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1.
ACS Nano ; 14(1): 993-1002, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31815429

RESUMO

Marcus-Hush theory of electron transfer is one of the pillars of modern electrochemistry with a large body of supporting experimental evidence presented to date. However, some predictions, such as the electrochemical behavior at disk ultramicroelectrodes, remain unverified. Herein, we present a study of electron tunneling across a hexagonal boron nitride acting as a barrier between a graphite electrode and redox mediators in a liquid solution. This was achieved by the fabrication of disk ultramicroelectrodes with a typical diameter of 5 µm. Analysis of voltammetric measurements, using two common outer-sphere redox mediators, yielded several electrochemical parameters, including the electron transfer rate constant, limiting current, and transfer coefficient. They depart significantly from the Butler-Volmer kinetics and instead show behavior previously predicted by the Marcus-Hush theory of electron transfer. In addition, our system provides a noteworthy experimental platform, which could be applied to address a number of scientific problems such as identification of reaction mechanisms, surface modification, or long-range electron transfer.

2.
Nature ; 576(7785): 75-79, 2019 12.
Artigo em Inglês | MEDLINE | ID: mdl-31802019

RESUMO

Hydrodynamics, which generally describes the flow of a fluid, is expected to hold even for fundamental particles such as electrons when inter-particle interactions dominate1. Although various aspects of electron hydrodynamics have been revealed in recent experiments2-11, the fundamental spatial structure of hydrodynamic electrons-the Poiseuille flow profile-has remained elusive. Here we provide direct imaging of the Poiseuille flow of an electronic fluid, as well as a visualization of its evolution from ballistic flow. Using a scanning carbon nanotube single-electron transistor12, 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 temperatures 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 direct confirmation of Poiseuille flow in the solid state, and enable exploration of the rich physics of interacting electrons in real space.

3.
Nano Lett ; 19(12): 8526-8532, 2019 12 11.
Artigo em Inglês | MEDLINE | ID: mdl-31664847

RESUMO

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 visualize 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.

4.
Nano Lett ; 19(9): 6475-6481, 2019 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-31426634

RESUMO

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 used 2D indium selenide (InSe) obtained by exfoliation and converted it by direct fluorination into indium fluoride (InF3), which has a nonlayered, rhombohedral structure and therefore cannot  possibly be 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 noncleavable ones opens exciting prospects for synthesizing a wide variety of novel atomically thin covalent crystals.

5.
Nat Nanotechnol ; 14(8): 756-761, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31285609

RESUMO

When two-dimensional electron gases (2DEGs) are exposed to a magnetic field, they resonantly absorb electromagnetic radiation via electronic transitions between Landau levels1. In 2DEGs with a Dirac spectrum, such as graphene, theory predicts an exceptionally high infrared magneto-absorption, even at zero doping2-5. However, the measured Landau-level magneto-optical effects in graphene have been much weaker than expected2,6-12 because of imperfections in the samples available for such experiments. Here, we measure magneto-transmission and Faraday rotation in high-mobility encapsulated monolayer graphene using a custom-designed set-up for magneto-infrared microspectroscopy. Our results show strongly enhanced magneto-optical activity in the infrared and terahertz ranges, characterized by absorption of light near to the 50% maximum allowed, 100% magnetic circular dichroism and high Faraday rotation. Considering that sizeable effects have been already observed at routinely achievable magnetic fields, our findings demonstrate the potential of magnetic tuning in 2D Dirac materials for long-wavelength optoelectronics and plasmonics.

6.
Phys Rev Lett ; 122(1): 016601, 2019 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-31012652

RESUMO

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.

7.
Nat Nanotechnol ; 14(5): 480-487, 2019 05.
Artigo em Inglês | MEDLINE | ID: mdl-30858521

RESUMO

A variety of physical phenomena associated with nanoscale electron transport often results in non-trivial spatial voltage and current patterns, 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 a magnetic field, across a broad range of temperatures and beneath an insulating surface. Here we present 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 aid in understanding the physics of two-dimensional electronic devices and enable new classes of experiments that image electron flow through buried nanostructures in the quantum and interaction-dominated regimes.

8.
Nat Commun ; 10(1): 987, 2019 02 25.
Artigo em Inglês | MEDLINE | ID: mdl-30804336

RESUMO

The original version of this Article contained an error in the spelling of the author Matthew Holwill, which was incorrectly given as Mathew Holwill. This has now been corrected in both the PDF and HTML versions of the Article.

