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Abstract:

After the eruption of volcanoes around the world, monitoring of the dispersion of ash in the atmosphere is an important task for satellite remote sensing since ash represents a threat to air traffic. In this work we present a novel method, tailored for Eyjafjallajökull ash but applicable to other eruptions as well, that uses thermal observations of the SEVIRI imager aboard the geostationary Meteosat Second Generation satellite to detect ash clouds and determine their mass column concentration and top height during the day and night. This approach requires the compilation of an extensive data set of synthetic SEVIRI observations to train an artificial neural network. This is done by means of the RTSIM tool that combines atmospheric, surface and ash properties and runs automatically a large number of radiative transfer calculations for the entire SEVIRI disk. The resulting algorithm is called “VADUGS” (Volcanic Ash Detection Using Geostationary Satellites) and has been evaluated against independent radiative transfer simulations. VADUGS detects ash-contaminated pixels with a probability of detection of 0.84 and a false-alarm rate of 0.05. Ash column concentrations are provided by VADUGS with correlations up to 0.5, a scatter up to 0.6 g m−2 for concentrations smaller than 2.0 g m−2 and small overestimations in the range 5 %–50 % for moderate viewing angles 35–65∘, but up to 300 % for satellite viewing zenith angles close to 90 or 0∘. Ash top heights are mainly underestimated, with the smallest underestimation of −9 % for viewing zenith angles between 40 and 50∘. Absolute errors are smaller than 70 % and with high correlation coefficients of up to 0.7 for ash clouds with high mass column concentrations. A comparison with spaceborne lidar observations by CALIPSO/CALIOP confirms these results: For six overpasses over the ash cloud from the Puyehue-Cordón Caulle volcano in June 2011, VADUGS shows similar features as the corresponding lidar data, with a correlation coefficient of 0.49 and an overestimation of ash column concentration by 55 %, although still in the range of uncertainty of CALIOP. A comparison with another ash algorithm shows that both retrievals provide plausible detection results, with VADUGS being able to detect ash further away from the Eyjafjallajökull volcano, but sometimes missing the thick ash clouds close to the vent. VADUGS is run operationally at the German Weather Service and this application is also presented.

Abstract:

AbstractThe high‐energy‐density synthesis of NxOy species is simulated in gas mixtures representing an O2‐free early‐Earth atmosphere by terawatt‐kilojoule‐class laser‐induced dielectric breakdown (LIDB). These experiments differ from previous LIDB experiments due to the 100 times greater energy delivered per pulse and sensitive analysis of products by high‐resolution infrared spectroscopy. The measured yields of NO, N2O, and NO2 are 0.08–8 × 1015, 5 × 1012, and 0.03–7 × 1014″��DZ��� J −1. The high N2O yield is above the upper‐limit constraint of previous tabletop LIDB experiments and the expected yield of a thermochemical freeze‐out at any temperature between 2000 and 5000 K, while the NO and NO2 yields are in broad agreement with freeze‐out models. Using a one dimensional chemical model of the Hadean atmosphere and a simple model of late bombardment, we compute the source flux of N2O assuming the same high production yield as measured experimentally and find the steady‐state partial pressure of N2O is insufficient to warm the climate.

Abstract:

Sulfuric acid is shown to form a core–shell particle on a micron-sized, optically-trapped spherical silica bead. The refractive indices of the silica and sulfuric acid, along with the shell thickness and bead radius were determined by reproducing Mie scattered optical white light as a function of wavelength in Mie spectroscopy. Micron-sized silica aerosols (silica beads were used as a proxy for atmospheric silica minerals) were levitated in a mist of sulfuric acid particles; continuous collection of Mie spectra throughout the collision of sulfuric acid aerosols with the optically trapped silica aerosol demonstrated that the resulting aerosol particle had a core–shell morphology. Contrastingly, the collision of aqueous sulfuric acid aerosols with optically trapped polystyrene aerosol resulted in a partially coated system. The light scattering from the optically levitated aerosols was successfully modelled to determine the diameter of the core aerosol (±0.003 μm), the shell thickness (±0.0003 μm) and the refractive index (±0.007). The experiment demonstrated that the presence of a thin film rapidly changed the light scattering of the original aerosol. When a 1.964 μm diameter silica aerosol was covered with a film of sulfuric acid 0.287 μm thick, the wavelength dependent Mie peak positions resembled sulfuric acid. Thus mineral aerosol advected into the stratosphere would likely be coated with sulfuric acid, with a core–shell morphology, and its light scattering properties would be effectively indistinguishable from a homogenous sulfuric acid aerosol if the film thickness was greater than a few 100 s of nm for UV-visible wavelengths.

Abstract:

Aerosol–cloud interactions (ACIs) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The nonlinearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well-defined sources provide “opportunistic experiments” (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatiotemporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors. We review the different experimental conditions and conduct a synthesis of the available satellite datasets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.