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Graphene is impermeable to all gases and liquids, and even such a small atom as hydrogen is not expected to penetrate through graphene's dense electronic cloud within billions of years. Here we show that monolayers of graphene and hexagonal boron nitride (hBN) are unexpectedly permeable to thermal protons, hydrogen ions under ambient conditions. As a reference, no proton transport could be detected for a monolayer of molybdenum disulfide, bilayer graphene or multilayer hBN. At room temperature, monolayer hBN exhibits the highest proton conductivity with a low activation energy of about 0.3 eV but graphene becomes a better conductor at elevated temperatures such that its resistivity to proton flow is estimated to fall below 10^-3 Ohm per cm2 above 250 C. The proton barriers can be further reduced by decorating monolayers with catalytic nanoparticles. These atomically thin proton conductors could be of interest for many hydrogen-based technologies., Comment: submitted, pre-edited version

Non-trivial topology of phase is crucial for many important physics phenomena such as, for example, the Aharonov-Bohm effect 1 and the Berry phase 2. Light phase allows one to create "twisted" photons 3, 4 , vortex knots 5, dislocations 6 which has led to an emerging field of singular optics relying on abrupt phase changes 7. Here we demonstrate the feasibility of singular visible-light nanooptics which exploits the benefits of both plasmonic field enhancement and non-trivial topology of light phase. We show that properly designed plasmonic nanomaterials exhibit topologically protected singular phase behaviour which can be employed to radically improve sensitivity of detectors based on plasmon resonances. By using reversible hydrogenation of graphene 8 and a streptavidin-biotin test 9, we demonstrate areal mass sensitivity at a level of femto-grams per mm2 and detection of individual biomolecules, respectively. Our proof-of-concept results offer a way towards simple and scalable single-molecular label-free biosensing technologies., Comment: 19 pages, 4 figures

We report a bipolar field effect tunneling transistor that exploits to advantage the low density of states in graphene and its one atomic layer thickness. Our proof-of-concept devices are graphene heterostructures with atomically thin boron nitride acting as a tunnel barrier. They exhibit room temperature switching ratios ~50, a value that can be enhanced further by optimizing the device structure. These devices have potential for high frequency operation and large scale integration.

We report a stoichiometric derivative of graphene with a fluorine atom attached to each carbon. Raman, optical, structural, micromechanical and transport studies show that the material is qualitatively different from the known graphene-based nonstoichiometric derivatives. Fluorographene is a high-quality insulator (resistivity >10^12 Ohm per square) with an optical gap of 3 eV. It inherits the mechanical strength of graphene, exhibiting Young's modulus of 100 N/m and sustaining strains of 15%. Fluorographene is inert and stable up to 400C even in air, similar to Teflon., Comment: to appear in Small 2010

Surface enhanced Raman scattering (SERS) exploits surface plasmons induced by the incident field in metallic nanostructures to significantly increase the Raman intensity. Graphene provides the ideal prototype two dimensional (2d) test material to investigate SERS. Its Raman spectrum is well known, graphene samples are entirely reproducible, height controllable down to the atomic scale, and can be made virtually defect-free. We report SERS from graphene, by depositing arrays of Au particles of well defined dimensions on graphene/SiO$_2$(300nm)/Si. We detect significant enhancements at 633nm. To elucidate the physics of SERS, we develop a quantitative analytical and numerical theory. The 2d nature of graphene allows for a closed-form description of the Raman enhancement. This scales with the nanoparticle cross section, the fourth power of the Mie enhancement, and is inversely proportional to the tenth power of the separation between graphene and the nanoparticle. One consequence is that metallic nanodisks are an ideal embodiment for SERS in 2d.

We present the first experimental study of optical response of collective plasmon resonances in regular arrays of nanoresonators to local environment. Recently observed collective plasmon modes arise due to diffractive coupling of localised plasmons and yield almost an order of magnitude improvement in resonance quality. We measure the response of these modes to tiny variations of the refractive index of both gaseous and liquid media. We show that the phase sensitivity of the collective resonances can be more than two orders of magnitude better than the best amplitude sensitivity of the same nanodot array as well as an order of magnitude better than the phase sensitivity in SPR sensors., Comment: 10 pages. 2 Figures, 1 Table, accepted to Optics Letters

We show that graphene deposited on a substrate has a non-negligible density of atomic scale defects. This is evidenced by a previously unnoticed D peak in the Raman spectra with intensity of about 1% with respect to the G peak. We evaluated the effect of such impurities on electron transport by mimicking them with hydrogen adsorbates and measuring the induced changes in both mobility and Raman intensity. If the intervalley scatterers responsible for the D peak are monovalent, their concentration is sufficient to account for the limited mobilities achievable in graphene on a substrate., Comment: version 2: several comments are taken into account and refs added

There is an increasing amount of literature concerning electronic properties of graphene close to the neutrality point. Many experiments continue using the two-probe geometry or invasive contacts or do not control samples' macroscopic homogeneity. We believe that it is helpful to point out some problems related to such measurements. By using experimental examples, we illustrate that the charge inhomogeneity induced by spurious chemical doping or metal contacts can lead to large systematic errors in assessing graphene's transport properties and, in particular, its minimal conductivity. The problems are most severe in the case of two-probe measurements where the contact resistance is found to strongly vary as a function of gate voltage.