9.
Nat Commun ; 10(1): 230, 2019 01 16.
Artigo em Inglês | MEDLINE | ID: mdl-30651554

RESUMO

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.

10.
Nat Commun ; 9(1): 5392, 2018 12 19.
Artigo em Inglês | MEDLINE | ID: mdl-30568184

RESUMO

Plasmons, collective oscillations of electron systems, can efficiently couple light and electric current, and thus can be used to create sub-wavelength photodetectors, radiation mixers, and on-chip spectrometers. Despite considerable effort, it has proven challenging to implement plasmonic devices operating at terahertz frequencies. The material capable to meet this challenge is graphene as it supports long-lived electrically tunable plasmons. Here we demonstrate plasmon-assisted resonant detection of terahertz radiation by antenna-coupled graphene transistors that act as both plasmonic Fabry-Perot cavities and rectifying elements. By varying the plasmon velocity using gate voltage, we tune our detectors between multiple resonant modes and exploit this functionality to measure plasmon wavelength and lifetime in bilayer graphene as well as to probe collective modes in its moiré minibands. Our devices offer a convenient tool for further plasmonic research that is often exceedingly difficult under non-ambient conditions (e.g. cryogenic temperatures) and promise a viable route for various photonic applications.

11.
Nat Commun ; 9(1): 4533, 2018 10 31.
Artigo em Inglês | MEDLINE | ID: mdl-30382090

RESUMO

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.

12.
Nat Nanotechnol ; 13(5): 392-397, 2018 05.
Artigo em Inglês | MEDLINE | ID: mdl-29556008

RESUMO

Coherent manipulation of the 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, whereas exploitation of the valley has only recently been started, albeit without control at 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 tunnelling 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.

13.
Nat Nanotechnol ; 13(4): 300-303, 2018 04.
Artigo em Inglês | MEDLINE | ID: mdl-29358638

RESUMO

Graphene has recently been shown to be permeable to thermal protons 1 , the nuclei of hydrogen atoms, which sparked interest in its use as a proton-conducting membrane in relevant technologies1-4. 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 ∼104 A W-1, which translates into a gain of ∼104 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 materials5-7. The photo-proton effect could be important for graphene's envisaged use in fuel cells and hydrogen isotope separation. Our observations may also be of interest for other applications such as light-induced water splitting, photocatalysis and novel photodetectors.

14.
Science ; 358(6368): 1303-1306, 2017 12 08.
Artigo em Inglês | MEDLINE | ID: mdl-29217571

RESUMO

Conversion of electric current into heat involves microscopic processes that operate on nanometer length scales and release minute amounts of power. Although central to our understanding of the electrical properties of materials, individual mediators of energy dissipation have so far eluded direct observation. Using scanning nanothermometry with submicrokelvin sensitivity, we visualized and controlled phonon emission from individual atomic-scale 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. Rare in the bulk but abundant at graphene's edges, switchable atomic-scale phonon emitters provide the dominant dissipation mechanism. Our work offers insights for addressing key materials challenges in modern electronics and enables control of dissipation at the nanoscale.

15.
Nat Nanotechnol ; 12(6): 546-550, 2017 07.
Artigo em Inglês | MEDLINE | ID: mdl-28369049

RESUMO

Graphene oxide membranes show exceptional molecular permeation properties, with promise for many applications. However, their use in ion sieving and desalination technologies is limited by a permeation cutoff of ∼9 Š(ref. 4), which is larger than the diameters of hydrated ions of common salts. The cutoff is determined by the interlayer spacing (d) of ∼13.5 Å, typical for graphene oxide laminates that swell in water. Achieving smaller d for the laminates immersed in water has proved to be a challenge. Here, we describe how to control d by physical confinement and achieve accurate and tunable ion sieving. Membranes with d from ∼9.8 Što 6.4 Šare demonstrated, providing a sieve size smaller than the diameters of hydrated ions. In this regime, ion permeation is found to be thermally activated with energy barriers of ∼10-100 kJ mol-1 depending on d. Importantly, permeation rates decrease exponentially with decreasing sieve size but water transport is weakly affected (by a factor of <2). The latter is attributed to a low barrier for the entry of water molecules and large slip lengths inside graphene capillaries. Building on these findings, we demonstrate a simple scalable method to obtain graphene-based membranes with limited swelling, which exhibit 97% rejection for NaCl.

