M. Begoin

Bio: M. Begoin is an academic researcher from University of Bremen. The author has contributed to research in topics: Sea ice & Ozone depletion. The author has an hindex of 5, co-authored 8 publications receiving 414 citations.

Global observations of tropospheric BrO columns using GOME-2 satellite data

Abstract: . Measurements from the GOME-2 satellite instrument have been analyzed for tropospheric BrO using a residual technique that combines measured BrO columns and estimates of the stratospheric BrO content from a climatological approach driven by O3 and NO2 observations. Comparisons between the GOME-2 results and BrO vertical columns derived from correlative ground-based and SCIAMACHY nadir observations, present a good level of consistency. We show that the adopted technique enables separation of stratospheric and tropospheric fractions of the measured total BrO columns and allows quantitative study of the BrO plumes in polar regions. While some satellite observed plumes of enhanced BrO can be explained by stratospheric descending air, we show that most BrO hotspots are of tropospheric origin, although they are often associated to regions with low tropopause heights as well. Elaborating on simulations using the p-TOMCAT tropospheric chemical transport model, this result is found to be consistent with the mechanism of bromine release through sea salt aerosols production during blowing snow events. No definitive conclusion can be drawn however on the importance of blowing snow sources in comparison to other bromine release mechanisms. Outside polar regions, evidence is provided for a global tropospheric BrO background with column of 1–3 × 1013 molec cm−2, consistent with previous estimates.

An improved NO 2 retrieval for the GOME-2 satellite instrument

Abstract: . Satellite observations of nitrogen dioxide (NO2) provide valuable information on both stratospheric and tropospheric composition. Nadir measurements from GOME, SCIAMACHY, OMI, and GOME-2 have been used in many studies on tropospheric NO2 burdens, the importance of different NOx emissions sources and their change over time. The observations made by the three GOME-2 instruments will extend the existing data set by more than a decade, and a high quality of the data as well as their good consistency with existing time series is of particular importance. In this paper, an improved GOME-2 NO2 retrieval is described which reduces the scatter of the individual NO2 columns globally but in particular in the region of the Southern Atlantic Anomaly. This is achieved by using a larger fitting window including more spectral points, and by applying a two step spike removal algorithm in the fit. The new GOME-2 data set is shown to have good consistency with SCIAMACHY NO2 columns. Remaining small differences are shown to be linked to changes in the daily solar irradiance measurements used in both GOME-2 and SCIAMACHY retrievals. In the large retrieval window, a not previously identified spectral signature was found which is linked to deserts and other regions with bare soil. Inclusion of this empirically derived pseudo cross-section significantly improves the retrievals and potentially provides information on surface properties and desert aerosols. Using the new GOME-2 NO2 data set, a long-term average of tropospheric columns was computed and high-pass filtered. The resulting map shows evidence for pollution from several additional shipping lanes, not previously identified in satellite observations. This illustrates the excellent signal to noise ratio achievable with the improved GOME-2 retrievals.

BrO, blizzards, and drivers of polar tropospheric ozone depletion events

Abstract: . The source of bromine that drives polar boundary layer ozone depletion events (ODEs) is still open to some debate. While ODEs are generally noted to form under conditions of a shallow stable boundary layer, observations of depleted air under high wind conditions are taken as being transport-related. Here we report observations from Antarctica in which an unusually large cloud of BrO formed over the Weddell Sea. The enhanced BrO was observed over Halley station in coastal Antarctica, providing an opportunity to probe the conditions within an active "bromine explosion" event. On this occasion, enhanced BrO and depleted boundary layer ozone coincided with high wind speeds and saline blowing snow. We derive a simple model to consider the environmental conditions that favour ODEs and find two maxima, one at low wind/stable boundary layer and one at high wind speeds with blowing snow. Modelling calculations aiming to reproduce the wider regional or global impacts of ODEs, either via radiative effects or as a halogen source, will also need to account for high wind speed mechanisms.

