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1.
Nature ; 516(7530): 227-30, 2014 Dec 11.
Article in English | MEDLINE | ID: mdl-25470058

ABSTRACT

Graphene is increasingly explored as a possible platform for developing novel separation technologies. This interest has arisen because it is a maximally thin membrane that, once perforated with atomic accuracy, may allow ultrafast and highly selective sieving of gases, liquids, dissolved ions and other species of interest. However, a perfect graphene monolayer is impermeable to all atoms and molecules under ambient conditions: even hydrogen, the smallest of atoms, is expected to take billions of years to penetrate graphene's dense electronic cloud. Only accelerated atoms possess the kinetic energy required to do this. The same behaviour might reasonably be expected in the case of other atomically thin crystals. Here we report transport and mass spectroscopy measurements which establish that monolayers of graphene and hexagonal boron nitride (hBN) are highly permeable to thermal protons under ambient conditions, whereas no proton transport is detected for thicker crystals such as monolayer molybdenum disulphide, bilayer graphene or multilayer hBN. Protons present an intermediate case between electrons (which can tunnel easily through atomically thin barriers) and atoms, yet our measured transport rates are unexpectedly high and raise fundamental questions about the details of the transport process. We see the highest room-temperature proton conductivity with monolayer hBN, for which we measure a resistivity to proton flow of about 10 Ω cm(2) and a low activation energy of about 0.3 electronvolts. At higher temperatures, hBN is outperformed by graphene, the resistivity of which is estimated to fall below 10(-3) Ω cm(2) above 250 degrees Celsius. Proton transport can be further enhanced by decorating the graphene and hBN membranes with catalytic metal nanoparticles. The high, selective proton conductivity and stability make one-atom-thick crystals promising candidates for use in many hydrogen-based technologies.

2.
Nat Mater ; 12(4): 304-9, 2013 Apr.
Article in English | MEDLINE | ID: mdl-23314104

ABSTRACT

The non-trivial behaviour of phase is crucial for many important physical phenomena, such as, for example, the Aharonov-Bohm effect and the Berry phase. By manipulating the phase of light one can create 'twisted' photons, vortex knots and dislocations which has led to the emergence of the field of singular optics relying on abrupt phase changes. Here we demonstrate the feasibility of singular visible-light nano-optics which exploits the benefits of both plasmonic field enhancement and the peculiarities of the phase of light. We show that properly designed plasmonic metamaterials exhibit topologically protected zero reflection yielding to sharp phase changes nearby, which can be employed to radically improve the sensitivity of detectors based on plasmon resonances. By using reversible hydrogenation of graphene and binding of streptavidin-biotin, we demonstrate an areal mass sensitivity at a level of fg mm(-2) and detection of individual biomolecules, respectively. Our proof-of-concept results offer a route towards simple and scalable single-molecule label-free biosensing technologies.

3.
Science ; 335(6071): 947-50, 2012 Feb 24.
Article in English | MEDLINE | ID: mdl-22300848

ABSTRACT

An obstacle to the use of graphene as an alternative to silicon electronics has been the absence of an energy gap between its conduction and valence bands, which makes it difficult to achieve low power dissipation in the OFF state. We report a bipolar field-effect transistor that exploits the low density of states in graphene and its one-atomic-layer thickness. Our prototype devices are graphene heterostructures with atomically thin boron nitride or molybdenum disulfide acting as a vertical transport barrier. They exhibit room-temperature switching ratios of ≈50 and ≈10,000, respectively. Such devices have potential for high-frequency operation and large-scale integration.

4.
Nat Commun ; 3: 640, 2012 Jan 24.
Article in English | MEDLINE | ID: mdl-22273678

ABSTRACT

Optics is renowned for displaying quantum phenomena. Indeed, studies of emission and absorption lines, the photoelectric effect and blackbody radiation helped to build the foundations of quantum mechanics. Nevertheless, it came as a surprise that the visible transparency of suspended graphene is determined solely by the fine structure constant, as this kind of universality had been previously reserved only for quantized resistance and flux quanta in superconductors. Here we describe a plasmonic system in which relative optical transparency is determined solely by the fine structure constant. The system consists of a regular array of gold nanoparticles fabricated on a thin metallic sublayer. We show that its relative transparency can be quantized in the near-infrared, which we attribute to the quantized contact resistance between the nanoparticles and the metallic sublayer. Our results open new possibilities in the exploration of universal dynamic conductance in plasmonic nanooptics.


Subject(s)
Gold/chemistry , Absorption , Graphite/chemistry , Materials Testing , Metal Nanoparticles/chemistry , Models, Statistical , Nanoparticles/chemistry , Nanotechnology/methods , Optics and Photonics , Physics/methods , Surface Properties
5.
Nano Lett ; 10(10): 3868-72, 2010 Oct 13.
Article in English | MEDLINE | ID: mdl-20795655

ABSTRACT

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 ∼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 currently achievable in graphene on a substrate.

6.
Opt Lett ; 35(7): 956-8, 2010 Apr 01.
Article in English | MEDLINE | ID: mdl-20364182

ABSTRACT

We present what we believe to be the first experimental study of the 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 localized plasmons and yield almost 1 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 2 orders of magnitude better than the best amplitude sensitivity of the same nanodot array as well as 1 order of magnitude better than the phase sensitivity in surface plasmon resonance sensors.


