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Iodine is an important nutrient and a significant sink of tropospheric ozone, a climate-forcing gas and air pollutant. Ozone interacts with seawater iodide, leading to volatile inorganic iodine release that likely represents the largest source of atmospheric iodine. Increasing ozone concentrations since the preindustrial period imply that iodine chemistry and its associated ozone destruction is now substantially more active. However, the lack of historical observations of ozone and iodine means that such estimates rely primarily on model calculations. Here we use seasonally resolved records from an Alpine ice core to investigate 20th century changes in atmospheric iodine. After carefully considering possible postdepositional changes in the ice core record, we conclude that iodine deposition over the Alps increased by at least a factor of 3 from 1950 to the 1990s in the summer months, with smaller increases during the winter months. We reproduce these general trends using a chemical transport model and show that they are due to increased oceanic iodine emissions, coupled to a change in iodine speciation over Europe from enhanced nitrogen oxide emissions. The model underestimates the increase in iodine deposition by a factor of 2, however, which may be due to an underestimate in the 20th century ozone increase. Our results suggest that iodine's impact on the Northern Hemisphere atmosphere accelerated over the 20th century and show a coupling between anthropogenic pollution and the availability of iodine as an essential nutrient to the terrestrial biosphere.
Assuntos
Poluentes Atmosféricos/química , Gelo/análise , Iodo/química , Água do Mar/química , Atmosfera , Clima , Europa (Continente) , Ozônio/química , Estações do AnoRESUMO
Marine cloud brightening (MCB) is proposed to offset global warming by emitting sea salt aerosols to the tropical marine boundary layer, which increases aerosol and cloud albedo. Sea salt aerosol is the main source of tropospheric reactive chlorine (Cl y ) and bromine (Br y ). The effects of additional sea salt on atmospheric chemistry have not been explored. We simulate sea salt aerosol injections for MCB under two scenarios (212-569 Tg/a) in the GEOS-Chem global chemical transport model, only considering their impacts as a halogen source. Globally, tropospheric Cl y and Br y increase (20-40%), leading to decreased ozone (-3 to -6%). Consequently, OH decreases (-3 to -5%), which increases the methane lifetime (3-6%). Our results suggest that the chemistry of the additional sea salt leads to minor total radiative forcing compared to that of the sea salt aerosol itself (~2%) but may have potential implications for surface ozone pollution in tropical coastal regions.
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Low cost pollution sensors have been widely publicized, in principle offering increased information on the distribution of air pollution and a democratization of air quality measurements to amateur users. We report a laboratory study of commonly-used electrochemical sensors and quantify a number of cross-interferences with other atmospheric chemicals, some of which become significant at typical suburban air pollution concentrations. We highlight that artefact signals from co-sampled pollutants such as CO2 can be greater than the electrochemical sensor signal generated by the measurand. We subsequently tested in ambient air, over a period of three weeks, twenty identical commercial sensor packages alongside standard measurements and report on the degree of agreement between references and sensors. We then explore potential experimental approaches to improve sensor performance, enhancing outputs from qualitative to quantitative, focusing on low cost VOC photoionization sensors. Careful signal handling, for example, was seen to improve limits of detection by one order of magnitude. The quantity, magnitude and complexity of analytical interferences that must be characterised to convert a signal into a quantitative observation, with known uncertainties, make standard individual parameter regression inappropriate. We show that one potential solution to this problem is the application of supervised machine learning approaches such as boosted regression trees and Gaussian processes emulation.
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Discovering low-dimensional structure in real-world networks requires a suitable null model that defines the absence of meaningful structure. Here we introduce a spectral approach for detecting a network's low-dimensional structure, and the nodes that participate in it, using any null model. We use generative models to estimate the expected eigenvalue distribution under a specified null model, and then detect where the data network's eigenspectra exceed the estimated bounds. On synthetic networks, this spectral estimation approach cleanly detects transitions between random and community structure, recovers the number and membership of communities, and removes noise nodes. On real networks spectral estimation finds either a significant fraction of noise nodes or no departure from a null model, in stark contrast to traditional community detection methods. Across all analyses, we find the choice of null model can strongly alter conclusions about the presence of network structure. Our spectral estimation approach is therefore a promising basis for detecting low-dimensional structure in real-world networks, or lack thereof.
Assuntos
Análise Espectral , Algoritmos , Animais , Encéfalo/metabolismo , Regulação da Expressão Gênica , Camundongos , Modelos TeóricosRESUMO
Iodine is a critical trace element involved in many diverse and important processes in the Earth system. The importance of iodine for human health has been known for over a century, with low iodine in the diet being linked to goitre, cretinism and neonatal death. Research over the last few decades has shown that iodine has significant impacts on tropospheric photochemistry, ultimately impacting climate by reducing the radiative forcing of ozone (O3) and air quality by reducing extreme O3 concentrations in polluted regions. Iodine is naturally present in the ocean, predominantly as aqueous iodide and iodate. The rapid reaction of sea-surface iodide with O3 is believed to be the largest single source of gaseous iodine to the atmosphere. Due to increased anthropogenic O3, this release of iodine is believed to have increased dramatically over the twentieth century, by as much as a factor of 3. Uncertainties in the marine iodine distribution and global cycle are, however, major constraints in the effective prediction of how the emissions of iodine and its biogeochemical cycle may change in the future or have changed in the past. Here, we present a synthesis of recent results by our team and others which bring a fresh perspective to understanding the global iodine biogeochemical cycle. In particular, we suggest that future climate-induced oceanographic changes could result in a significant change in aqueous iodide concentrations in the surface ocean, with implications for atmospheric air quality and climate.
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[This corrects the article DOI: 10.1038/s41558-020-0883-0.].