Search

Unconventional superconductivity, where electron pairing does not involve electron-phonon interactions, is often attributed to magnetic correlations in a material. Well known examples include high-T_c cuprates and uranium-based heavy fermion superconductors. Less explored are unconventional superconductors with strong spin-orbit coupling, where interactions between spin-polarised electrons and external magnetic field can result in multiple superconducting phases and field-induced transitions between them, a rare phenomenon in the superconducting state. Here we report a magnetic-field driven phase transition in \beta-PdBi2, a layered non-magnetic superconductor. Our tunnelling spectroscopy on thin PdBi2 monocrystals incorporated in planar superconductor-insulator-normal metal junctions reveals a marked discontinuity in the superconducting properties with increasing in-plane field, which is consistent with a transition from conventional (s-wave) to nodal pairing. Our theoretical analysis suggests that this phase transition may arise from spin polarisation and spin-momentum locking caused by locally broken inversion symmetry, with p-wave pairing becoming energetically favourable in high fields. Our findings also reconcile earlier predictions of unconventional multigap superconductivity in \beta-PdBi2 with previous experiments where only a single s-wave gap could be detected., Comment: 29 pages, including 4 main Figures, Methods, 8 Supplementary Figures and 5 Supplementary Notes

The ongoing efforts to optimize Li-ion batteries led to the interest in intercalation of nanoscale layered compounds, including bilayer graphene. Its lithium intercalation has been demonstrated recently but the mechanisms underpinning the storage capacity remain poorly understood. Here, using magnetotransport measurements, we report in-operando intercalation dynamics of bilayer graphene. Unexpectedly, we find four distinct intercalation stages that correspond to well-defined Li-ion densities. We refer to these stages as 'in-plane', with no in-plane analogues in bulk graphite. The fully intercalated bilayers represent a stoichiometric compound C14LiC14 with a Li density of 2.7x10^{14} cm^{-2}, notably lower than fully intercalated graphite. Combining the experimental findings and DFT calculations, we show that the critical step in bilayer intercalation is a transition from AB to AA stacking which occurs at a density of 0.9x10^{14} cm^{-2}. Our findings reveal the mechanism and limits for electrochemical intercalation of bilayer graphene and suggest possible avenues for increasing the Li storage capacity., Comment: 30 pages, 17 figures

Biological nanostructures change their shape and function in response to external stimuli, and significant efforts have been made to design artificial biomimicking devices operating on similar principles. In this work we demonstrate a programmable nanofluidic switch, driven by elastocapillarity, and based on nanochannels built from layered two-dimensional nanomaterials possessing atomically smooth surfaces and exceptional mechanical properties. We explore operational modes of the nanoswitch and develop a theoretical framework to explain the phenomenon. By predicting the switching-reversibility phase diagram - based on material, interfacial and wetting properties, as well as the geometry of the nanofluidic circuit - we rationally design switchable nano-capsules capable of enclosing zeptoliter volumes of liquid, as small as the volumes enclosed in viruses. The nanoswitch will find useful application as an active element in integrated nanofluidic circuitry and could be used to explore nanoconfined chemistry and biochemistry, or be incorporated into shape-programmable materials.

Periodic systems feature the Hofstadter butterfly spectrum produced by Brown--Zak minibands of electrons formed when magnetic field flux through the lattice unit cell is commensurate with flux quantum and manifested by magneto-transport oscillations. Quantum oscillations, such as Shubnikov -- de Haas effect and Aharonov--Bohm effect, are also characteristic for electronic systems with closed orbits in real space and reciprocal space. Here we show the intricate relation between these two phenomena by tracing quantum magneto-oscillations to Lifshitz transitions in graphene superlattices, where they persist even at relatively low fields and very much above liquid-helium temperatures. The oscillations originate from Aharonov--Bohm interference on cyclotron trajectories that form a kagom\'e-shaped network characteristic for Lifshitz transitions. In contrast to Shubnikov - de Haas oscillations, the kagom\'e oscillations are robust against thermal smearing and they can be detected even when the Hofstadter butterfly spectrum is undermined by electron's scattering. We expect that kagom\'e quantum oscillations are generic to rotationally-symmetric two-dimensional crystals close to Lifshitz transitions., Comment: 7+7 pages

Recent experiments have shown that the out-of-plane dielectric constant of water confined in nanoslits of graphite and hexagonal boron nitride (hBN) is vanishingly small. Despite extensive effort based mainly on classical force-field molecular dynamics (FFMD) approaches, the origin of this phenomenon is under debate. Here we used ab initio molecular dynamics simulations (AIMD) and AIMD-trained machine learning potentials to explore the structure and electronic properties of water confined inside graphene and hBN slits. We found that the reduced dielectric constant arises mainly from the anti-parallel alignment of the water dipoles in the perpendicular direction to the surface in the first two water layers near the solid interface. Although the water molecules retain liquid-like mobility, the interfacial layers exhibit a net ferroelectric ordering and constrained hydrogen-bonding orientations which lead to much reduced polarization fluctuations in the out-of-plane direction at room temperature. Importantly, we show that this effect is independent of the distance between the two confining surfaces of the slit, and it originates in the spontaneous polarization of interfacial water. Our calculations also show no significant variations in the structure and polarization of water near graphene and hBN, despite their different electronic structures. These results are important as they offer new insight into a property of water that plays a critical role in the long-range interactions between surfaces, the electric double-layer formation, ion solvation and transport, as well as biomolecular functioning.