16.
Nano Lett ; 17(3): 1425-1430, 2017 03 08.
Artigo em Inglês | MEDLINE | ID: mdl-28211273

RESUMO

We report on experimental investigations of an electrically driven WSe2 based light-emitting van der Waals heterostructure. We observe a threshold voltage for electroluminescence significantly lower than the corresponding single particle band gap of monolayer WSe2. This observation can be interpreted by considering the Coulomb interaction and a tunneling process involving excitons, well beyond the picture of independent charge carriers. An applied magnetic field reveals pronounced magneto-oscillations in the electroluminescence of the free exciton emission intensity with a 1/B periodicity. This effect is ascribed to a modulation of the tunneling probability resulting from the Landau quantization in the graphene electrodes. A sharp feature in the differential conductance indicates that the Fermi level is pinned and allows for an estimation of the acceptor binding energy.

17.
Nat Nanotechnol ; 12(3): 223-227, 2017 03.
Artigo em Inglês | MEDLINE | ID: mdl-27870843

RESUMO

A decade of intense research on two-dimensional (2D) atomic crystals has revealed that their properties can differ greatly from those of the parent compound. These differences are governed by changes in the band structure due to quantum confinement and are most profound if the underlying lattice symmetry changes. Here we report a high-quality 2D electron gas in few-layer InSe encapsulated in hexagonal boron nitride under an inert atmosphere. Carrier mobilities are found to exceed 103 cm2 V-1 s-1 and 104 cm2 V-1 s-1 at room and liquid-helium temperatures, respectively, allowing the observation of the fully developed quantum Hall effect. The conduction electrons occupy a single 2D subband and have a small effective mass. Photoluminescence spectroscopy reveals that the bandgap increases by more than 0.5 eV with decreasing the thickness from bulk to bilayer InSe. The band-edge optical response vanishes in monolayer InSe, which is attributed to the monolayer's mirror-plane symmetry. Encapsulated 2D InSe expands the family of graphene-like semiconductors and, in terms of quality, is competitive with atomically thin dichalcogenides and black phosphorus.

18.
Nano Lett ; 16(9): 5798-805, 2016 09 14.
Artigo em Inglês | MEDLINE | ID: mdl-27466881

RESUMO

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 toward 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.

19.
ACS Nano ; 10(3): 3685-92, 2016 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-26882095

RESUMO

The rate of water flow through hydrophobic nanocapillaries is greatly enhanced as compared to that expected from macroscopic hydrodynamics. This phenomenon is usually described in terms of a relatively large slip length, which is in turn defined by such microscopic properties as the friction between water and capillary surfaces and the viscosity of water. We show that the viscosity of water and, therefore, its flow rate are profoundly affected by the layered structure of confined water if the capillary size becomes less than 2 nm. To this end, we study the structure and dynamics of water confined between two parallel graphene layers using equilibrium molecular dynamics simulations. We find that the shear viscosity is not only greatly enhanced for subnanometer capillaries, but also exhibits large oscillations that originate from commensurability between the capillary size and the size of water molecules. Such oscillating behavior of viscosity and, consequently, the slip length should be taken into account in designing and studying graphene-based and similar membranes for desalination and filtration.

20.
Sci Rep ; 5: 18298, 2015 Dec 17.
Artigo em Inglês | MEDLINE | ID: mdl-26673395

RESUMO

In this paper, we report highly conductive, highly flexible, light weight and low cost printed graphene for wireless wearable communications applications. As a proof of concept, printed graphene enabled transmission lines and antennas on paper substrates were designed, fabricated and characterized. To explore its potentials in wearable communications applications, mechanically flexible transmission lines and antennas under various bended cases were experimentally studied. The measurement results demonstrate that the printed graphene can be used for RF signal transmitting, radiating and receiving, which represents some of the essential functionalities of RF signal processing in wireless wearable communications systems. Furthermore, the printed graphene can be processed at low temperature so that it is compatible with heat-sensitive flexible materials like papers and textiles. This work brings a step closer to the prospect to implement graphene enabled low cost and environmentally friendly wireless wearable communications systems in the near future.


Assuntos
Grafite/química , Impressão/instrumentação , Processamento de Sinais Assistido por Computador/instrumentação , Tecnologia sem Fio/instrumentação , Condutividade Elétrica , Microscopia Eletrônica de Varredura , Nanocompostos/química , Nanocompostos/ultraestrutura , Papel , Porosidade , Impressão/métodos
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