Satellite observations of long range transport of a large BrO plume in the Arctic

Abstract: . Ozone Depletion Events (ODE) during polar springtime are a well known phenomenon in the Arctic and Antarctic boundary layer. They are caused by the catalytic destruction of ozone by halogens producing reactive halogen oxides like bromine monoxide (BrO). The key halogen bromine can be rapidly transferred into the gas phase in an autocatalytic process – the so called "Bromine Explosion". However, the exact mechanism, which leads to an initial bromine release as well as the influence of transport and chemical processes on BrO, is still not clearly understood. In this study, BrO measurements from the satellite instrument GOME-2 are used together with model calculations with the dispersion model FLEXPART to study an arctic BrO event in March 2007, which could be tracked over several days and a large area. Full BrO activation was observed within one day east of Siberia with subsequent transport to Hudson Bay. The event was linked to a cyclone with very high surface wind speeds, which could have been involved in the production and lifting of aerosols or blowing snow. Considering the short life time of BrO, transported aerosols or snow can also provide the surface for BrO recycling within the plume for several days. The evolution of the BrO plume could be reproduced by FLEXPART simulations of a passive tracer indicating that the activated air mass was transported all the way from Siberia to Hudson Bay. To localise the most probable transport height, model runs initialised in different heights have been performed showing similar transport patterns throughout the troposphere but best agreement with the measurements between the surface and 3 km. The influence of changes in tropopause height on measured BrO values has been considered, but cannot completely explain the observed high BrO values. Backward trajectories from the area of BrO initialisation show upward lifting from the surface up to 3 km and no indication for intrusion of stratospheric air. These observations are consistent with a scenario in which bromine in the air mass was activated on the surface within the cyclone, lifted upwards and transported over several thousand kilometres to Hudson Bay.

Simultaneous satellite observations of IO and BrO over Antarctica

Abstract: . This article reports on satellite observations of iodine monoxide (IO) and bromine monoxide (BrO). The region of interest is Antarctica in the time between spring and autumn. Both molecules, IO and BrO, are reactive halogen species and strongly influence tropospheric composition. As a result, a better understanding of their spatial distribution and temporal evolution is necessary to assess accurately their role in tropospheric chemistry. Especially in the case of IO, information on its present magnitude, spatial distribution patterns and source regions is still sparse. The present study is based on six years of SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY) data recorded in nadir viewing geometry. Multi-year averages of monthly mean IO columns are presented and compared to the distributions of BrO. Influences of the IO air mass factor and the IO absorption cross section temperature dependence on the absolute vertical columns are discussed. The long-term observations of IO and BrO columns yield new insight into the temporal and spatial variation of IO above the Antarctic region. The occurrence of IO on Antarctic sea ice in late spring (November) is discovered and presented. In addition, the comparison between IO and BrO distributions show many differences, which argues for different mechanisms and individual nature of the release of the two halogen oxide precursors. The state of the ecosystem, in particular the changing condition of the sea ice in late spring, is used to explain the observations of the IO behaviour over Antarctica and the differences between IO and BrO distributions.

Mercury as a Global Pollutant: Sources, Pathways, and Effects

Abstract: Mercury (Hg) is a global pollutant that affects human and ecosystem health. We synthesize understanding of sources, atmosphere-land-ocean Hg dynamics and health effects, and consider the implications of Hg-control policies. Primary anthropogenic Hg emissions greatly exceed natural geogenic sources, resulting in increases in Hg reservoirs and subsequent secondary Hg emissions that facilitate its global distribution. The ultimate fate of emitted Hg is primarily recalcitrant soil pools and deep ocean waters and sediments. Transfers of Hg emissions to largely unavailable reservoirs occur over the time scale of centuries, and are primarily mediated through atmospheric exchanges of wet/dry deposition and evasion from vegetation, soil organic matter and ocean surfaces. A key link between inorganic Hg inputs and exposure of humans and wildlife is the net production of methylmercury, which occurs mainly in reducing zones in freshwater, terrestrial, and coastal environments, and the subsurface ocean. Elevated human exposure to methylmercury primarily results from consumption of estuarine and marine fish. Developing fetuses are most at risk from this neurotoxin but health effects of highly exposed populations and wildlife are also a concern. Integration of Hg science with national and international policy efforts is needed to target efforts and evaluate efficacy.

