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  Diurnal variability, photochemical production and loss processes of hydrogen peroxide in the boundary layer over Europe

Fischer, H., Axinte, R., Bozem, H., Crowley, J. N., Ernest, C. T., Gilge, S., et al. (2018). Diurnal variability, photochemical production and loss processes of hydrogen peroxide in the boundary layer over Europe. Atmospheric Chemistry and Physics Discussions, 18.

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Fischer, Horst1, Author              
Axinte, Raoul1, Author              
Bozem, Heiko1, Author              
Crowley, John N.1, Author              
Ernest, Cheryl T.1, Author              
Gilge, Stefan, Author
Hafermann, Sascha1, Author              
Harder, Hartwig1, Author              
Hens, Korbinian1, Author              
Königstedt, Rainer1, Author              
Kubistin, Dagmar1, Author              
Mallik, Chinmay1, Author              
Martinez-Harder, Monica1, Author              
Novelli, Anna1, Author              
Parchatka, Uwe1, Author              
Plass-Dülmer, Christian, Author
Pozzer, Andrea1, Author              
Regelin, Eric1, Author              
Reiffs, Andreas1, Author              
Schmidt, Torsten1, Author              
Schuladen, Jan1, Author              Lelieveld, Jos1, Author               more..
Affiliations:
1Atmospheric Chemistry, Max Planck Institute for Chemistry, Max Planck Society, ou_1826285              

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 Abstract: Black carbon (BC) emissions from open biomass burning (BB) are known to have a considerable impact on the radiative budget of the atmosphere on global and regional scales but are poorly constrained in models by atmospheric observations, especially in remote regions. Here, we investigate the feasibility of constraining BC emissions from BB with satellite observations of the aerosol absorption optical depth (AAOD) and the aerosol extinction optical depth (AOD) retrieved from OMI (Ozone monitoring instrument) and MODIS (Moderate Resolution Imaging Spectroradiometer) measurements, respectively. We consider the case of Siberian BB BC emissions, which have a strong potential to impact the Arctic climate system. Using aerosol remote sensing data collected at Siberian sites of the Aerosol Robotic Network (AERONET) along with the results of the Fourth Fire Lab at Missoula Experiment (FLAME-4), we establish an empirical parameterization relating the ratio of the elemental carbon (EC) and organic carbon (OC) contents in BB aerosol to the ratio of AAOD and AOD at the wavelengths of the satellite observations. Applying this parameterization to the BC and OC column amounts simulated with the CHIMERE chemistry transport model, we optimize the parameters of the BB emission model based on MODIS measurements of the fire radiative power (FRP) and obtain top-down optimized estimates of the total monthly BB BC amounts emitted from intense Siberian fires that occurred in May–September 2012. The top-down estimates are compared to the corresponding values obtained using the Global Fire Emissions Database (GFED4) and the Fire Emission Inventory–northern Eurasia (FEI-NE). Our simulations using the optimized BB aerosol emissions are verified against AAOD and AOD data that were withheld from the estimation procedure. The simulations are further evaluated against in situ EC and OC measurements at the Zotino Tall Tower Observatory (ZOTTO) and also against aerosol measurement data collected on board of an aircraft in the framework of the Airborne Extensive Regional Observations (YAK-AEROSIB) experiments. We conclude that our BC and OC emission estimates, considered with their confidence intervals, are consistent with the ensemble of the measurement data analyzed in this study. Siberian fires are found to emit 0.41±0.14Tg of BC over the whole period of the five months considered; this estimate is a factor of 2 larger and a factor of 1.5 smaller compared to that the corresponding estimates based on the GFED4 (0.20Tg) and FEI-NE (0.61Tg) data, respectively. Our estimates of monthly BC emissions are also found to be larger than the BC amounts calculated with the GFED4 data and smaller than those calculated with the FEI-NE data for any of the five months. Especially large positive differences of our estimates of monthly BC emissions with respect to the GFED4 data are found in May and September. This finding indicates that the GFED4 database is likely to strongly underestimate BC emissions from agricultural burns and grass fires in Siberia. All these differences have important implications for climate change in the Arctic, as it is found that about a quarter of the huge BB BC mass emitted in Siberia during the fire season of 2012 was transported across the polar circle into the Arctic. Overall, the results of our analysis indicate that a combination of the available satellite observations of AAOD and AOD can provide the necessary constraints on BB BC emissions.

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Language(s): eng - English
 Dates: 2018
 Publication Status: Published in print
 Pages: 29
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.5194/acp-2018-1179
 Degree: -

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Title: Atmospheric Chemistry and Physics Discussions
  Abbreviation : Atmos. Chem. Phys. Discuss.
Source Genre: Journal
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Publ. Info: Katlenburg-Lindau, Germany : European Geophysical Society, Copernicus Publ.
Pages: 29 Volume / Issue: 18 Sequence Number: - Start / End Page: - Identifier: ISSN: 1680-7367
CoNE: https://pure.mpg.de/cone/journals/resource/111076360006006