Measurements of Atmospheric OH and HO2 Radicals by Laser-Induced Fluorescence on the HALO Aircraft during the OMO-ASIA 2015 Campaign
In: Schriften des Forschungszentrums Jülich . Energie & Umwelt 495
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In: Schriften des Forschungszentrums Jülich . Energie & Umwelt 495
The coronavirus-19 (COVID-19) pandemic led to government interventions to limit the spread of the disease which are unprecedented in recent history; for example, stay at home orders led to sudden decreases in atmospheric emissions from the transportation sector. In this review article, the current understanding of the influence of emission reductions on atmospheric pollutant concentrations and air quality is summarized for nitrogen dioxide (NO2), particulate matter (PM2.5), ozone (O3), ammonia, sulfur dioxide, black carbon, volatile organic compounds, and carbon monoxide (CO). In the first 7 months following the onset of the pandemic, more than 200 papers were accepted by peer-reviewed journals utilizing observations from ground-based and satellite instruments. Only about one-third of this literature incorporates a specific method for meteorological correction or normalization for comparing data from the lockdown period with prior reference observations despite the importance of doing so on the interpretation of results. We use the government stringency index (SI) as an indicator for the severity of lockdown measures and show how key air pollutants change as the SI increases. The observed decrease of NO2 with increasing SI is in general agreement with emission inventories that account for the lockdown. Other compounds such as O3, PM2.5, and CO are also broadly covered. Due to the importance of atmospheric chemistry on O3 and PM2.5 concentrations, their responses may not be linear with respect to primary pollutants. At most sites, we found O3 increased, whereas PM2.5 decreased slightly, with increasing SI. Changes of other compounds are found to be understudied. We highlight future research needs for utilizing the emerging data sets as a preview of a future state of the atmosphere in a world with targeted permanent reductions of emissions. Finally, we emphasize the need to account for the effects of meteorology, emission trends, and atmospheric chemistry when determining the lockdown effects on pollutant ...
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Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks. ; Research at the University of Cambridge was supported by a Marie Curie Intra-European fellowship (project no. 254319) and the ERC grant no. 279405. We thank the SAPHIR and TNA2012 team in Jülich for supporting our measurements and the support by EUROCHAMP2 contract no. 228335. The field-work was funded by ERC grant 227463 and the Academy of Finland Centre of Excellence (grants 1118615 and 272041) and by the Office of Science (BER), US Department of Energy via Biogenic Aerosols - Effects on Clouds and Climate (BAECC). European Union's Horizon 2020 research and innovation programme under grant agreement no. 654109 and previously from the European Union Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 262254. We thank the Met Office for use of the NAME model. S.C. thanks the UK Natural Environment Research Council for her studentship.
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Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62°N and 10° W – 26°E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36–64%) of NR-PM1 followed by sulfate (12–44%) and nitrate (6–35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in mid-latitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (μg/m³) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 μg/m³ at half of the sites. ; This study was partially supported by the European Union's projects ACTRIS (EU FP7-262254) and ACTRIS-2 (EU Horizon 2020–654109). COST Action CA16109 COLOSSAL, Chemical On-Line cOmpoSition and Source Apportionment of fine aerosoL, is acknowledged. The ACSM observations at Birkenes was funded by the Norwegian Ministry of Climate and Environment Strategic Institute Program. IDAEA-CSIC (3 datasets: BCN, MSA, MSY) was partially supported by the Spanish Ministry of Economy and Competitiveness and FEDER funds under the PRISMA project (CGL 2012-39623-C02-1). The London measurements were supported by the UK National Research Council through the ClearfLo project and a PhD studentship (grant refs. NE/H008136/1 and NE/I528142/1) and the Department of Environment, Food and Rural Affairs (DEFRA). ECPL personel, namely Nikolaos Mihalopoulos, Aikaterini Bougiatioti and Iasonas Stavroulas acknowledge support by the project "Panhellenic infrastructure for atmospheric composition and climate change, PANACEA" (MIS 5021516) which is implemented under the Action "Reinforcement of the Research and Innovation Infrastructure", funded by the Operational Programme" Competitiveness, Entrepreneurship and Innovation" (NSRF 2014–2020) and co-financed by Greece and the European Union (European Regional Development Fund). IMT Lille Douai acknowledges financial support from the CaPPA (Chemical and Physical Properties of the Atmosphere) project funded by the French National Research Agency (ANR) through the PIA (Programme d'Investissement d'Avenir) under contract ANR-11-LABX-0005-01, and two CPER projects funded by the French Ministry of Higher Education and Research, the CNRS, the Regional Council "Hauts-de-France" and the European Regional Development Fund (ERDF): Climibio, and IRENI (additionally financed by the Communauté Urbaine de Dunkerque). S. Zhang thanks IMT Lille Douai and the Regional Council "Hauts-de-France" for her PhD grant. Prague co-authors would like to acknowledge a Czech MEYS's project under INTER-EXCELENCE INTERCOST program under grant agreement LTC18068 and from European Regional Development Fund-Project under the grant ACTRIS-CZ RI (CZ.02.1.01/0.0/0.0/16_013/0001315). EPA Ireland, Department of Communications, Climate Action and Environment (DCCAE) and the European Union's Seventh Framework Programme (FP7/2007–2013) project BACCHUS under grant agreement n_603445 are acknowledged for research support at Mace Head. The physical measurements were also funded by the German Ultrafine Aerosol Network GUAN, which was jointly established with help of the German Federal Environment Ministry (BMU) grants F&E 370343200 (German title: "Erfassung der Zahl feiner und ultrafeiner Partikel in der Auβenluft"), 2008–2010, and F&E 371143232 (German title: "Trendanalysen gesundheitsgefährdender Fein-und Ultrafeinstaubfraktionen unter Nutzung der im German Ultrafine Aerosol Network (GUAN) ermittelten Immissionsdaten durch Fortführung und Interpretation der Messreihen") 2012–2014. We also acknowledge the WCCAP (World Calibration Center for Aerosol Physics) as part of the WMO-GAW program. The WCCAP is base-funded by the German Federal Environmental Agency (Umweltbundesamt), Germany. Support by the European Regional Development Funds (EFRE – Europe funds Saxony) is gratefully acknowledged. Atmospheric measurements performed in Corsica is part of the ChArMEx project supported by CNRS-INSU, ADEME, Météo-France and CEA in the framework of the multidisciplinary programme MISTRALS (Mediterranean Integrated Studies aT Regional And Local Scales; http://mistrals-home.org/, last access: June 10, 2020). Final data processing of these measurements has been supported by the EMME-CARE (Eastern Mediterranean and Middle East Climate and Atmosphere Research Center) which has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No. 856612 and the Cyprus Government. The measurements in Switzerland were supported by the Federal Office for the Environment. We thank the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG) for the opportunity to perform experiments on the Jungfraujoch. ; Peer reviewed
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