Subject(s)
Gold/chemistry , Nanostructures/chemistry , Nanostructures/ultrastructure , Nanotechnology/instrumentation , Surface Plasmon Resonance/instrumentation , Transducers , Computer-Aided Design , Equipment Design , Equipment Failure Analysis , Reproducibility of Results , Sensitivity and Specificity
7.
Nano Lett ; 10(3): 874-9, 2010 Mar 10.
Article in English | MEDLINE | ID: mdl-20143865

ABSTRACT

We present results from composite plasmonic nanostructures designed to achieve the cascaded enhancement of electromagnetic fields at optical frequencies. Our structures comprise a small metallic nanodisc suspended above a larger disk. We probe the optical properties of these structures by coating them with a layer of a visible-light fluorophore and observing fluorescence signals with the help of scanning confocal microscopy. A 43 +/- 5-fold increase in the far-field fluorescence signal has been observed for two-tier composite nanostructures, when compared to the signal obtained from individual nanodiscs. Our results offer the prospect of using such nanostructures for field concentration, optical manipulation of nanoobjects, chemical and biological sensing.


Subject(s)
Gold/chemistry , Nanostructures/chemistry , Nanostructures/ultrastructure , Nanotechnology/methods , Spectrometry, Fluorescence/methods , Surface Plasmon Resonance/methods , Crystallization/methods , Light , Macromolecular Substances/chemistry , Materials Testing , Molecular Conformation , Particle Size , Surface Properties
8.
Phys Rev Lett ; 105(24): 246806, 2010 Dec 10.
Article in English | MEDLINE | ID: mdl-21231549

ABSTRACT

We present composite plasmonic nanostructures designed to achieve cascaded enhancement of electromagnetic fields at optical frequencies. Our structures were made with the help of electron-beam lithography and comprise a set of metallic nanodisks placed one above another. The optical properties of reproducible arrays of these structures were studied by using scanning confocal Raman spectroscopy. We show that our composite nanostructures robustly demonstrate dramatic enhancement of the Raman signals when compared to those measured from constituent elements.

9.
Phys Rev Lett ; 102(20): 206603, 2009 May 22.
Article in English | MEDLINE | ID: mdl-19519058

ABSTRACT

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-kappa 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 attainable for graphene on a substrate.

10.
Phys Rev Lett ; 101(8): 087403, 2008 Aug 22.
Article in English | MEDLINE | ID: mdl-18764660

ABSTRACT

We experimentally demonstrate extremely narrow plasmon resonances with half-width of just several nanometers in regular arrays of metallic nanoparticles. These resonances are observed at Rayleigh's cutoff wavelengths for Wood anomalies and based on diffraction coupling of localized plasmons. We show experimentally that reflection from an array of nanoparticles can be completely suppressed at certain wavelengths. As a result, our metal nanostructures exhibit pi-jump for the phase of the reflected light.

11.
Science ; 320(5874): 356-8, 2008 Apr 18.
Article in English | MEDLINE | ID: mdl-18420930

ABSTRACT

The exceptional electronic properties of graphene, with its charge carriers mimicking relativistic quantum particles and its formidable potential in various applications, have ensured a rapid growth of interest in this new material. We report on electron transport in quantum dot devices carved entirely from graphene. At large sizes (>100 nanometers), they behave as conventional single-electron transistors, exhibiting periodic Coulomb blockade peaks. For quantum dots smaller than 100 nanometers, the peaks become strongly nonperiodic, indicating a major contribution of quantum confinement. Random peak spacing and its statistics are well described by the theory of chaotic neutrino billiards. Short constrictions of only a few nanometers in width remain conductive and reveal a confinement gap of up to 0.5 electron volt, demonstrating the possibility of molecular-scale electronics based on graphene.

12.
Phys Rev Lett ; 100(1): 016602, 2008 Jan 11.
Article in English | MEDLINE | ID: mdl-18232798

ABSTRACT

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 show that mobilities higher than 200 000 cm2/V s are achievable, if extrinsic disorder is eliminated. A sharp (thresholdlike) increase in resistivity observed above approximately 200 K is unexpected but can qualitatively be understood within a model of a rippled graphene sheet in which scattering occurs on intraripple flexural phonons.

13.
Nat Mater ; 6(9): 652-5, 2007 Sep.
Article in English | MEDLINE | ID: mdl-17660825

ABSTRACT

The ultimate aim of any detection method is to achieve such a level of sensitivity that individual quanta of a measured entity 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 graphene's 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.

14.
Phys Rev Lett ; 97(1): 016801, 2006 Jul 07.
Article in English | MEDLINE | ID: mdl-16907394

ABSTRACT

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. The unexpected observation is attributed to mesoscopic corrugations of graphene sheets which can cause a dephasing effect similar to that of a random magnetic field.

15.
Proc Natl Acad Sci U S A ; 102(30): 10451-3, 2005 Jul 26.
Article in English | MEDLINE | ID: mdl-16027370

ABSTRACT

We report free-standing atomic crystals that are strictly 2D and can be viewed as individual atomic planes pulled out of bulk crystals or as unrolled single-wall nanotubes. By using micromechanical cleavage, we have prepared and studied a variety of 2D crystals including single layers of boron nitride, graphite, several dichalcogenides, and complex oxides. These atomically thin sheets (essentially gigantic 2D molecules unprotected from the immediate environment) are stable under ambient conditions, exhibit high crystal quality, and are continuous on a macroscopic scale.

16.
Phys Rev Lett ; 86(17): 3811-4, 2001 Apr 23.
Article in English | MEDLINE | ID: mdl-11329330

ABSTRACT

The structures of the polar surfaces of ZnO are studied using ab initio calculations and surface x-ray diffraction. The experimental and theoretical relaxations are in good agreement. The polar surfaces are shown to be very stable; the cleavage energy for the (0001)-Zn and (0001;)-O surfaces is 4.0 J/m(2) comparable to 2.32 J/m(2) for the most stable nonpolar (1010) surface. The surfaces are stabilized by an electronic mechanism involving the transfer of 0.17 electrons between them. This leads to 2D metallic surface states, which has implications for the use of the material in gas sensing and catalytic applications.

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