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Controlled transport of water molecules through membranes and capillaries is important in areas as diverse as water purification and healthcare technologies 1 – 7 . Previous attempts to control water permeation through membranes (mainly polymeric ones) have concentrated on modulating the structure of the membrane and the physicochemical properties of its surface by varying the pH, temperature or ionic strength 3 , 8 . Electrical control over water transport is an attractive alternative; however, theory and simulations 9 – 14 have often yielded conflicting results, from freezing of water molecules to melting of ice 14 – 16 under an applied electric field. Here we report electrically controlled water permeation through micrometre-thick graphene oxide membranes 17 – 21 . Such membranes have previously been shown to exhibit ultrafast permeation of water 17 , 22 and molecular sieving properties 18 , 21 , with the potential for industrial-scale production. To achieve electrical control over water permeation, we create conductive filaments in the graphene oxide membranes via controllable electrical breakdown. The electric field that concentrates around these current-carrying filaments ionizes water molecules inside graphene capillaries within the graphene oxide membranes, which impedes water transport. We thus demonstrate precise control of water permeation, from ultrafast permeation to complete blocking. Our work opens up an avenue for developing smart membrane technologies for artificial biological systems, tissue engineering and filtration. The rapid water transport through graphene oxide membranes can be switched off by introducing localized electric fields within the membranes that ionize surrounding water molecules and thus block transport.

Van der Waals assembly of two-dimensional crystals continue attract intense interest due to the prospect of designing novel materials with on-demand properties. One of the unique features of this technology is the possibility of trapping molecules between two-dimensional crystals. The trapped molecules are predicted to experience pressures as high as 1 GPa. Here we report measurements of this interfacial pressure by capturing pressure-sensitive molecules and studying their structural and conformational changes. Pressures of 1.2±0.3 GPa are found using Raman spectrometry for molecular layers of 1-nm in thickness. We further show that this pressure can induce chemical reactions, and several trapped salts are found to react with water at room temperature, leading to two-dimensional crystals of the corresponding oxides. This pressure and its effect should be taken into account in studies of van der Waals heterostructures and can also be exploited to modify materials confined at the atomic interfaces. Molecules trapped between the layers of two-dimensional materials are thought to experience high pressure. Here, the authors report measurements of this interfacial pressure by capturing pressure-sensitive molecules and studying their structural changes, and show that it can also induce chemical reaction.

Van der Waals (vdW) interaction between two-dimensional crystals (2D) can trap substances in high pressurized (of order 1 GPa) on nanobubbles. Increasing the adhesion between the 2D crystals further enhances the pressure and can lead to a phase transition of the trapped material. We found that the shape of the nanobubble can depend critically on the properties of the trapped substance. In the absence of any residual strain in the top 2D crystal, flat nanobubbles can be formed by trapped long hydrocarbons (that is, hexadecane). For large nanobubbles with radius 130 nm, our atomic force microscopy measurements show nanobubbles filled with hydrocarbons (water) have a cylindrical symmetry (asymmetric) shape which is in good agreement with our molecular dynamics simulations. This study provides insights into the effects of the specific material and the vdW pressure on the microscopic details of graphene bubbles. Graphene nanobubbles can act as enclosures for holding small volumes of substances. Here the authors find a correlation between bubble shape and the encapsulated material providing a potential method for determining the graphene bubble content by its deformation.

Developing 'smart' membranes that allow precise and reversible control of molecular permeation using external stimuli would be of intense interest for many areas of science: from physics and chemistry to life-sciences. In particular, electrical control of water permeation through membranes is a long-sought objective and is of crucial importance for healthcare and related areas. Currently, such adjustable membranes are limited to the modulation of wetting of the membranes and controlled ion transport, but not the controlled mass flow of water. Despite intensive theoretical work yielding conflicting results, the experimental realisation of electrically controlled water permeation has not yet been achieved. Here we report electrically controlled water permeation through micrometre-thick graphene oxide (GO) membranes. By controllable electric breakdown, conductive filaments are created in the GO membrane. The electric field concentrated around such current carrying filaments leads to controllable ionisation of water molecules in graphene capillaries, allowing precise control of water permeation: from ultrafast permeation to complete blocking. Our work opens up an avenue for developing smart membrane technologies and can revolutionize the field of artificial biological systems, tissue engineering and filtration.