Nanoporous membranes based on two dimensional materials are predicted to provide highly selective gas transport in combination with extreme permeability. Here we investigate membranes made from multilayer graphdiyne, a graphene-like crystal with a larger unit cell. Despite being nearly a hundred of nanometers thick, the membranes allow fast, Knudsen-type permeation of light gases such as helium and hydrogen whereas heavy noble gases like xenon exhibit strongly suppressed flows. Using isotope and cryogenic temperature measurements, the seemingly conflicting characteristics are explained by a high density of straight-through holes (direct porosity of ~0.1%), in which heavy atoms are adsorbed on the walls, partially blocking Knudsen flows. Our work offers important insights into intricate transport mechanisms playing a role at nanoscale.

Optical device is a key component in our lives and organic liquid crystals are nowadays widely used to reduce human imprint. However, this technology still suffers from relatively high costs, toxicity and other environmental impacts, and cannot fully meet the demand of future sustainable society. Here we describe an alternative approach to colour-tuneable optical devices, which is based on sustainable inorganic liquid crystals derived from two-dimensional mineral materials abundant in nature. The prototypical two-dimensional mineral of vermiculite is massively produced by a green method, possessing size-to-thickness ratios of >103, in-plane magnetisation of >10 emu g-1, and an optical bandgap of >3 eV. These characteristics endow two-dimensional vermiculite with sensitive magneto-birefringence response, which is several orders of magnitude larger than organic counterparts, as well as capability of broad-spectrum modulation. Our finding consequently permits the fabrication of various chromic devices with low or even zero-energy consumption, which can be used for sustainable optics., Comment: 16 pages, 4 figures

Electrical resistance usually originates from lattice imperfections. However, even a perfect lattice has a fundamental resistance limit, given by the Landauer conductance caused by a finite number of propagating electron modes. This resistance, shown by Sharvin to appear at the contacts of electronic devices, sets the ultimate conductance limit of non-interacting electrons. Recent years have seen growing evidence of hydrodynamic electronic phenomena, prompting recent theories to ask whether an electronic fluid can radically break the fundamental Landauer-Sharvin limit. Here, we use single-electron transistor imaging of electronic flow in high-mobility graphene Corbino disk devices to answer this question. First, by imaging ballistic flows at liquid-helium temperatures, we observe a Landauer-Sharvin resistance that does not appear at the contacts but is instead distributed throughout the bulk. This underpins the phase-space origin of this resistance - as emerging from spatial gradients in the number of conduction modes. At elevated temperatures, by identifying and accounting for electron-phonon scattering, we reveal the details of the purely hydrodynamic flow. Strikingly, we find that electron hydrodynamics eliminates the bulk Landuer-Sharvin resistance. Finally, by imaging spiraling magneto-hydrodynamic Corbino flows, we reveal the key emergent length scale predicted by hydrodynamic theories - the Gurzhi length. These observations demonstrate that electronic fluids can dramatically transcend the fundamental limitations of ballistic electrons, with important implications for fundamental science and future technologies

Superconductors with nontrivial band structure topology represent a class of materials with unconventional and potentially useful properties. Recent years have seen much success in creating artificial hybrid structures exhibiting main characteristics of two-dimensional (2D) topological superconductors. Yet, bulk materials known to combine inherent superconductivity with nontrivial topology remain scarce, largely because distinguishing their central characteristic -- topological surface states -- proved challenging due to a dominant contribution from the superconducting bulk. Reported here is a highly anomalous behaviour of surface superconductivity in topologically nontrivial 3D superconductor In2Bi where the surface states result from its nontrivial band structure, which itself is a consequence of the non-symmorphic crystal symmetry and strong spin-orbit coupling. In contrast to smoothly decreasing diamagnetic susceptibility above the bulk critical field Hc2, associated with surface superconductivity in conventional superconductors, we observe near-perfect, Meissner-like screening of low-frequency magnetic fields well above Hc2. The enhanced diamagnetism disappears at a new phase transition close to the critical field of surface superconductivity Hc3. Using theoretical modelling, we show that the anomalous screening is consistent with modification of surface superconductivity due to the presence of topological surface states. The demonstrated possibility to detect signatures of the surface states using macroscopic magnetization measurements provides an important new tool for discovery and identification of topological superconductors., Comment: 30 pages, 4 main figures, 11 supporting figures

