Simulating tropospheric BrO in the Arctic using an artificial neural network

An intriguing natural phenomenon occurs every polar spring, namely the bromine explosion, in which plumes of tropospheric bromine monoxide (BrO) are formed. These plumes are observed in the BrO vertical column densities (VCDs), retrieved from satellite sensors. Tropospheric BrO depletes tropospheric ozone and facilitates the deposition of mercury. Bromine molecules are mainly released from young sea ice, and meteorological parameters determine the formation and evolution of enhanced BrO VCD plumes. Due to the complexity of the physicochemical processes involved in the bromine explosion, the modeling of tropospheric BrO VCDs in chemical transport models is challenging and not yet adequate. The first of its type, this study demonstrates the potential of using an artificial neural network (ANN), which uses meteorological parameters and sea ice age as inputs to simulate and predict tropospheric BrO VCDs in the Arctic. The ANN is trained and validated using a 22-year satellite remote sensing dataset of Arctic tropospheric BrO VCDs. A generally satisfactory spatial agreement between observed and simulated tropospheric BrO VCDs is observed. However, the magnitude of the observed BrO VCD plumes is underestimated. Air temperature and mean sea level pressure are the most important parameters influencing the magnitude of tropospheric BrO VCD simulations. Although the changing spatial distribution of tropospheric BrO VCDs over time is well captured, the trend reported in the observations of tropospheric BrO VCDs is not reproduced by the ANN, suggesting that additional parameters not included in the ANN also influence the formation of tropospheric BrO VCD plumes

Substantial contribution of iodine to Arctic ozone destruction

Unlike bromine, the effect of iodine chemistry on the Arctic surface ozone budget is poorly constrained. We present ship-based measurements of halogen oxides in the high Arctic boundary layer from the sunlit period of March to October 2020 and show that iodine enhances springtime tropospheric ozone depletion. We find that chemical reactions between iodine and ozone are the second highest contributor to ozone loss over the study period, after ozone photolysis-initiated loss and ahead of bromine.Iodine chemistry plays a more important role than bromine chemistry in tropospheric ozone losses in the Arctic, according to ship-based observations of halogen oxides from March to October 2020.Peer reviewe

Overview: On the transport and transformation of pollutants in the outflow of major population centres – observational data from the EMeRGe European intensive operational period in summer 2017

Megacities and other major population centres (MPCs) worldwide are major sources of air pollution, both locally as well as downwind. The overall assessment and prediction of the impact of MPC pollution on tropospheric chemistry are challenging. The present work provides an overview of the highlights of a major new contribution to the understanding of this issue based on the data and analysis of the EMeRGe (Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales) international project. EMeRGe focuses on atmospheric chemistry, dynamics, and transport of local and regional pollution originating in MPCs. Airborne measurements, taking advantage of the long range capabilities of the High Altitude and LOng Range Research Aircraft (HALO, https://www.halo-spp.de, last access: 22 March 2022), are a central part of the project. The synergistic use and consistent interpretation of observational data sets of different spatial and temporal resolution (e.g. from ground-based networks, airborne campaigns, and satellite measurements) supported by modelling within EMeRGe provide unique insight to test the current understanding of MPC pollution outflows. In order to obtain an adequate set of measurements at different spatial scales, two field experiments were positioned in time and space to contrast situations when the photochemical transformation of plumes emerging from MPCs is large. These experiments were conducted in summer 2017 over Europe and in the inter-monsoon period over Asia in spring 2018. The intensive observational periods (IOPs) involved HALO airborne measurements of ozone and its precursors, volatile organic compounds, aerosol particles, and related species as well as coordinated ground-based ancillary observations at different sites. Perfluorocarbon (PFC) tracer releases and model forecasts supported the flight planning, the identification of pollution plumes, and the analysis of chemical transformations during transport. This paper describes the experimental deployment and scientific questions of the IOP in Europe. The MPC targets – London (United Kingdom; UK), the Benelux/Ruhr area (Belgium, the Netherlands, Luxembourg and Germany), Paris (France), Rome and the Po Valley (Italy), and Madrid and Barcelona (Spain) – were investigated during seven HALO research flights with an aircraft base in Germany for a total of 53 flight hours. An in-flight comparison of HALO with the collaborating UK-airborne platform Facility for Airborne Atmospheric Measurements (FAAM) took place to assure accuracy and comparability of the instrumentation on board. Overall, EMeRGe unites measurements of near- and far-field emissions and hence deals with complex air masses of local and distant sources. Regional transport of several European MPC outflows was successfully identified and measured. Chemical processing of the MPC emissions was inferred from airborne observations of primary and secondary pollutants and the ratios between species having different chemical lifetimes. Photochemical processing of aerosol and secondary formation or organic acids was evident during the transport of MPC plumes. Urban plumes mix efficiently with natural sources as mineral dust and with biomass burning emissions from vegetation and forest fires. This confirms the importance of wildland fire emissions in Europe and indicates an important but discontinuous contribution to the European emission budget that might be of relevance in the design of efficient mitigation strategies. The present work provides an overview of the most salient results in the European context, with these being addressed in more detail within additional dedicated EMeRGe studies. The deployment and results obtained in Asia will be the subject of separate publications

Climatologies of Geometric and Tropospheric BrO Vertical Column Densities derived from multiple UV-Vis Satellite Remote Sensors for Polar Spring over the Arctic

This dataset contains long-term averages of geometric and tropospheric BrO Vertical Column Densities (VCDs), derived using the DOAS method (Platt and Stutz, 2008), for polar springs (March, April, May) over the Arctic, retrieved from four UV-VIS satellite sensors: GOME (1996-2003), SCIAMACHY (2002-2012), GOME-2A (2007-2017) and GOME-2B (2013-2017), i.e. 22 years in total. All data is available on a 0.5° x 0.5° degree grid. The underlying retrievals of BrO have been verified for consistency between the sensors. Geometric VCDs are derived from total slant columns of BrO by application of a stratospheric air mass factor. The method by Theys et al. (2011) is applied in order to derive tropospheric VCDs from retrieved total slant columns of BrO and a simple tropospheric AMF assuming a surface reflectance of 0.9 and a BrO surface layer of 400 m thickness. The data is available for every sensor separately. In addition, corresponding merged data have been derived by averaging retrievals for dates for which more than one sensor was in operation. Merged climatological monthly means for the months with sufficient light and hence coverage (March to September) are provided in addition. Finally, geometric and tropospheric annual cycles (on a daily and monthly basis) are provided for each instrument separately. We gratefully acknowledge the funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - Projektnummer 268020496 - TRR 172, within the Transregional Collaborative Research Center "ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)³"