Graphene oxide membranes show exceptional molecular permeation properties, with a promise for many applications. However, their use in ion sieving and desalination technologies is limited by a permeation cutoff of ~9 Angstrom, which is larger than hydrated ion diameters for common salts. The cutoff is determined by the interlayer spacing d ~13.5 Angstrom, 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 tuneable ion sieving. Membranes with d from ~ 9.8 Angstrom to 6.4 Angstrom are demonstrated, providing the sieve size smaller than typical ions' hydrated diameters.In this regime, ion permeation is found to be thermally activated with energy barriers of ~10-100 kJ/mol depending on d. Importantly, permeation rates decrease exponentially with decreasing the sieve size but water transport is weakly affected (by a factor of <2). The latter is attributed to a low barrier for water molecules entry 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.

Van der Waals assembly of two-dimensional (2D) crystals continue attract intense interest due to the prospect of designing novel materials with on-demand properties. One of the unique features of this technology is the possibility of trapping molecules or compounds between 2D crystals. The trapped molecules are predicted to experience pressures as high as 1 GPa. Here we report measurements of this interfacial pressure by capturing pressure-sensitive molecules and studying their structural and conformational changes. Pressures of 1.2 +/- 0.3 GPa are found using Raman spectrometry for molecular layers of one nanometer in thickness. We further show that this pressure can induce chemical reactions and several trapped salts or compounds are found to react with water at room temperature, leading to 2D crystals of the corresponding oxides. This pressure and its effect should be taken into account in studies of van der Waals heterostructures and can also be exploited to modify materials confined at the atomic interfaces.

We report ultrafast response of femtosecond photoexcited carriers in single layer reduced graphene oxide flakes suspended in water as well as few layer thick film deposited on indium tin oxide coated glass plate using pump-probe differential transmission spectroscopy at 790 nm. The carrier relaxation dynamics has three components: ~200 fs, 1 to 2 ps, and ~25 ps, all of them independent of pump fluence. It is seen that the second component (1 to 2 ps) assigned to the lifetime of hot optical phonons is larger for graphene in suspensions whereas other two time constants are the same for both the suspension and the film. The value of third order nonlinear susceptibility estimated from the pump-probe experiments is compared with that obtained from the open aperture Z-scan results for the suspension.

We demonstrate top-gated field effect transistor made of reduced graphene oxide (RGO) monolayer (graphene) by dielectrophoresis. Raman spectrum of RGO flakes of typical size of 5{\\mu}m x 5{\\mu}m show a single 2D band at 2687 cm-1, characteristic of a single layer graphene. The two probe current - voltage measurements of RGO flakes, deposited in between the patterned electrodes with a gap of 2.5 {\\mu}m using a.c. dielectrophoresis show ohmic behavior with a resistance of ~ 37k{\\Omega}. The temperature dependence of the resistance (R) of RGO measured between temperatures 305 K to 393 K yields temperature coefficient of resistance [dR/dT]/R ~ -9.5x10-4 K-1, same as mechanically exfoliated single layer graphene. The field effect transistor action was obtained by electrochemical top-gating using solid polymer electrolyte (PEO + LiClO4) and Pt wire. Ambipolar nature of graphene flakes is observed upto a doping level of ~ 6x1012/cm2 and carrier mobility of ~ 50 cm2V-1sec-1. The source - drain current characteristics shows a tendency of current saturation at high source - drain voltage which is analyzed quantitatively by a diffusive transport model.

We show that single walled carbon nanotubes (SWNT) decorated with sugar functionalized poly (propyl ether imine) (PETIM) dendrimer is a very sensitive platform to quantitatively detect carbohydrate recognizing proteins, namely, lectins. The changes in electrical conductivity of SWNT in field effect transistor device due to carbohydrate - protein interactions form the basis of present study. The mannose sugar attached PETIM dendrimers undergo charge - transfer interactions with the SWNT. The changes in the conductance of the dendritic sugar functionalized SWNT after addition of lectins in varying concentrations were found to follow the Langmuir type isotherm, giving the concanavalin A (Con A) - mannose affinity constant to be 8.5 x 106 M-1. The increase in the device conductance observed after adding 10 nM of Con A is same as after adding 20 \\muM of a non - specific lectin peanut agglutinin, showing the high specificity of the Con A - mannose interactions. The specificity of sugar-lectin interactions was characterized further by observing significant shifts in Raman modes of the SWNT.

Third-order nonlinear absorption and refraction coefficients of a few-layer boron carbon nitride (BCN) and reduced graphene oxide (RGO) suspensions have been measured at 3.2 eV in the femtosecond regime. Optical limiting behavior is exhibited by BCN as compared to saturable absorption in RGO. Nondegenerate time-resolved differential transmissions from BCN and RGO show different relaxation times. These differences in the optical nonlinearity and carrier dynamics are discussed in the light of semiconducting electronic band structure of BCN vis-à-vis the Dirac linear band structure of graphene.