Van der Waals heterostructures display a rich variety of unique electronic properties. To identify novel transport mechanisms, nonlocal measurements have been widely used, wherein a voltage is measured at contacts placed far away from the expected classical flow of charge carriers. This approach was employed in search of dissipationless spin and valley transport, topological charge-neutral currents, hydrodynamic flows and helical edge modes. Monolayer, bilayer, and few-layer graphene, transition-metal dichalcogenides, and moire superlattices were found to display pronounced nonlocal effects. However, the origin of these effects is hotly debated. Graphene, in particular, exhibits giant nonlocality at charge neutrality, a prominent behavior that attracted competing explanations. Utilizing superconducting quantum interference device on a tip (SQUID-on-tip) for nanoscale thermal and scanning gate imaging, we demonstrate that the commonly-occurring charge accumulation at graphene edges leads to giant nonlocality, producing narrow conductive channels that support long-range currents. Unexpectedly, while the edge conductance has little impact on the current flow in zero magnetic field, it leads to field-induced decoupling between edge and bulk transport at moderate fields. The resulting giant nonlocality both at charge neutrality and away from it produces exotic flow patterns in which charges can flow against the global electric field. We have visualized surprisingly intricate patterns of nonlocal currents, which are sensitive to edge disorder. The observed one-dimensional edge transport, being generic and nontopological, is expected to support nonlocal transport in many electronic systems, offering insight into numerous controversies in the literature and linking them to long-range guided electronic states at system edges., Comment: Main text: 14 pages, 4 figures. Methods and Supplementary information: 27 pages, 6 figures. Supplementary videos: 9

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.

Two-dimensional atomic crystals can radically change their properties in response to external influences such as substrate orientation or strain, resulting in essentially new materials in terms of the electronic structure. A striking example is the creation of flat-bands in bilayer-graphene for certain 'magic' twist-angles between the orientations of the two layers. The quenched kinetic-energy in these flat-bands promotes electron-electron interactions and facilitates the emergence of strongly-correlated phases such as superconductivity and correlated-insulators. However, the exquisite fine-tuning required for finding the magic-angle where flat-bands appear in twisted-bilayer graphene, poses challenges to fabrication and scalability. Here we present an alternative route to creating flat-bands that does not involve fine tuning. Using scanning tunneling microscopy and spectroscopy, together with numerical simulations, we demonstrate that graphene monolayers placed on an atomically-flat substrate can be forced to undergo a buckling-transition, resulting in a periodically modulated pseudo-magnetic field, which in turn creates a post-graphene material with flat electronic bands. Bringing the Fermi-level into these flat-bands by electrostatic doping, we observe a pseudogap-like depletion in the density-of-states, which signals the emergence of a correlated-state. The described approach of 2D crystal buckling offers a strategy for creating other superlattice systems and, in particular, for exploring interaction phenomena characteristic of flat-bands., Comment: 22 pages, 15 figures. arXiv admin note: substantial text overlap with arXiv:1904.10147

Defect-free graphene is impermeable to gases and liquids but highly permeable to thermal protons. Atomic-scale defects such as vacancies, grain boundaries and Stone-Wales defects are predicted to enhance graphene's proton permeability and may even allow small ions through, whereas larger species such as gas molecules should remain blocked. These expectations have so far remained untested in experiment. Here we show that atomically thin carbon films with a high density of atomic-scale defects continue blocking all molecular transport, but their proton permeability becomes ~1,000 times higher than that of defect-free graphene. Lithium ions can also permeate through such disordered graphene. The enhanced proton and ion permeability is attributed to a high density of 8-carbon-atom rings. The latter pose approximately twice lower energy barriers for incoming protons compared to the 6-atom rings of graphene and a relatively low barrier of ~0.6 eV for Li ions. Our findings suggest that disordered graphene could be of interest as membranes and protective barriers in various Li-ion and hydrogen technologies.

We describe how the out-of-plane dielectric polarizability of monolayer graphene influences the electrostatics of bilayer graphene -- both Bernal (BLG) and twisted (tBLG). We compare the polarizability value computed using density functional theory with the output from previously published experimental data on the electrostatically controlled interlayer asymmetry potential in BLG and data on the on-layer density distribution in tBLG. We show that monolayers in tBLG are described well by polarizability $\alpha_{exp} = 10.8 \unicode{x212B}^3$ and effective out-of-plane dielectric susceptibility $\epsilon_z = 2.5$, including their on-layer electron density distribution at zero magnetic field and the inter-layer Landau level pinning at quantizing magnetic fields., Comment: 4 pages

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.