It is widely assumed that the dominant source of scattering in graphene is charged impurities in a substrate. We have tested this conjecture by studying graphene placed on various substrates and in high-k media. Unexpectedly, we have found no significant changes in carrier mobility either for different substrates or by using glycerol, ethanol and water as a top dielectric layer. This suggests that Coulomb impurities are not the scattering mechanism that limits the mean free path currently attainable for graphene on a substrate., Comment: further experiments proving the point are reported in the final version

Graphene is only one atom thick, optically transparent, chemically inert and an excellent conductor. These properties seem to make this material an excellent candidate for applications in various photonic devices that require conducting but transparent thin films. In this letter we demonstrate liquid crystal devices with electrodes made of graphene which show excellent performance with a high contrast ratio. We also discuss the advantages of graphene compared to conventionally-used metal oxides in terms of low resistivity, high transparency and chemical stability.

We report on transport characteristics of quantum dot devices etched entirely in graphene. At large sizes, they behave as conventional single-electron transistors, exhibiting periodic Coulomb blockade peaks. For quantum dots smaller than 100 nm, the peaks become strongly non-periodic indicating a major contribution of quantum confinement. Random peak spacing and its statistics are well described by the theory of chaotic neutrino (Dirac) billiards. Short constrictions of only a few nm in width remain conductive and reveal a confinement gap of up to 0.5eV, which demonstrates the in-principle possibility of molecular-scale electronics based on graphene.

We have studied temperature dependences of electron transport in graphene and its bilayer and found extremely low electron-phonon scattering rates that set the fundamental limit on possible charge carrier mobilities at room temperature. Our measurements have shown that mobilities significantly higher than 200,000 cm2/Vs are achievable, if extrinsic disorder is eliminated. A sharp (threshold-like) increase in resistivity observed above approximately 200K is unexpected but can qualitatively be understood within a model of a rippled graphene sheet in which scattering occurs on intra-ripple flexural phonons.

Graphene - a single atomic layer of graphite - is a recently-found two-dimensional form of carbon, which exhibits high crystal quality and ballistic electron transport at room temperature. Soft magnetic NiFe electrodes have been used to inject polarized spins into graphene and a 10% change in resistance has been observed as the electrodes switch from the parallel to the antiparallel state. This coupled with the fact that a field effect electrode can modulate the conductivity of these graphene films makes them exciting potential candidates for spin electronic devices., Comment: 3 pages, 6 figures

The ultimate aspiration of any detection method is to achieve such a level of sensitivity that individual quanta of a measured value can be resolved. In the case of chemical sensors, the quantum is one atom or molecule. Such resolution has so far been beyond the reach of any detection technique, including solid-state gas sensors hailed for their exceptional sensitivity. The fundamental reason limiting the resolution of such sensors is fluctuations due to thermal motion of charges and defects which lead to intrinsic noise exceeding the sought-after signal from individual molecules, usually by many orders of magnitude. Here we show that micrometre-size sensors made from graphene are capable of detecting individual events when a gas molecule attaches to or detaches from graphenes surface. The adsorbed molecules change the local carrier concentration in graphene one by one electron, which leads to step-like changes in resistance. The achieved sensitivity is due to the fact that graphene is an exceptionally low-noise material electronically, which makes it a promising candidate not only for chemical detectors but also for other applications where local probes sensitive to external charge, magnetic field or mechanical strain are required., Comment: the final version is significantly different from the earlier 2006 version

Low-field magnetoresistance is ubiquitous in low-dimensional metallic systems with high resistivity and well understood as arising due to quantum interference on self-intersecting diffusive trajectories. We have found that in graphene this weak-localization magnetoresistance is strongly suppressed and, in some cases, completely absent. This unexpected observation is attributed to mesoscopic corrugations of graphene sheets which cause a dephasing effect similar to that of a random magnetic field., Comment: improved presentation of the theory part after referees comments; important experimental info added (see "note added in proof")

There are known two distinct types of the integer quantum Hall effect. One is the conventional quantum Hall effect, characteristic of two-dimensional semiconductor systems, and the other is its relativistic counterpart recently observed in graphene, where charge carriers mimic Dirac fermions characterized by Berry's phase pi, which results in a shifted positions of Hall plateaus. Here we report a third type of the integer quantum Hall effect. Charge carriers in bilayer graphene have a parabolic energy spectrum but are chiral and exhibit Berry's phase 2pi affecting their quantum dynamics. The Landau quantization of these fermions results in plateaus in Hall conductivity at standard integer positions but the last (zero-level) plateau is missing. The zero-level anomaly is accompanied by metallic conductivity in the limit of low concentrations and high magnetic fields, in stark contrast to the conventional, insulating behavior in this regime. The revealed chiral fermions have no known analogues and present an intriguing case for quantum-mechanical studies., Comment: to appear in Nature Physics