydrophilic ion paths through graphene and unveils a novel route to rationalize transmembrane hydron transport through 2D 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.

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

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

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

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.

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

We have theoretically investigated the intrinsic carrier mobility in semimetals with distorted Dirac cones under both longitudinal and transverse acoustic phonon scattering. An analytic formula for the carrier mobility was obtained. It shows that tilting significantly reduces the mobility. The theory was then applied to 8B-Pmmn borophene and borophane (fully hydrogenated borophene), both of which have tilted Dirac cones. The predicted carrier mobilities in 8B-Pmmn borophene at room temperature are both higher than that in graphene. For borophane, despite its superhigh Fermi velocity, the carrier mobility is lower than that in 8B-Pmmn owing to its smaller elastic constant under shear strain., Comment: 24 pages, 5 figures, 1 table

Nano-thick metallic transition metal dichalcogenides such as VS$_{2}$ are essential building blocks for constructing next-generation electronic and energy-storage applications, as well as for exploring unique physical issues associated with the dimensionality effect. However, such 2D layered materials have yet to be achieved through either mechanical exfoliation or bottom-up synthesis. Herein, we report a facile chemical vapor deposition route for direct production of crystalline VS$_{2}$ nanosheets with sub-10 nm thicknesses and domain sizes of tens of micrometers. The obtained nanosheets feature spontaneous superlattice periodicities and excellent electrical conductivities (~3$\times$10$^{3}$ S cm$^{-1}$), which has enabled a variety of applications such as contact electrodes for monolayer MoS$_{2}$ with contact resistances of ~1/4 to that of Ni/Au metals, and as supercapacitor electrodes in aqueous electrolytes showing specific capacitances as high as 8.6$\times$10$^{2}$ F g$^{-1}$. This work provides fresh insights into the delicate structure-property relationship and the broad application prospects of such metallic 2D materials., Comment: 23 pages, 5 figues

The rise of graphene marks the advent of two-dimensional atomic crystals, which have exhibited a cornucopia of intriguing properties, such as the integer and fractional quantum Hall effects, valley Hall effect, charge density waves and superconductivity, to name a few. Yet, magnetism, a property of extreme importance in both science and technology, remains elusive. There is a paramount need for magnetic two-dimensional crystals. With the availability of many magnetic materials consisting of van der Waals coupled two-dimensional layers, it thus boils down to the question of how the magnetic order will evolve with reducing thickness. Here we investigate the effect of thickness on the magnetic ordering in nanothick V$_5$S$_8$. We uncover an anomalous Hall effect, by which the magnetic ordering in V$_5$S$_8$ down to 3.2 nm is probed. With decreasing thickness, a breakdown of antiferromagnetism is evident, followed by a spin-glass-like state. For thinnest samples, a weak ferromagnetic ordering emerges. The results not only show an interesting effect of reducing thickness on the magnetic ordering in a potential candidate for magnetic two-dimensional crystals, but demonstrate the anomalous Hall effect as a useful characterization tool for magnetic orderings in two-dimensional systems., Comment: 17 pages, 5 figures and supplementary material

Electron transport properties of a topological insulator Bi$_2$Se$_3$ thin film are studied in Hall-bar geometry. The film with a thickness of 10 nm is grown by van der Waals epitaxy on fluorophlogopite mica and Hall-bar devices are fabricated from the as-grown film directly on the mica substrate. Weak antilocalization and electron-electron interaction effects are observed and analyzed at low temperatures. The phase-coherence length extracted from the measured weak antilocalization characteristics shows a strong power-law increase with decreasing temperature and the transport in the film is shown to occur via coupled multiple (topological surface and bulk states) channels. The conductivity of the film shows a logarithmically decrease with decreasing temperature and thus the electron-electron interaction plays a dominant role in quantum corrections to the conductivity of the film at low temperatures., Comment: 12 pages, 5 figures