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Long-range transport of Asian emissions to the West Pacific tropical tropopause layer

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Abstract

Rapid transport by deep convection is an important mechanism for delivering surface emissions of reactive halocarbons and other trace species to the tropical tropopause layer (TTL), a key region of transport to the stratosphere. Recent model studies have indicated that increased delivery of short-lived halocarbons to the TTL could delay stratospheric ozone recovery. We report here measurements in the TTL over the western Pacific Ocean of short-lived halocarbons and other trace gases that were transported eastward after convective lofting over Asia. Back-trajectories indicate the sampled air primarily originated from the Indian subcontinent. While short-lived organic bromine species show no measurable change over background mixing ratios, short-lived chlorinated organic species were elevated above background mixing ratios (dichloromethane (Δ48.2 ppt), 1,2-dichloroethane (Δ4.21 ppt), and chloroform (Δ4.85 ppt)), as well as longer-lived halogenated species, methyl chloride (Δ82.0 ppt) and methyl bromide (Δ1.91 ppt). This transported air mass thus contributed an excess equivalent effective chlorine burden of 316 ppt, with 119 ppt from short lived chlorinated species, to the TTL. Non-methane hydrocarbons (NMHC) were elevated 60 - 400% above background mixing ratios. The NMHC measurements were used to characterize the potential source regions, which are consistent with the convective influence analysis. The measurements indicate a chemical composition heavily impacted by biofuel/biomass burning and industrial emissions. This work shows that convection can loft Asian emissions, including short-lived chlorocarbons, and transport them to the remote TTL.

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Acknowledgements

We gratefully acknowledge the engineers, technicians, and pilots of National Aeronautics and Space Administration (NASA) Armstrong Flight Research Center, and NASA-ESPO Project Management, and all POSIDON participants. A special thank you to the lead PIs Ru-Shan Gao and Eric Jensen. We thank Richard Lueb and Roger Hendershot for technical support in the field, and Leslie Pope for WAS support. Thanks to Geoff Dutton, Eric Hintsa, and J. David Nance at NOAA/CIRES. This work was supported by NASA Grants NNX13AH20G and NNX17AE43G, and National Science Foundation Grant AGS-1853948. We acknowledge the NOAA Air Resources Laboratory for use of the HYSPLIT model and the NASA EOSDIS for use of the use of imagery from the NASA Worldview application (https://worldview.earthdata.nasa.gov/). POSIDON data is available at https://espoarchive.nasa.gov/archive/browse/posidon.

Funding

NASA Grants NNX13AH20G and NNX17AE43G, and NSF Grant AGS-1853948.

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Author notes

  1. Maria Navarro: deceased.

Authors and Affiliations

  1. Department of Atmospheric Sciences, Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL, USA

    Victoria Treadaway, Elliot Atlas & Maria Navarro

  2. Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA

    Sue Schauffler

  3. NASA Ames Research Center, Moffett Field, CA, USA

    Rei Ueyama & Leonhard Pfister

  4. NOAA Chemical Sciences Laboratory, Boulder, CO, USA

    Troy Thornberry, Andrew Rollins & Karen Rosenlof

  5. NOAA Global Monitoring Laboratory, Boulder, CO, USA

    James Elkins & Fred Moore

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Treadaway, V., Atlas, E., Schauffler, S. et al. Long-range transport of Asian emissions to the West Pacific tropical tropopause layer. J Atmos Chem 79, 81–100 (2022). https://doi.org/10.1007/s10874-022-09430-7

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