Aura OMI observations of regional SO2 and NO2 pollution changes from 2005 to 2015

Abstract: . The Ozone Monitoring Instrument (OMI) onboard NASA's Aura satellite has been providing global observations of the ozone layer and key atmospheric pollutant gases, such as nitrogen dioxide (NO2) and sulfur dioxide (SO2), since October 2004. The data products from the same instrument provide consistent spatial and temporal coverage and permit the study of anthropogenic and natural emissions on local-to-global scales. In this paper, we examine changes in SO2 and NO2 over some of the world's most polluted industrialized regions during the first decade of OMI observations. In terms of regional pollution changes, we see both upward and downward trends, sometimes in opposite directions for NO2 and SO2, for different study areas. The trends are, for the most part, associated with economic and/or technological changes in energy use, as well as regional regulatory policies. Over the eastern US, both NO2 and SO2 levels decreased dramatically from 2005 to 2015, by more than 40 and 80 %, respectively, as a result of both technological improvements and stricter regulations of emissions. OMI confirmed large reductions in SO2 over eastern Europe's largest coal-fired power plants after installation of flue gas desulfurization devices. The North China Plain has the world's most severe SO2 pollution, but a decreasing trend has been observed since 2011, with about a 50 % reduction in 2012–2015, due to an economic slowdown and government efforts to restrain emissions from the power and industrial sectors. In contrast, India's SO2 and NO2 levels from coal power plants and smelters are growing at a fast pace, increasing by more than 100 and 50 %, respectively, from 2005 to 2015. Several SO2 hot spots observed over the Persian Gulf are probably related to oil and gas operations and indicate a possible underestimation of emissions from these sources in bottom-up emission inventories. Overall, OMI observations have proved valuable in documenting rapid changes in air quality over different parts of the world during last decade. The baseline established during the first 11 years of OMI is indispensable for the interpretation of air quality measurements from current and future satellite atmospheric composition missions.

The CAMS reanalysis of atmospheric composition

Abstract: . The Copernicus Atmosphere Monitoring Service (CAMS) reanalysis is the latest global reanalysis dataset of atmospheric composition produced by the European Centre for Medium-Range Weather Forecasts (ECMWF), consisting of three-dimensional time-consistent atmospheric composition fields, including aerosols and chemical species. The dataset currently covers the period 2003–2016 and will be extended in the future by adding 1 year each year. A reanalysis for greenhouse gases is being produced separately. The CAMS reanalysis builds on the experience gained during the production of the earlier Monitoring Atmospheric Composition and Climate (MACC) reanalysis and CAMS interim reanalysis. Satellite retrievals of total column CO; tropospheric column NO2 ; aerosol optical depth (AOD); and total column, partial column and profile ozone retrievals were assimilated for the CAMS reanalysis with ECMWF's Integrated Forecasting System. The new reanalysis has an increased horizontal resolution of about 80 km and provides more chemical species at a better temporal resolution (3-hourly analysis fields, 3-hourly forecast fields and hourly surface forecast fields) than the previously produced CAMS interim reanalysis. The CAMS reanalysis has smaller biases compared with most of the independent ozone, carbon monoxide, nitrogen dioxide and aerosol optical depth observations used for validation in this paper than the previous two reanalyses and is much improved and more consistent in time, especially compared to the MACC reanalysis. The CAMS reanalysis is a dataset that can be used to compute climatologies, study trends, evaluate models, benchmark other reanalyses or serve as boundary conditions for regional models for past periods.

Tropospheric Halogen Chemistry: Sources, Cycling,and Impacts

Abstract: In the past 40 years, atmospheric chemists have come to realize that halogens exert a powerful influence on the chemical composition of the troposphere and through that influence affect the fate of pollutants and may affect climate. Of particular note for climate is that halogen cycles affect methane, ozone, and particles, all of which are powerful climate forcing agents through direct and indirect radiative effects. This influencecomes from the high reactivity of atomic halogen radicals (e.g.,Cl, Br, I) and halogen oxides (e.g., ClO, BrO, IO, and higher oxides), known as reactive halogen species in this review. These reactive halogens are potent oxidizers for organic and inorganic compounds throughout the troposphere.

Reactive halogen chemistry in the troposphere

Abstract: Halogen chemistry is well known for ozone destruction in the stratosphere, however reactive halogens also play an important role in the chemistry of the troposphere. In the last two decades, an increasing number of reactive halogen species have been detected in a wide range of environmental conditions from the polar to the tropical troposphere. Growing observational evidence suggests a regional to global relevance of reactive halogens for the oxidising capacity of the troposphere. This critical review summarises our current understanding and uncertainties of the main halogen photochemistry processes, including the current knowledge of the atmospheric impact of halogen chemistry as well as open questions and future research needs.