The field of nanofluidics has shown considerable progress over the past decade thanks to key instrumental advances, leading to the discovery of a number of exotic transport phenomena for fluids and ions under extreme confinement. Recently, van der Waals assembly of 2D materials allowed fabrication of artificial channels with angstr\"om-scale precision. This ultimate confinement to the true molecular scale revealed unforeseen behaviour for both mass and ionic transport. In this work, we explore pressure-driven streaming in such molecular-size slits and report a new electro-hydrodynamic effect under coupled pressure and electric force. It takes the form of a transistor-like response of the pressure induced ionic streaming: an applied bias of a fraction of a volt results in an enhancement of the streaming mobility by up to 20 times. The gating effect is observed with both graphite and boron nitride channels but exhibits marked material-dependent features. Our observations are rationalized by a theoretical framework for the flow dynamics, including the frictional interaction of water, ions and the confining surfaces as a key ingredient. The material dependence of the voltage modulation can be traced back to a contrasting molecular friction on graphene and boron nitride. The highly nonlinear transport under molecular-scale confinement offers new routes to actively control molecular and ion transport and design elementary building blocks for artificial ionic machinery, such as ion pumps. Furthermore, it provides a versatile platform to explore electro-mechanical couplings potentially at play in recently discovered mechanosensitive ionic channels.

Recent advances in materials science have made it possible to achieve conditions under which electrons in metals start behaving as highly viscous fluids, "thicker than honey", and exhibit fascinating hydrodynamic effects. In this short review we provide a popular introduction to the emerging field of electron hydrodynamics., Comment: 13 pages, 5 figures, submitted to Physics Today on July 28, 2019

Most of the studied two-dimensional (2D) materials have been obtained by exfoliation of van der Waals crystals. Recently, there has been growing interest in fabricating synthetic 2D crystals which have no layered bulk analogues. These efforts have been focused mainly on the surface growth of molecules in high vacuum. Here, we report an approach to making 2D crystals of covalent solids by chemical conversion of van der Waals layers. As an example, we use 2D indium selenide (InSe) obtained by exfoliation and converted it by direct fluorination into indium fluoride (InF3), which has a non-layered, rhombohedral structure and therefore cannot be possibly obtained by exfoliation. The conversion of InSe into InF3 is found to be feasible for thicknesses down to three layers of InSe, and the obtained stable InF3 layers are doped with selenium. We study this new 2D material by optical, electron transport and Raman measurements and show that it is a semiconductor with a direct bandgap of 2.2 eV, exhibiting high optical transparency across the visible and infrared spectral ranges. We also demonstrate the scalability of our approach by chemical conversion of large-area, thin InSe laminates obtained by liquid exfoliation into InF3 films. The concept of chemical conversion of cleavable thin van der Waals crystals into covalently-bonded non-cleavable ones opens exciting prospects for synthesizing a wide variety of novel atomically thin covalent crystals.

Topology is a powerful recent concept asserting that quantum states could be globally protected against local perturbations. Dissipationless topologically protected states are thus of major fundamental interest as well as of practical importance in metrology and quantum information technology. Although topological protection can be robust theoretically, in realistic devices it is often fragile against various dissipative mechanisms, which are difficult to probe directly because of their microscopic origins. By utilizing scanning nanothermometry, we visualize and investigate microscopic mechanisms undermining the apparent topological protection in the quantum Hall state in graphene. Our simultaneous nanoscale thermal and scanning gate microscopy shows that the dissipation is governed by crosstalk between counterpropagating pairs of downstream and upstream channels that appear at graphene boundaries because of edge reconstruction. Instead of local Joule heating, however, the dissipation mechanism comprises two distinct and spatially separated processes. The work generating process that we image directly and which involves elastic tunneling of charge carriers between the quantum channels, determines the transport properties but does not generate local heat. The independently visualized heat and entropy generation process, in contrast, occurs nonlocally upon inelastic resonant scattering off single atomic defects at graphene edges, while not affecting the transport. Our findings offer a crucial insight into the mechanisms concealing the true topological protection and suggest venues for engineering more robust quantum states for device applications., Comment: Main text: 12 pages, 3 figures. Supplementary information: 19 pages, 9 figures

Hydrodynamics is a general description for the flow of a fluid, and is expected to hold even for fundamental particles such as electrons when inter-particle interactions dominate. While various aspects of electron hydrodynamics were revealed in recent experiments, the fundamental spatial structure of hydrodynamic electrons, the Poiseuille flow profile, has remained elusive. In this work, we provide the first real-space imaging of Poiseuille flow of an electronic fluid, as well as visualization of its evolution from ballistic flow. Utilizing a scanning nanotube single electron transistor, we image the Hall voltage of electronic flow through channels of high-mobility graphene. We find that the profile of the Hall field across the channel is a key physical quantity for distinguishing ballistic from hydrodynamic flow. We image the transition from flat, ballistic field profiles at low temperature into parabolic field profiles at elevated temperatures, which is the hallmark of Poiseuille flow. The curvature of the imaged profiles is qualitatively reproduced by Boltzmann calculations, which allow us to create a 'phase diagram' that characterizes the electron flow regimes. Our results provide long-sought, direct confirmation of Poiseuille flow in the solid state, and enable a new approach for exploring the rich physics of interacting electrons in real space.

