Influence of regional-scale anthropogenic emissions on CO2 distributions over the western North Pacific

We report here airborne measurements of atmospheric CO2 over the western North Pacific during the March-April 2001 Transport and Chemical Evolution over the Pacific (TRACE-P) mission. The CO2 spatial distributions were notably influenced by cyclogenesis-triggered transport of regionally polluted continental air masses. Examination of the CO2 to C2H2/CO ratio indicated rapid outflow of combustion-related emissions in the free troposphere below 8 km. Although the highest CO2 mixing ratios were measured within the Pacific Rim region, enhancements were also observed further east over the open ocean at locations far removed from surface sources. Near the Asian continent, discrete plumes encountered within the planetary boundary layer contained up to 393 ppmv of CO2. Coincident enhancements in the mixing ratios of C2Cl4, C2H2, and C2H4 measured concurrently revealed combustion and industrial sources. To elucidate the source distributions of CO2, an emissions database for Asia was examined in conjunction with the chemistry and 5-day backward trajectories that revealed the WNW/W sector of northeast Asia was a major contributor to these pollution events. Comparisons of NOAA/CMDL and JMA surface data with measurements obtained aloft showed a strong latitudinal gradient that peaked between 35° and 40°N. We estimated a net CO2 flux from the Asian continent of approximately 13.93 Tg C day-1 for late winter/early spring with the majority of the export (79%) occurring in the lower free troposphere (2-8 km). The apportionment of the flux between anthropogenic and biospheric sources was estimated at 6.37 Tg C day-1 and 7.56 Tg C day-1, respectively.