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Volume 16, issue 15 | Copyright
Atmos. Chem. Phys., 16, 10133-10158, 2016
https://doi.org/10.5194/acp-16-10133-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 11 Aug 2016

Research article | 11 Aug 2016

Nine years of global hydrocarbon emissions based on source inversion of OMI formaldehyde observations

Maite Bauwens1, Trissevgeni Stavrakou1, Jean-François Müller1, Isabelle De Smedt1, Michel Van Roozendael1, Guido R. van der Werf2, Christine Wiedinmyer3, Johannes W. Kaiser4, Katerina Sindelarova5,6, and Alex Guenther7 Maite Bauwens et al.
  • 1Royal Belgian Institute for Space Aeronomy, Avenue Circulaire 3, 1180 Brussels, Belgium
  • 2Vrije Universiteit Amsterdam, Faculty of Earth and Life Sciences, Amsterdam, the Netherlands
  • 3National Centre for Atmospheric Research, Boulder, CO, USA
  • 4Max Planck Institute for Chemistry, Mainz, Germany
  • 5UPMC Univ. Paris 06, Université Versailles St-Quentin, CNRS/INSU, LATMOS-IPSL, Paris, France
  • 6Charles University in Prague, Department of Atmospheric Physics, Prague, Czech Republic
  • 7University of California, Irvine, USA

Abstract. As formaldehyde (HCHO) is a high-yield product in the oxidation of most volatile organic compounds (VOCs) emitted by fires, vegetation, and anthropogenic activities, satellite observations of HCHO are well-suited to inform us on the spatial and temporal variability of the underlying VOC sources. The long record of space-based HCHO column observations from the Ozone Monitoring Instrument (OMI) is used to infer emission flux estimates from pyrogenic and biogenic volatile organic compounds (VOCs) on the global scale over 2005–2013. This is realized through the method of source inverse modeling, which consists in the optimization of emissions in a chemistry-transport model (CTM) in order to minimize the discrepancy between the observed and modeled HCHO columns. The top–down fluxes are derived in the global CTM IMAGESv2 by an iterative minimization algorithm based on the full adjoint of IMAGESv2, starting from a priori emission estimates provided by the newly released GFED4s (Global Fire Emission Database, version 4s) inventory for fires, and by the MEGAN-MOHYCAN inventory for isoprene emissions. The top–down fluxes are compared to two independent inventories for fire (GFAS and FINNv1.5) and isoprene emissions (MEGAN-MACC and GUESS-ES).

The inversion indicates a moderate decrease (ca. 20%) in the average annual global fire and isoprene emissions, from 2028Tg C in the a priori to 1653Tg C for burned biomass, and from 343 to 272Tg for isoprene fluxes. Those estimates are acknowledged to depend on the accuracy of formaldehyde data, as well as on the assumed fire emission factors and the oxidation mechanisms leading to HCHO production. Strongly decreased top–down fire fluxes (30–50%) are inferred in the peak fire season in Africa and during years with strong a priori fluxes associated with forest fires in Amazonia (in 2005, 2007, and 2010), bushfires in Australia (in 2006 and 2011), and peat burning in Indonesia (in 2006 and 2009), whereas generally increased fluxes are suggested in Indochina and during the 2007 fires in southern Europe. Moreover, changes in fire seasonal patterns are suggested; e.g., the seasonal amplitude is reduced over southeast Asia. In Africa, the inversion indicates increased fluxes due to agricultural fires and decreased maxima when natural fires are dominant. The top–down fire emissions are much better correlated with MODIS fire counts than the a priori inventory in regions with small and agricultural fires, indicating that the OMI-based inversion is well-suited to assess the associated emissions.

Regarding biogenic sources, significant reductions in isoprene fluxes are inferred in tropical ecosystems (30–40%), suggesting overestimated basal emission rates in those areas in the bottom–up inventory, whereas strongly positive isoprene emission updates are derived over semiarid and desert areas, especially in southern Africa and Australia. This finding suggests that the parameterization of the soil moisture stress used in MEGAN greatly exaggerates the flux reduction due to drought in those regions. The isoprene emission trends over 2005–2013 are often enhanced after optimization, with positive top–down trends in Siberia (4.2%year−1) and eastern Europe (3.9%year−1), likely reflecting forest expansion and warming temperatures, and negative trends in Amazonia (−2.1%year−1), south China (−1%year−1), the United States (−3.7%year−1), and western Europe (−3.3%year−1), which are generally corroborated by independent studies, yet their interpretation warrants further investigation.

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Relying on a 9-year record of satellite observations of formaldehyde, we use inverse techniques to derive global top–down hydrocarbon fluxes over 2005–2013, infer seasonal and interannual variability, and detect emission trends. Our results suggest changes in fire seasonal patterns, a stronger contribution of agricultural burning, overestimated isoprene flux rates in the tropics, overly decreased isoprene emissions due to soil moisture stress in arid areas, and enhanced isoprene trends.
Relying on a 9-year record of satellite observations of formaldehyde, we use inverse techniques...
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