When two-dimensional electron gases (2DEGs) are exposed to magnetic field, they resonantly absorb electromagnetic radiation via electronic transitions between Landau levels (LLs). In 2DEGs with a Dirac spectrum, such as graphene, theory predicts an exceptionally high infrared magneto-absorption, even at zero doping. However, the measured LL magneto-optical effects in graphene have been much weaker than expected because of imperfections in the samples available so far for such experiments. Here we measure magneto-transmission and Faraday rotation in high-mobility encapsulated monolayer graphene using a custom designed setup for magneto-infrared microspectroscopy. Our results show a strongly enhanced magneto-optical activity in the infrared and terahertz ranges characterized by a maximum allowed (50%) absorption of light, a 100% magnetic circular dichroism as well as a record high Faraday rotation. Considering that sizeable effects have been already observed at routinely achievable magnetic fields, our findings demonstrate a new potential of magnetic tuning in 2D Dirac materials for long-wavelength optoelectronics and plasmonics., Comment: 14 pages, 4 figures

Interactions between stacked two-dimensional (2D) atomic crystals can radically change their properties, leading to essentially new materials in terms of the electronic structure. Here we show that monolayers placed on an atomically flat substrate can be forced to undergo a buckling transition, which results in periodically strained superlattices. By using scanning tunneling microscopy and spectroscopy and support from numerical simulations, we show that such lateral superlattices in graphene lead to a periodically modulated pseudo-magnetic field, which in turn creates a post-graphene material with flat electronic bands. The described approach of controllable buckling of 2D crystals offers a venue for creating other superlattice systems and, in particular, for exploring interaction phenomena characteristic of flat bands., Comment: 23 pages, 15 figures

Despite a rich choice of two-dimensional materials, which exists these days, heterostructures, both vertical (van der Waals) and in-plane, offer an unprecedented control over the properties and functionalities of the resulted structures. Thus, planar heterostructures allow p-n junctions between different two-dimensional semiconductors and graphene nanoribbons with well-defined edges; and vertical heterostructures resulted in the observation of superconductivity in purely carbon-based systems and realisation of vertical tunnelling transistors. Here we demonstrate simultaneous use of in-plane and van der Waals heterostructures to build vertical single electron tunnelling transistors. We grow graphene quantum dots inside the matrix of hexagonal boron nitride, which allows a dramatic reduction of the number of localised states along the perimeter of the quantum dots. The use of hexagonal boron nitride tunnel barriers as contacts to the graphene quantum dots make our transistors reproducible and not dependent on the localised states, opening even larger flexibility when designing future devices.

Electron transport in nanoscale devices can often result in nontrivial spatial patterns of voltage and current that reflect a variety of physical phenomena, particularly in nonlocal transport regimes. While numerous techniques have been devised to image electron flows, the need remains for a nanoscale probe capable of simultaneously imaging current and voltage distributions with high sensitivity and minimal invasiveness, in magnetic field, across a broad range of temperatures, and beneath an insulating surface. Here we present such a technique for spatially mapping electron flows based on a nanotube single-electron transistor, which achieves high sensitivity for both voltage and current imaging. In a series of experiments using high-mobility graphene devices, we demonstrate the ability of our technique to visualize local aspects of intrinsically nonlocal transport, as in ballistic flows, which are not easily resolvable via existing methods. This technique should both aid in understanding the physics of two-dimensional electronic devices, as well as enable new classes of experiments that image electron flow through buried nanostructures in the quantum and interaction-dominated regimes.

Despite topological protection and the absence of magnetic impurities, two-dimensional topological insulators display quantized conductance only in surprisingly short channels, which can be as short as 100 nm for atomically thin materials. We show that the combined action of short-range nonmagnetic impurities located near the edges and on site electron-electron interactions effectively creates noncollinear magnetic scatterers, and, hence, results in strong backscattering. The mechanism causes deviations from quantization even at zero temperature and for a modest strength of electron-electron interactions. Our theory provides a straightforward conceptual framework to explain experimental results, especially those in atomically thin crystals, plagued with short-range edge disorder., Comment: 8 pages, 9 figures, 5 appendices

Viscous electron fluids have emerged recently as a new paradigm of strongly-correlated electron transport in solids. Here we report on a direct observation of the transition to this long-sought-for state of matter in a high-mobility electron system in graphene. Unexpectedly, the electron flow is found to be interaction-dominated but non-hydrodynamic (quasiballistic) in a wide temperature range, showing signatures of viscous flows only at relatively high temperatures. The transition between the two regimes is characterized by a sharp maximum of negative resistance, probed in proximity to the current injector. The resistance decreases as the system goes deeper into the hydrodynamic regime. In a perfect darkness-before-daybreak manner, the interaction-dominated negative response is strongest at the transition to the quasiballistic regime. Our work provides the first demonstration of how the viscous fluid behavior emerges in an interacting electron system., Comment: 8pgs, 4fgs

