Abstract. We present an updated mechanism for tropospheric halogen (Cl + Br + I) chemistry in the GEOS-Chem global atmospheric chemical transportmodel and apply it to investigate halogen radical cycling and implications for tropospheric oxidants. Improved representation of HOBr heterogeneouschemistry and its pH dependence in our simulation leads to less efficient recycling and mobilization of bromine radicals and enables the model toinclude mechanistic sea salt aerosol debromination without generating excessive BrO. The resulting global mean tropospheric BrO mixingratio is 0.19 ppt (parts per trillion), lower than previous versions of GEOS-Chem. Model BrO shows variable consistency and biases in comparison tosurface and aircraft observations in marine air, which are often near or below the detection limit. The model underestimates the daytimemeasurements of Cl2 and BrCl from the ATom aircraft campaign over the Pacific and Atlantic, which if correct would imply a very largemissing primary source of chlorine radicals. Model IO is highest in the marine boundary layer and uniform in the free troposphere, with a globalmean tropospheric mixing ratio of 0.08 ppt, and shows consistency with surface and aircraft observations. The modeled global meantropospheric concentration of Cl atoms is 630 cm−3, contributing 0.8 % of the global oxidation of methane, 14 % of ethane,8 % of propane, and 7 % of higher alkanes. Halogen chemistry decreases the global tropospheric burden of ozone by 11 %,NOx by 6 %, and OH by 4 %. Most of the ozone decrease is driven by iodine-catalyzed loss. The resulting GEOS-Chem ozonesimulation is unbiased in the Southern Hemisphere but too low in the Northern Hemisphere.
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Temporary pause in the growth of atmospheric ethane and propane in 2015–2018
Abstract. Atmospheric non-methane hydrocarbons (NMHCs) play an important role in theformation of secondary organic aerosols and ozone. After a multidecadalglobal decline in atmospheric mole fractions of ethane and propane – themost abundant atmospheric NMHCs – previous work has shown a reversal ofthis trend with increasing atmospheric abundances from 2009 to 2015 in theNorthern Hemisphere. These concentration increases were attributed to theunprecedented growth in oil and natural gas (O&NG) production in NorthAmerica. Here, we supplement this trend analysis building on the long-term(2008–2010; 2012–2020) high-resolution (∼3 h) record ofambient air C2–C7 NMHCs from in situ measurements at the GreenlandEnvironmental Observatory at Summit station (GEOSummit, 72.58 ∘ N,38.48 ∘ W; 3210 m above sea level). We confirm previous findingsthat the ethane mole fraction significantly increased by +69.0 [+47.4,+73.2; 95 % confidence interval] ppt yr−1 from January 2010 toDecember 2014. Subsequent measurements, however, reveal a significantdecrease by −58.4 [−64.1, −48.9] ppt yr−1 from January 2015 to December2018. A similar reversal is found for propane. The upturn observed after2019 suggests, however, that the pause in the growth of atmospheric ethaneand propane might only have been temporary. Discrete samples collected atother northern hemispheric baseline sites under the umbrella of the NOAAcooperative global air sampling network show a similar decrease in 2015–2018and suggest a hemispheric pattern. Here, we further discuss the potentialcontribution of biomass burning and O&NG emissions (the main sources ofethane and propane) and conclude that O&NG activities likely played arole in these recent changes. This study highlights the crucial need forbetter constrained emission inventories.
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- Award ID(s):
- 1822406
- PAR ID:
- 10300586
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 21
- Issue:
- 19
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 15153 to 15170
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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