Airborne observations of the tropospheric CO2 distribution and its controlling factors over the South Pacific Basin

Highly precise measurements of CO2 mixing ratios were recorded aboard both the NASA DC-8 and P3-B aircraft during the Pacific Exploratory Mission-Tropics conducted in August-October 1996. Data were obtained at altitudes ranging from 0.1 to 12 km over a large portion of the South Pacific Basin representing the most geographically extensive CO2 data set recorded in this region. These data along with CO2 surface measurements from the National Oceanic and Atmospheric Administration/Climate Monitoring and Diagnostics Laboratory (NOAA/CMDL) and the National Institute of Water and Atmospheric Research (NIWA) were examined to establish vertical and meridional gradients. The CO2 spatial distribution in the southern hemisphere appeared to be largely determined by interhemispheric transport as air masses with depleted CO2 levels characteristic of northern hemispheric air were frequently observed south of the Intertropical Convergence Zone. However, regional processes also played a role in modulating background concentrations. Comparisons of CO2 with other trace gases indicated that CO2 values were influenced by continental sources. Large scale plumes from biomass burning activities produced enhanced CO2 mixing ratios within the lower to midtroposphere over portions of the remote Pacific. An apparent CO2 source was observed in the NOAA/ CMDL surface data between 15° N and 15° S and in the lower altitude flight data between 8° N and 8.5° S with a zone of intensity from 6.5° N to 1° S. Inferred from these data is the presence of a Southern Ocean sink from south of 15° S having two distinct zones seasonally out of phase with one another. Copyright 1999 by the American Geophysical Union

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

Chemical transport across the ITCZ in the central Pacific during an El Niño-Southern Oscillation cold phase event in March-April 1999

We examine interhemispheric transport processes that occurred over the central Pacific during the PEM-Tropics B mission (PTB) in March-April 1999 by correlating the observed distribution of chemical tracers with the prevailing and anomalous windfields. The Intertropical Convergence Zone (ITCZ) had a double structure during PTB, and interhemispheric mixing occurred in the equatorial region between ITCZ branches. The anomalously strong tropical easterly surface wind had a large northerly component across the equator in the central Pacific, causing transport of aged, polluted air into the Southern Hemisphere (SH) at altitudes below 4 km. Elevated concentrations of chemical tracers from the Northern Hemisphere (NH) measured south of the equator in the central Pacific during PTB may represent an upper limit because the coincidence of seasonal and cold phase ENSO conditions are optimum for this transport. Stronger and more consistent surface convergence between the northeasterly and southeasterly trade winds in the Southern Hemisphere (SH) resulted in more total convective activity in the SH branch of the ITCZ, at about 6° S. The middle troposphere between 4-7 km was a complex shear zone between prevailing northeasterly winds at low altitudes and southwesterly winds at higher altitudes. Persistent anomalous streamline patterns and the chemical tracer distribution show that during PTB most transport in the central Pacific was from SH to NH across the equator in the upper troposphere. Seasonal differences in source strength caused larger interhemispheric gradients of chemical tracers during PTB than during the complementary PEM-Tropics A mission in September-October 1996. Copyright 2001 by the American Geophysical Union

Nonmethane hydrocarbon measurements in the North Atlantic Flight Corridor during the Subsonic Assessment Ozone and Nitrogen Oxide Experiment

Mixing ratios of nonmethane hydrocarbons (NMHCs) were not enhanced in whole air samples collected within the North Atlantic Flight Corridor (NAFC) during the fall of 1997. The investigation was conducted aboard NASA's DC-8 research aircraft, as part of the Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX). NMHC enhancements were not detected within the general organized tracking system of the NAFC, nor during two tail chases of the DC-8's own exhaust. Because positive evidence of aircraft emissions was demonstrated by enhancements in both nitrogen oxides and condensation nuclei during SONEX, the NMHC results suggest that the commercial air traffic fleet operating in the North Atlantic region does not contribute at all or contributes negligibly to NMHCs in the NAFC. Copyright 2000 by the American Geophysical Union

Aerosols from biomass burning over the tropical South Atlantic region: Distributions and impacts

The NASA Global Tropospheric Experiment (GTE) Transport and Atmospheric Chemistry Near the Equator-Atlantic (TRACE A) expedition was conducted September 21 through October 26, 1992, to investigate factors responsible for creating the seasonal South Atlantic tropospheric ozone maximum. During these flights, fine aerosol (0.1-3.0 μm) number densities were observed to be enhanced roughly tenfold over remote regions of the tropical South Atlantic and greater over adjacent continental areas, relative to northern hemisphere observations and to measurements recorded in the same area during Ac wet season. Chemical and meteorological analyses as well as visual observations indicate that the primary source of these enhancements was biomass burning occurring within grassland regions of north central Brazil and southeastern Africa. These fires exhibited fine aerosol (N) emission ratios relative to CO (dN/dCO) of 22.5 ± 9.7 and 23.6 ± 15.1 cm-3 parts per billion by volume (ppbv)-1 over Brazil and Africa, respectively. Convection coupled with counterclockwise flow around the South Atlantic subtropical anticyclone subsequently distributed these aerosols throughout the remote South Atlantic troposphere. We calculate that dilute smoke from biomass burning produced an average tenfold enhancement in optical depth over the continental regions as well as a 50% increase in this parameter over the middle South Atlantic Ocean; these changes correspond to an estimated net cooling of up to 25 W m-2 and 2.4 W m-2 during clear-sky conditions over savannas and ocean respectively. Over the ocean our analyses suggest that modification of CCN concentrations within the persistent eastern Atlantic marine stratocumulus clouds by entrainment of subsiding haze layers could significantly increase cloud albedo resulting in an additional surface radiative cooling potentially greater in magnitude than that caused by direct extinction of solar radiation by the aerosol particles themselves