It is well known that superconductivity in thin films is generally suppressed with decreasing thickness. This suppression is normally governed by either disorder-induced localization of Cooper pairs, weakening of Coulomb screening, or generation and unbinding of vortex-antivortex pairs as described by the Berezinskii-Kosterlitz-Thouless (BKT) theory. Defying general expectations, few-layer NbSe2 - an archetypal example of ultrathin superconductors - has been found to remain superconducting down to monolayer thickness. Here we report measurements of both the superconducting energy gap and critical temperature in high-quality monocrystals of few-layer NbSe2, using planar-junction tunneling spectroscopy and lateral transport. We observe a fully developed gap that rapidly reduces for devices with the number of layers N < 5, as does their ctitical temperature. We show that the observed reduction cannot be explained by disorder, and the BKT mechanism is also excluded by measuring its transition temperature that for all N remains very close to Tc. We attribute the observed behavior to changes in the electronic band structure predicted for mono- and bi- layer NbSe2 combined with inevitable suppression of the Cooper pair density at the superconductor-vacuum interface. Our experimental results for N > 2 are in good agreement with the dependences of the gap and Tc expected in the latter case while the effect of band-structure reconstruction is evidenced by a stronger suppression of the gap and the disappearance of its anisotropy for N = 2. The spatial scale involved in the surface suppression of the density of states is only a few angstroms but cannot be ignored for atomically thin superconductors., Comment: 21 pages, including supporting information

The growing family of two-dimensional (2D) materials that are now available can be used to assemble van der Waals heterostructures with a wide range of properties. Of particular interest are tunnelling heterostructures, which have been used to study the electronic states both in the tunnelling barrier and in the emitter and collector contacts. Recently, 2D ferromagnets have been studied theoretically and experimentally. Here we investigate electron tunnelling through a thin (2-6 layers) ferromagnetic CrBr3 barrier. For devices with non-magnetic barriers, conservation of momentum can be relaxed by phonon-assisted tunnelling or by tunnelling through localised states. In the case of our ferromagnetic barrier the dominant tunnelling mechanisms are the emission of magnons at low temperatures or scattering of electrons on localised magnetic excitations above the Curie temperature. Tunnelling with magnon emission offers the possibility of injecting spin into the collector electrode.

Graphene has recently been shown to be permeable to thermal protons, the nuclei of hydrogen atoms, which sparked interest in its use as a proton-conducting membrane in relevant technologies. However, the influence of light on proton permeation remains unknown. Here we report that proton transport through Pt-nanoparticle-decorated graphene can be enhanced strongly by illuminating it with visible light. Using electrical measurements and mass spectrometry, we find a photoresponsivity of 10^4 A W-1, which translates into a gain of 10^4 protons per photon with response times in the microsecond range. These characteristics are competitive with those of state-of-the-art photodetectors that are based on electron transport using silicon and novel two-dimensional materials. The photo-proton effect can be important for graphene's envisaged use in fuel cells and hydrogen isotope separation. Our observations can also be of interest for other applications such as light-induced water splitting, photocatalysis and novel photodetectors.

Conversion of electric current into heat involves microscopic processes that operate on nanometer length-scales and release minute amounts of power. While central to our understanding of the electrical properties of materials, individual mediators of energy dissipation have so far eluded direct observation. Using scanning nano-thermometry with sub-micro K sensitivity we visualize and control phonon emission from individual atomic defects in graphene. The inferred electron-phonon 'cooling power spectrum' exhibits sharp peaks when the Fermi level comes into resonance with electronic quasi-bound states at such defects, a hitherto uncharted process. Rare in the bulk but abundant at graphene's edges, switchable atomic-scale phonon emitters define the dominant dissipation mechanism. Our work offers new insights for addressing key materials challenges in modern electronics and engineering dissipation at the nanoscale.

Coherent manipulation of binary degrees of freedom is at the heart of modern quantum technologies. Graphene offers two binary degrees: the electron spin and the valley. Efficient spin control has been demonstrated in many solid state systems, while exploitation of the valley has only recently been started, yet without control on the single electron level. Here, we show that van-der Waals stacking of graphene onto hexagonal boron nitride offers a natural platform for valley control. We use a graphene quantum dot induced by the tip of a scanning tunneling microscope and demonstrate valley splitting that is tunable from -5 to +10 meV (including valley inversion) by sub-10-nm displacements of the quantum dot position. This boosts the range of controlled valley splitting by about one order of magnitude. The tunable inversion of spin and valley states should enable coherent superposition of these degrees of freedom as a first step towards graphene-based qubits.

