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Reduced graphene oxide modified by pulsed laser ablation causes water splitting under visible light illumination (532 nm). When the light source is a pulsed laser, water splitting is accompanied by carbon gasification (CO formation); however, conventional (LED) light sources produce water splitting exclusively.
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The combined effect of nanoscale dielectric and metallic layers prepared by atomic layer deposition (ALD) and chemical vapor deposition (CVD) on the refractometric properties of tilted optical fiber Bragg gratings (TFBG) is studied. A high index intermediate layer made up of either 50 nm or 100 nm layers of Al2O3 (refractive index near 1.62) was deposited by ALD and followed by thin gold layers (30-65 nm) deposited from a known single-source gold (I) iminopyrrolidinate CVD precursor. The fabricated devices were immersed in different surrounding refractive indices (SRI) and the spectral transmission response of the TFBGs was measured. Preliminary results indicate that the addition of the dielectric Al2O3 pre-coating enhances the SRI sensitivity by up to 75% but this enhancement is highly dependent on the polarization and dielectric thickness. In fact, the sensitivity decreases by up to 50% for certain cases. These effects are discussed with support from TFBG simulations and models, by quantifying the penetration of the evanescently coupled light out of the fiber through the various coating layers. Additional characterization studies have been carried out on these samples to further correlate the optical behaviour of the coated TFBGs with the physical properties of the gold and Al2O3 layers, using atomic force microscopy x-ray photoelectron spectroscopy and an ensemble of other optical and x-ray absorption spectroscopy techniques. The purity, roughness, and morphology of gold thin films deposited by CVD onto the dielectric-TFBG surface are also provided.
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A specialized genetic algorithm (GA) is used to search the structural space of samarium-doped ceria (SDC) for the most energetically stable configurations which will predominate in low temperature fuel cells. A systematic investigation of all configurations of 3.2% SDC and a GA investigation of 6.6% SDC are presented for the first time at the DFT+U level of theory. It was found that Sm atoms prefer to occupy the nearest neighbor (NN) position relative to the oxygen vacancy at 3.2%, while at 6.6%, a balance exists between various Sm-vacancy interactions and the vacancies prefer to be separated by â¼6 Å. Also, the migration barriers for oxygen diffusion are calculated amongst the best structures in 3.2% and 6.6% SDC and are found to be comparable to the barriers in Gd-doped ceria at the DFT+U level of theory. While the migration calculations provide insight on the oxygen diffusion mechanism in this material, the favored configurations from our GA enable future research on concentrated SDC and contribute to the atomistic understanding of the influence of dopant-vacancy and vacancy-vacancy interactions on ionic conductivity.
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Classical force field simulations and genetic algorithms are used to navigate low-energy configurations of samarium-doped ceria (SDC) at a number of concentrations, up to 20% SDC, such that the experimentally observed peak in ionic conductivity is mapped out in its entirety and fresh insight into samarium's role is reported.
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Depth resolved X-ray photoelectron spectroscopy (XPS) combined with a 25 µm liquid jet is used to quantify the spatial distribution of 3 nm SnO2 nanoparticles (NPs) from the air-water interface (AWI) into the suspension bulk. Results are consistent with those of a layer several nm thick at the AWI that is completely devoid of NPs.
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The adsorption of AFGP 8 on mica was studied by atomic force microscopy. The results shown in this paper emphasize the strong adsorption affinity of these proteins to hydrophilic surfaces, in this case mica. The dependence of the surface morphology while drying a droplet of protein solution, and the tendency to form 3-D aggregates at high concentration was observed. The behavior indicates that single-molecule-high aggregates (8.1 Å) are formed at low concentration; as the concentration increases, a double layer seems to appear in equilibrium with large aggregates; and as the concentration is increased further, the equilibrium is shifted toward larger aggregates leaving behind residual single-molecule-high aggregates. The hydrophilicity of the protein was demonstrated by the spontaneous adsorption of the protein directly from solution, as monitored by in situ imaging.
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Silicatos de Aluminio/química , Proteínas Anticongelantes/química , Desecación , Humectabilidad , Adsorción , Fraccionamiento Químico , Microscopía de Fuerza Atómica , Soluciones , Solventes/químicaRESUMEN
Surface patterning of antifreeze glycoprotein fraction 8 (AFGP 8) via a solvent evaporation method is reported here. In this process, lines of AFGP 8 particles and gridlike patterns were formed as as result of the receding of the droplet contact line and the accumulation of the solute during evaporation. The solution concentration strongly affects the protein line spacing. The average height of the protein was measured to be 8.1 +/- 2.5 A, which may be attributed to the height of a single molecule.
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Proteínas Anticongelantes/química , Solventes/química , Animales , Regiones Antárticas , Proteínas Anticongelantes/ultraestructura , Regiones Árticas , Peces , Microscopía de Fuerza Atómica , Soluciones/química , Volatilización , Agua/químicaRESUMEN
A sub-monolayer of atomic sodium was deposited on a LiF(001) surface at 40 K. The adsorbed sodium exists at the surface as single atoms and clusters. The surface was dosed with 1 L of HF, to form adsorbed (HF)2...Na(n) (n=1,2,3,...) complexes, which were then irradiated by 640 nm laser light, to induce charge-transfer reaction. The reaction-product atomic H(g) was observed leaving the surface by two-color Rydberg-atom time-of-flight (TOF) spectroscopy. The TOF spectrum of the desorbed H atoms contained two components; a "fast" component with a maximum at approximately 0.85 eV, and a "slow" component with a maximum at 0.45 eV. These two components were attributed to photoreaction on adsorbed single atoms and clusters of sodium, respectively. The fast component exhibited a structure (48+/-17 meV spacing) near the high-energy end of spectrum. This structure was attributed to vibration of NaFHF photoproduct residing on the surface. The cross section of the harpooning event in the Na...(HF)2 adsorbed complex was determined as (9.1+/-2.0)x10(-19) cm(2). To interpret the experimental vibrational structure and the relative energies of the fast and slow components of the TOF spectrum, high-level ab initio calculations were performed for reactants Na(n)...(HF)(m) (n,m=1,2) and reaction products Na(n)F(m)H(m-1). The calculated NaF-HF and Na-Na(HF)(2) bond dissociation energies indicated that photoexcitation of the precursor complexes led not only to ejection of H atoms, but also to dissociation of the Na(n)...(HF)(2) (n=1,2) species through cleavage of the NaF-HF and Na-Na(HF)(2) bonds.
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Alumina-supported vanadium particles were prepared under ultrahigh vacuum (UHV) conditions and characterized with respect to their structural and CO adsorption properties. As supporting oxide, we used a thin, well-ordered alumina film grown on NiAl(110). This allows the application of scanning tunneling microscopy (STM), infrared reflection-absorption spectroscopy (IRAS), and X-ray photoelectron spectroscopy (XPS) without charging effects. Vanadium evaporation under UHV conditions leads to the growth of nanometer-sized particles which strongly interact with the alumina support. At very low vanadium coverages, these particles are partially incorporated into the alumina film and get oxidized through the contact to alumina. Low-temperature CO adsorption in this coverage regime permits the preparation of isolated vanadium carbonyls, of which we have identified mono-, di-, and tricarbonyls of the V(CO)(y)() type. A charge-frequency relationship was set up which allows one to quantify the extent of charge transfer from vanadium to alumina. It turns out that this charge transfer depends on the V nucleation site.