We demonstrate that water is almost universally present on apparently dry self-assembled monolayers, even on those considered almost hydrophobic by conventional methods such as water contact goniometry. The structure and kinetics of nanoscale water adsorption onto these surfaces were investigated using X-ray and neutron reflectometry, as well as atomic force microscopy. Condensation of water on hydrophilic surfaces under ambient conditions formed a dense sub-nanometre surface layer; the thickness of which increased with exponentially limiting kinetics. Tapping mode AFM measurements show the presence of nanosized droplets that covered a small percentage (∼2%) of the total surface area, and which became fewer in number and larger in size with time. While low vacuum pressures (∼10-8 bar) at room temperature did nothing to remove the adsorbed water from these monolayers, heating to temperatures above 65 °C under atmospheric conditions did lead to evaporation from the surface. We demonstrate that water contact angle measurements are not necessarily sensitive to the presence of nanoscale adsorbed water and do not vary with time. For the most part they are a poor indicator of the kinetics and the amount of water condensation onto these surfaces at the molecular level. In summary, this study reveals the need to exclude air containing even trace amounts of water vapor from such surfaces when characterizing using techniques such as X-ray reflectometry. 2011 The Royal Society of Chemistry. We demonstrate that water is almost universally present on apparently dry self-assembled monolayers, even on those considered almost hydrophobic by conventional methods such as water contact goniometry. The structure and kinetics of nanoscale water adsorption onto these surfaces were investigated using X-ray and neutron reflectometry, as well as atomic force microscopy. Condensation of water on hydrophilic surfaces under ambient conditions formed a dense sub-nanometre surface layer; the thickness of which increased with exponentially limiting kinetics. Tapping mode AFM measurements show the presence of nanosized droplets that covered a small percentage ($2%) of the total surface area, and which became fewer in number and larger in size with time. While low vacuum pressures ($10 À8 bar) at room temperature did nothing to remove the adsorbed water from these monolayers, heating to temperatures above 65 C under atmospheric conditions did lead to evaporation from the surface.We demonstrate that water contact angle measurements are not necessarily sensitive to the presence of nanoscale adsorbed water and do not vary with time. For the most part they are a poor indicator of the kinetics and the amount of water condensation onto these surfaces at the molecular level. In summary, this study reveals the need to exclude air containing even trace amounts of water vapor from such surfaces when characterizing using techniques such as X-ray reflectometry.
The zirconates Ln(2)Zr(2)O(7) (Ln = lanthanoid) have been studied using a combination of Zr L-edge X-ray absorption near edge structure (XANES) and synchrotron X-ray and neutron powder diffraction methods. These studies demonstrate that as the size of the lanthanoid cation decreases, the local structure evolves smoothly from the ideal pyrochlore toward the defect fluorite rather than undergoing an abrupt transformation. The Zr L-edge spectrum is found to be extremely sensitive to changes in the local coordination environment and demonstrates an increase in local disorder across the pyrochlore oxides. The sensitivity of the XANES measurements enables us to identify the progressive nature of the transition that could not be detected using bulk diffraction techniques.
Sets of lattice parameter data have been obtained from high resolution neutron and synchrotron x-ray powder diffraction patterns collected in situ as a function of temperature for perovskites in the (Ca,Sr)TiO3 solid solution. An updated phase diagram is proposed in which there is a stability field for the I4/mcm structure at all compositions across the solid solution. The transition is close to tricritical in the composition range 0–70% SrTiO3 component and then evolves towards second order character (Landau 246 solution) in the range 85–100% SrTiO3. Transition temperatures as a function of composition for and transitions at lower temperatures show a break in slope at ∼60% SrTiO3. Variations of octahedral tilt angles and spontaneous strains are much the same for Pbcm structures as they are for Pnma structures. Nearly cubic lattice geometry of orthorhombic structures at intermediate compositions is ascribed to only weak coupling between octahedral tilting and the shear strain e4. The phase diagram topology and variations in structural evolution at different compositions indicate that there is a distinct change in the behaviour of the solid solution at ∼85% SrTiO3.
Heretofore, global burned area (BA) products are only available at coarse spatial resolution, since most of the current global BA products are produced with the help of active fire detection or dense time-series change analysis, which requires very high temporal resolution. In this study, however, we focus on automated global burned area mapping approach based on Landsat images. By utilizing the huge catalog of satellite imagery as well as the high-performance computing capacity of Google Earth Engine, we proposed an automated pipeline for generating 30-meter resolution global-scale annual burned area map from time-series of Landsat images, and a novel 30-meter resolution global annual burned area map of 2015 (GABAM 2015) is released.GABAM 2015 consists of spatial extent of fires that occurred during 2015 and not of fires that occurred in previous years. Cross-comparison with recent Fire cci version 5.0 BA product found a similar spatial distribution and a strong correlation (R 2 = 0.74) between the burned areas from the two products, although differences were found in specific land cover categories (particularly in agriculture land). Preliminary global validation showed the commission and omission error of GABAM 2015 are 13.17% and 30.13%, respectively.
We have studied the long-range average and local structures in Y 2 Sn 2−x Zr x O 7 (x = 0−2.0) using synchrotron X-ray powder diffraction and X-ray absorption spectroscopy, respectively, and by theoretical methods. While the diffraction data indicate a clear phase transition from ordered pyrochlore to disordered defectfluorite at x ∼ 1.0−1.2, X-ray absorption near-edge structure (XANES) results at the Zr L 3 -and Y L 2 -edges reveal a gradual structural evolution across the whole compositional range. These findings provide experimental evidence that the local disorder occurs long before the pyrochlore to defect-fluorite phase boundary, as determined by X-ray diffraction, and the extent of disorder continues to develop throughout the defectfluorite region. The Zr and Y L-edge spectra are very sensitive to changes in the local structure; such sensitivity enables us to reveal the progressive nature of the phase transition. Experimental results are supported by ab initio atomic scale simulations, which provide a mechanism for disorder to initiate in the pyrochlore structure. Further, the coordination numbers of the cations in both the defect-fluorite and pyrochlore structures are predicted, and the trends agree well with the experimental XANES results. The calculations predict that the coordination of cations in the Y 2 Zr 2 O 7 defect-fluorite (normally considered to be 7 for all cations) varies depending on the species with the average coordination of Y and Zr being 7.2 and 6.8, respectively.
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