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

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.