Research on black phosphorus (BP) has been experiencing a renaissance over the last few years, after the demonstration that few-layer BP exhibits high carrier mobility and a thickness-dependent band gap. For a long time, bulk BP is also known to be a superconductor under high pressure exceeding 10 GPa. The superconductivity is due to a structural transformation into another allotrope of phosphorous and accompanied by a semiconductor-metal transition. No superconductivity could be achieved for BP itself (that is, in its normal orthorhombic form) despite several attempts reported in the literature. Here we describe successful intercalation of BP by several alkali metals (Li, K, Rb, Cs) and alkali-earth Ca. All the intercalated compounds are found to be superconducting, exhibiting the same (within our experimental accuracy) critical temperature of 3.8+-0.1 K and practically identical characteristics in the superconducting state. Such universal superconductivity, independent of the chemical composition, is highly unusual. We attribute it to intrinsic superconductivity of heavily-doped individual phosphorene layers, while the intercalated layers of metal atoms mostly play a role of charge reservoirs., Comment: 16 pages; 4 figures in the main text and 9 supplementary figures

The electrostatic confinement of massless charge carriers is hampered by Klein tunneling. Circumventing this problem in graphene mainly relies on carving out nanostructures or applying electric displacement fields to open a band gap in bilayer graphene. So far, these approaches suffer from edge disorder or insufficiently controlled localization of electrons. Here we realize an alternative strategy in monolayer graphene, by combining a homogeneous magnetic field and electrostatic confinement. Using the tip of a scanning tunneling microscope, we induce a confining potential in the Landau gaps of bulk graphene without the need for physical edges. Gating the localized states towards the Fermi energy leads to regular charging sequences with more than 40 Coulomb peaks exhibiting typical addition energies of 7-20 meV. Orbital splittings of 4-10 meV and a valley splitting of about 3 meV for the first orbital state can be deduced. These experimental observations are quantitatively reproduced by tight binding calculations, which include the interactions of the graphene with the aligned hexagonal boron nitride substrate. The demonstrated confinement approach appears suitable to create quantum dots with well-defined wave function properties beyond the reach of traditional techniques.

In highly viscous electron systems such as, for example, high quality graphene above liquid nitrogen temperature, a linear response to applied electric current becomes essentially nonlocal, which can give rise to a number of new and counterintuitive phenomena including negative nonlocal resistance and current whirlpools. It has also been shown that, although both effects originate from high electron viscosity, a negative voltage drop does not principally require current backflow. In this work, we study the role of geometry on viscous flow and show that confinement effects and relative positions of injector and collector contacts play a pivotal role in the occurrence of whirlpools. Certain geometries may exhibit backflow at arbitrarily small values of the electron viscosity, whereas others require a specific threshold value for whirlpools to emerge.

Two-dimensional materials are characterised by a number of unique physical properties which can potentially make them useful to a wide diversity of applications. In particular, the large thermal conductivity of graphene and hexagonal boron nitride has already been acknowledged and these materials have been suggested as novel core materials for thermal management in electronics. However, it was not clear if mass produced flakes of hexagonal boron nitride would allow one to achieve an industrially-relevant value of thermal conductivity. Here we demonstrate that laminates of hexagonal boron nitride exhibit thermal conductivity of up to 20 W/mK, which is significantly larger than that currently used in thermal management. We also show that the thermal conductivity of laminates increases with the increasing volumetric mass density, which creates a way of fine-tuning its thermal properties., Comment: 6 pages, 4 figures

Understanding magnetoresistance, the change in electrical resistance upon an external magnetic field, at the atomic level is of great interest both fundamentally and technologically. Graphene and other two-dimensional layered materials provide an unprecedented opportunity to explore magnetoresistance at its nascent stage of structural formation. Here, we report an extremely large local magnetoresistance of ~ 2,000% at 400 K and a non-local magnetoresistance of > 90,000% in 9 T at 300 K in few-layer graphene/boron-nitride heterostructures. The local magnetoresistance is understood to arise from large differential transport parameters, such as the carrier mobility, across various layers of few-layer graphene upon a normal magnetic field, whereas the non-local magnetoresistance is due to the magnetic field induced Ettingshausen-Nernst effect. Non-local magnetoresistance suggests the possibility of a graphene based gate tunable thermal switch. In addition, our results demonstrate that graphene heterostructures may be promising for magnetic field sensing applications.

Few-layer black phosphorus was recently rediscovered as a narrow-bandgap atomically thin semiconductor and has already attracted unprecedented attention due to its interesting properties. One feature of this material that sets it apart from other atomically thin crystals is its structural in-plane anisotropy which manifests in strongly anisotropic transport characteristics. However, traditional angle-resolved conductance measurements present a challenge for nanoscale systems such as black phosphorus, calling for new approaches in precision studies of transport anisotropy. Here we show that the nonlocal response, being exponentially sensitive to the anisotropy value, provides a powerful tool for determining the anisotropy. This is established by combining measurements of the orientation-dependent nonlocal resistance response with the analysis based on the anamorphosis relations. We demonstrate that the nonlocal response can differ by orders of magnitude for different crystallographic directions even when the anisotropy is at most order-one, allowing us to extract accurate anisotropy values.

