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Title: How consistent are top-down hydrocarbon emissions based on formaldehyde observations from GOME-2 and OMI?

Journal Article · · Atmospheric Chemistry and Physics
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [3];  [4];  [5]
  1. Belgium Inst. for Space Aeronomy, Brussels (Belgium)
  2. UPMC Univ., Paris (France)
  3. UPMC Univ., Paris (France); Free University of Brussels (Germany)
  4. Free University of Brussels (Germany)
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

The vertical columns of formaldehyde (HCHO) retrieved from two satellite instruments, the Global Ozone Monitoring Instrument-2 (GOME-2) on Metop-A and the Ozone Monitoring Instrument (OMI) on Aura, are used to constrain global emissions of HCHO precursors from open fires, vegetation and human activities in the year 2010. To this end, the emissions are varied and optimized using the ad-joint model technique in the IMAGESv2 global CTM (chem-ical transport model) on a monthly basis and at the model res-olution. Given the different local overpass times of GOME- 2 (09:30 LT) and OMI (13:30 LT), the simulated diurnal cy-cle of HCHO columns is investigated and evaluated against ground-based optical measurements at seven sites in Europe, China and Africa. The modeled diurnal cycle exhibits large variability, reflecting competition between photochemistry and emission variations, with noon or early afternoon max-ima at remote locations (oceans) and in regions dominated by anthropogenic emissions, late afternoon or evening max-ima over fire scenes, and midday minima in isoprene-rich re-gions. The agreement between simulated and ground-based columns is generally better in summer (with a clear after-noon maximum at mid-latitude sites) than in winter, and the annually averaged ratio of afternoon to morning columns is slightly higher in the model (1.126) than in the ground-based measurements (1.043).The anthropogenic VOC (volatile organic compound) sources are found to be weakly constrained by the inversions on the global scale, mainly owing to their generally minor contribution to the HCHO columns, except over strongly pol-luted regions, like China. The OMI-based inversion yields total flux estimates over China close to the bottom-up inven-tory (24.6 vs. 25.5 TgVOC yr-1 in the a priori) with, how-ever, pronounced increases in the northeast of China and re-ductions in the south. Lower fluxes are estimated based on GOME-2 HCHO columns (20.6 TgVOC yr-1), in particular over the northeast, likely reflecting mismatches between the observed and the modeled diurnal cycle in this region.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1243272
Report Number(s):
PNNL-SA-115411; KP1704020
Journal Information:
Atmospheric Chemistry and Physics, Vol. 15, Issue 20; ISSN 1680-7316
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English

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