100 research outputs found
Wet chemical deposition of crystalline, redispersable ATO and ITO nanoparticles
A new wet chemical concept to produce coatings by dip, spin or spray processes is presented. It is based on the preparation of solutions made of crystalline nanoparticles fully redispersable in a solvent. It is exemplified for the preparation of SnO2 : Sb (ATO) and In2O3 : Sn (ITO) transparent conducting coatings. The process combines the advantages of using particles having already a low resistivity and the possibility to sinter the coatings at low temperature. The particles are prepared using an in-situ monitoring of the surface energy to control the growth of the particles and to avoid their agglomeration. The dried powders can be fully redispersed in alcohol (ITO) or water (ATO). Single layers with thickness up to 200 nm (ATO) and 400 nm (ITO) have been fabricated. The sheet resistance of the coatings decreases with the sintering temperature. Typical values are 430 Ω(open square) for ATO (550°C) and 380 Ω(open square) for ITO (550°C). Sols made by redispersing the powders in organosilanes allow to produce coatings at low temperature with antistatic (R(open square) > 100 kΩ(open square)) and anti-glare properties (R(open square) > 100 kΩ(open square), 60 to 80 gloss units)
Ultrafiltration conducting membranes and coatings from redispersable, nanoscaled, crystalline SnO2:Sb particles
Inorganic membranes prepared by the sol-gel method are promising candidates for use as filters in separation processes. Conducting supported membranes and coatings have been produced from redispersable nanoscaled crystalline Sb-doped SnO2 powders with Sb contents up to 10 mol%. The crystalline particles (ca. 4 nm) are fully redispersable in aqueous solution at ph ≥ 8 with a solid content up to 37 vol.% and are monosized. After thermal treatment at different temperatures and times, the pore size diameter of such a powder can be adjusted from 4-20 nm with a very narrow pore size distribution (ca. ±1 nm) and a total porosity of 63%, practically independent of the sintering parameters. Uniaxial compacted substrates (unsupported membranes) present similar characteristics but with a larger pore size distribution (± 5 nm) and 80% total porosity. Their electrical resistance decreases with sintering temperature and time to 4 Ω (800 °C, 8 h). Crack free transparent conducting coatings on glasses and ceramics have been obtained by spin-coating using fully dispersed aqueous solutions of the powder with volume content up to 7.8%. After thermal treatment (1 h at 550 °C) single layers 200 nm thick are still porous and exhibit specific electrical resistivity as low as p = 2.5 x 10-2 Ω cm with 90% transmission in the visible range
10K Ring Electrode Trap - Tandem Mass Spectrometer for Infrared Spectroscopy of Mass Selected Ions
A novel instrumental setup for measuring infrared photodissociation spectra of buffer gas cooled, mass-selected ions is described and tested. It combines a cryogenically cooled, linear radio frequency ion trap with a tandem mass spectrometer, optimally coupling continuous ion sources to pulsed laser experiments. The use of six independently adjustable DC potentials superimposed over the trapping radio frequency field provides control over the ion distribution within, as well as the kinetic energy distribution of the ions extracted from the ion trap. The scheme allows focusing the ions in space and time, such that they can be optimally irradiated by a pulsed, widely tunable infrared photodissociation laser. Ion intensities are monitored with a time-of-flight mass spectrometer mounted orthogonally to the ion trap axis
Surface-Enhanced Nitrate Photolysis on Ice
Heterogeneous nitrates photolysis is the trigger for many chemical processes occurring in the polar boundary layer and is widely believed to occur in a quasi-liquid layer (QLL) at the surface of ice. The dipole forbidden character of the electronic transition relevant to boundary layer atmospheric chemistry and the small photolysis/photoproducts quantum yields in ice (and in water) may confer a significant enhancement and interfacial specificity to this important photochemical reaction at the surface of ice. Using amorphous solid water films at cryogenic temperatures as models for the disordered interstitial air/ice interface within the snowpack suppresses the diffusive uptake kinetics thereby prolonging the residence time of nitrate anions at the surface of ice. This approach allows their slow heterogeneous photolysis kinetics to be studied providing the first direct evidence that nitrates adsorbed onto the first molecular layer at the surface of ice are photolyzed more effectively than those dissolved within the bulk. Vibrational spectroscopy allows the ~3-fold enhancement in photolysis rates to be correlated with the nitrates’ distorted intramolecular geometry thereby hinting at the role played by the greater chemical heterogeneity in their solvation environment at the surface of ice than in the bulk. A simple 1D kinetic model suggests 1-that a 3(6)-fold enhancement in photolysis rate for nitrates adsorbed onto the ice surface could increase the photochemical NO[subscript 2] emissions from a 5(8) nm thick photochemically active interfacial layer by 30%(60)%, and 2-that 25%(40%) of the NO[subscript 2] photochemical emissions to the snowpack interstitial air are released from the top-most molecularly thin surface layer on ice. These findings may provide a new paradigm for heterogeneous (photo)chemistry at temperatures below those required for a QLL to form at the ice surface
Wet chemical deposition of crystalline, redispersable ATO and ITO nanoparticles