Motivated by recent experimental progress in preparing encapsulated graphene sheets with ultra-high mobilities up to room temperature, we present a theoretical study of dc transport in doped graphene in the hydrodynamic regime. By using the continuity and Navier-Stokes equations, we demonstrate analytically that measurements of non-local resistances in multi-terminal Hall bar devices can be used to extract the hydrodynamic shear viscosity of the two-dimensional (2D) electron liquid in graphene. We also discuss how to probe the viscosity-dominated hydrodynamic transport regime by scanning probe potentiometry and magnetometry. Our approach enables measurements of the viscosity of any 2D electron liquid in the hydrodynamic transport regime., Comment: 12 pages, 4 multi-panel figures

One of the most desirable goals of graphene research is to produce ordered 2D chemical derivatives of suitable quality for monolayer device fabrication. Here we reveal, by focal series exit wave reconstruction, that C2F chair is a stable graphene derivative and demonstrates pristine long-range order limited only by the size of a functionalized domain. Focal series of images of graphene and C2F chair formed by reaction with XeF2 were obtained at 80 kV in an aberration-corrected transmission electron microscope. EWR images reveal that single carbon atoms and carbon-fluorine pairs in C2F chair alternate strictly over domain sizes of at least 150 nm^2 with electron diffraction indicating ordered domains >/= 0.16 square micrometer. Our results also indicate that, within an ordered domain, functionalization occurs on one side only as theory predicts. Additionally we show that electron diffraction provides a quick and easy method for distinguishing between graphene, C2F chair and fully fluorinated stoichiometric CF 2D phases.

The celebrated electronic properties of graphene have opened way for materials just one-atom-thick to be used in the post-silicon electronic era. An important milestone was the creation of heterostructures based on graphene and other two-dimensional (2D) crystals, which can be assembled in 3D stacks with atomic layer precision. These layered structures have already led to a range of fascinating physical phenomena, and also have been used in demonstrating a prototype field effect tunnelling transistor - a candidate for post-CMOS technology. The range of possible materials which could be incorporated into such stacks is very large. Indeed, there are many other materials where layers are linked by weak van der Waals forces, which can be exfoliated and combined together to create novel highly-tailored heterostructures. Here we describe a new generation of field effect vertical tunnelling transistors where 2D tungsten disulphide serves as an atomically thin barrier between two layers of either mechanically exfoliated or CVD-grown graphene. Our devices have unprecedented current modulation exceeding one million at room temperature and can also operate on transparent and flexible substrates.

We investigate the electronic properties of heterostructures based on ultrathin hexagonal boron nitride (h-BN) crystalline layers sandwiched between two layers of graphene as well as other conducting materials (graphite, gold). The tunnel conductance depends exponentially on the number of h-BN atomic layers, down to a monolayer thickness. Exponential behaviour of I-V characteristics for graphene/BN/graphene and graphite/BN/graphite devices is determined mainly by the changes in the density of states with bias voltage in the electrodes. Conductive atomic force microscopy scans across h-BN terraces of different thickness reveal a high level of uniformity in the tunnel current. Our results demonstrate that atomically thin h-BN acts as a defect-free dielectric with a high breakdown field; it offers great potential for applications in tunnel devices and in field-effect transistors with a high carrier density in the conducting channel., Comment: 7 pages, 5 figures

In this letter we use graphene bubbles to study the Raman spectrum of graphene under biaxial (e.g. isotropic) strain. Our Gruneisen parameters are in excellent agreement with the theoretical values. Discrepancy in the previously reported values is attributed to the interaction of graphene with the substrate. Bilayer balloons (intentionally pressurized membranes) have been used to avoid the effect of the substrate and to study the dependence of strain on the inter-layer interactions., Comment: 14 pages, 4 figures

Carbon fibres (CF) represent a significant volume fraction of modern structural airframes. Embedded into polymer matrices, they provide significant strength and stiffness gains over unit weight as compared to other competing structural materials. Nevertheless, no conclusive structural model yet exists to account for their extraordinary properties. In particular, polyacrynonitrile (PAN) derived CF are known to be fully turbostratic: the graphene layers are slipped sideways relative to each other, which leads to an inter-graphene distance much greater than graphite. Here, we demonstrate that CF derive their mechanical properties from those of graphene itself. By monitoring the Raman G peak shift with strain for both CF and graphene, we develop a universal master plot relating the G peak strain sensitivity of all types of CF to graphene over a wide range of tensile moduli. A universal value of - average- shift rate with axial stress of ~ -5{\omega}0^-1 (cm^-1 MPa^-1)is calculated for both graphene and all CF exhibiting annular ("onion-skin") morphology., Comment: 25 pages, 5 figs