A new wet chemical concept to produce coatings by dip, spin or spray processes is presented. It is based on the preparation of solutions made of crystalline nanoparticles fully redispersable in a solvent. It is exemplified for the preparation of SnO2 : Sb (ATO) and In2O3 : Sn (ITO) transparent conducting coatings. The process combines the advantages of using particles having already a low resistivity and the possibility to sinter the coatings at low temperature. The particles are prepared using an in-situ monitoring of the surface energy to control the growth of the particles and to avoid their agglomeration. The dried powders can be fully redispersed in alcohol (ITO) or water (ATO). Single layers with thickness up to 200 nm (ATO) and 400 nm (ITO) have been fabricated. The sheet resistance of the coatings decreases with the sintering temperature. Typical values are 430 Ω(open square) for ATO (550°C) and 380 Ω(open square) for ITO (550°C). Sols made by redispersing the powders in organosilanes allow to produce coatings at low temperature with antistatic (R(open square) > 100 kΩ(open square)) and anti-glare properties (R(open square) > 100 kΩ(open square), 60 to 80 gloss units)
Pixels and Predictions: Potential of GPT-4V in Meteorological Imagery Analysis and Forecast Communication
Generative AI, such as OpenAI\u27s GPT-4V large-language model, has rapidly entered mainstream discourse. Novel capabilities in image processing and natural-language communication may augment existing forecasting methods. Large language models further display potential to better communicate weather hazards in a style honed for diverse communities and different languages. This study evaluates GPT-4V\u27s ability to interpret meteorological charts and communicate weather hazards appropriately to the user, despite challenges of hallucinations, where generative AI delivers coherent, confident, but incorrect responses. We assess GPT-4V\u27s competence via its web interface ChatGPT in two tasks: (1) generating a severe-weather outlook from weather-chart analysis and conducting self-evaluation, revealing an outlook that corresponds well with a Storm Prediction Center human-issued forecast; and (2) producing hazard summaries in Spanish and English from weather charts. Responses in Spanish, however, resemble direct (not idiomatic) translations from English to Spanish, yielding poorly translated summaries that lose critical idiomatic precision required for optimal communication. Our findings advocate for cautious integration of tools like GPT-4V in meteorology, underscoring the necessity of human oversight and development of trustworthy, explainable AI.Supplementary material PDF attached. Submitted to Artificial Intelligence for the Earth Systems (American Meteorological Society) on 18 April 202
Characterizing the Intramolecular H-bond and Secondary Structure in Methylated GlyGlyH+ with H2 Predissociation Spectroscopy
Click on the DOI link below to access the article (may not be free).We report vibrational predissociation spectra of the four protonated dipeptides derived from glycine and sarcosine, GlyGlyH(+)center dot(H-2)(1,2), GlySarH(+)center dot(D-2)(2), SarGlyH(+)center dot(H-2)(2), and SarSarH(+)center dot(D-2)(2), generated in a cryogenic ion trap. Sharp bands were recovered by monitoring photoevaporation of the weakly bound H-2 (D-2) molecules in a linear action regime throughout the 700-4200 cm(-1) range using a table-top laser system. The spectral patterns were analyzed in the context of the low energy structures obtained from electronic structure calculations. These results indicate that all four species are protonated on the N-terminus, and feature an intramolecular H-bond involving the amino group. The large blue-shift in the H-bonded N-H fundamental upon incorporation of a methyl group at the N-terminus indicates that this modification significantly lowers the strength of the intramolecular H-bond. Methylation at the amide nitrogen, on the other hand, induces a significant rotation (similar to 110 degrees) about the peptide backbone.Peer reviewe
Six-Coordinate Nitrito and Nitrato Complexes of Manganese Porphyrin
Reaction of small increments of NO2 gas with sublimed amorphous layers of Mn(II)(TPP) (TPP = meso-tetra-phenylporphyrinato dianion) in a vacuum cryostat leads to formation of the 5-coordinate monodentate nitrato complex Mn(III)(TPP)(η(1)-ONO2) (II). This transformation proceeds through the two distinct steps with initial formation of the five coordinate O-nitrito complex Mn(III)(TPP)(η(1)-ONO) (I) as demonstrated by the electronic absorption spectra and by FTIR spectra using differently labeled nitrogen dioxide. A plausible mechanism for the second stage of reaction is offered based on the spectral changes observed upon subsequent interaction of (15)NO2 and NO2 with the layered Mn(TPP). Low-temperature interaction of I and II with the vapors of various ligands L (L = O-, S-, and N-donors) leads to formation of the 6-coordinate O-nitrito Mn(III)(TPP)(L)(η(1)-ONO) and monodentate nitrato Mn(III)(TPP)(L)(η(1)-ONO2) complexes, respectively. Formation of the 6-coordinate O-nitrito complex is accompanied by the shifts of the ν(N═O) band to lower frequency and of the ν(N-O) band to higher frequency. The frequency difference between these bands Δν = ν(N═O) - ν(N-O) is a function of L and is smaller for the stronger bases. Reaction of excess NH3 with I leads to formation of Mn(TPP)(NH3)(η(1)-ONO) and of the cation [Mn(TPP)(NH3)2](+) plus ionic nitrite. The nitrito complexes are relatively unstable, but several of the nitrato species can be observed in the solid state at room temperature. For example, the tetrahydrofuran complex Mn(TPP)(THF)(η(1)-ONO2) is stable in the presence of THF vapors (∼5 mm), but it loses this ligand upon high vacuum pumping at RT. When L = dimethylsulfide (DMS), the nitrato complex is stable only to ∼-30 °C. Reactions of II with the N-donor ligands NH3, pyridine, or 1-methylimidazole are more complex. With these ligands, the nitrato complexes Mn(III)(TPP)(L)(η(1)-ONO2) and the cationic complexes [Mn(TPP)(L)2](+) coexist in the layer at room temperature, the latter formed as a result of NO3(-) displacement when L is in excess
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