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

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

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

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

Patterns of CO2 and radiocarbon across high northern latitudes during International Polar Year 2008

High-resolution in situ CO2 measurements were conducted aboard the NASA DC-8 aircraft during the ARCTAS/POLARCAT field campaign, a component of the wider 2007-2008 International Polar Year activities. Data were recorded during large-scale surveys spanning the North American sub-Arctic to the North Pole from 0.04 to 12 km altitude in spring and summer of 2008. Influences on the observed CO2 concentrations were investigated using coincident CO, black carbon, CH3CN, HCN, O3, C2Cl4, and Δ14CO2 data, and the FLEXPART model. In spring, the CO2 spatial distribution from 55̊N to 90̊N was largely determined by the long-range transport of air masses laden with Asian anthropogenic pollution intermingled with Eurasian fire emissions evidenced by the greater variability in the mid-to-upper troposphere. At the receptor site, the enhancement ratios of CO2 to CO in pollution plumes ranged from 27 to 80 ppmv ppmv-1 with the highest anthropogenic content registered in plumes sampled poleward of 80̊N. In summer, the CO2 signal largely reflected emissions from lightning-ignited wildfires within the boreal forests of northern Saskatchewan juxtaposed with uptake by the terrestrial biosphere. Measurements within fresh fire plumes yielded CO2 to CO emission ratios of 4 to 16 ppmv ppmv-1 and a mean CO2 emission factor of 1698 ± 280 g kg-1 dry matter. From the 14C in CO2 content of 48 whole air samples, mean spring (46.6 ± 4.4%) and summer (51.5 ± 5%) D14CO2 values indicate a 5%seasonal difference. Although the northern midlatitudes were identified as the emissions source regions for the majority of the spring samples, depleted Δ14CO2 values were observed in <1% of the data set. Rather, ARCTAS Δ14CO2 observations (54%) revealed predominately a pattern of positive disequilibrium (1-7%) with respect to background regardless of season owing to both heterotrophic respiration and fire-induced combustion of biomass. Anomalously enriched Δ14CO2 values (101-262%) measured in emissions from Lake Athabasca and Eurasian fires speak to biomass burning as an increasingly important contributor to the mass excess in Δ14CO2 observations in a warming Arctic, representing an additional source of uncertainty in the quantification of fossil fuel CO2

Large-scale latitudinal and vertical distributions of NMHCs and selected halocarbons in the troposphere over the Pacific Ocean during the March-April 1999 Pacific Exploratory Mission (PEM-Tropics B)

Nonmethane hydrocarbons (NMHCs) and selected halocarbons were measured in whole air samples collected over the remote Pacific Ocean during NASA's Global Tropospheric Experiment (GTE) Pacific Exploratory Mission-Tropics B (PEM-Tropics B) in March and early April 1999. The large-scale spatial distributions of NMHCs and C2Cl4 reveal a much more pronounced north-south interhemispheric gradient, with higher concentrations in the north and lower levels in the south, than for the late August to early October 1996 PEM-Tropics A experiment. Strong continental outflow and winter-long accumulation of pollutants led to seasonally high Northern Hemisphere trace gas levels during PEM-Tropics B. Observations of enhanced levels of Halon 1211 (from developing Asian nations such as the PRC) and CH3Cl (from SE Asian biomass burning) support a significant southern Asian influence at altitudes above 1 km and north of 10° N. By contrast, at low altitude over the North Pacific the dominance of urban/industrial tracers, combined with low levels of Halon 1211 and CH3Cl, indicate a greater influence from developed nations such as Japan, Europe, and North America. Penetration of air exhibiting aged northern hemisphere characteristics was frequently observed at low altitudes over the equatorial central and western Pacific south to ∼5° S. The relative lack of southern hemisphere biomass burning sources and the westerly position of the South Pacific convergence zone contributed to significantly lower PEM-Tropics B mixing ratios of the NMHCs and CH3Cl south of 10° S compared to PEM-Tropics A. Therefore the trace gas composition of the South Pacific troposphere was considerably more representative of minimally polluted tropospheric conditions during PEM-Tropics B. Copyright 2001 by the American Geophysical Union

Carbonyl sulfide (OCS): Large-scale distributions over North America during INTEX-NA and relationship to CO2

An extensive set of carbonyl sulfide (OCS) observations were made as part of the NASA Intercontinental Chemical Transport Experiment-North America (INTEX-NA) study, flown from 1 July to 14 August 2004 mostly over the eastern United States and Canada. These data show that summertime OCS mixing ratios at low altitude were dominated by surface drawdown and were highly correlated with CO2. Although local plumes were observed on some low-altitude flight legs, anthropogenic OCS sources were small compared to this sink. These INTEX-NA observations were in marked contrast to the early springtime 2001 Transport and Chemical Evolution over the Pacific experiment, which sampled Asian outflow dominated by anthropogenic OCS emissions. To test the gridded OCS fluxes used in past models, the INTEX-NA observations were combined with the sulfur transport Eulerian model (STEM) regional atmospheric chemistry model for a top-down assessment of bottom-up OCS surface fluxes for North America. Initial STEM results suggest that the modeled fluxes underestimate the OCS plant sink by more than 200%. Copyright 2008 by the American Geophysical Union

Seasonal differences in the photochemistry of the South Pacific: A comparison of observations and model results from PEM-Tropics A and B

A time-dependent photochemical box model is used to examine the photochemistry of the equatorial and southern subtropical Pacific troposphere with aircraft data obtained during two distinct seasons: the Pacific Exploratory Mission-Tropics A (PEM-Tropics A) field campaign in September and October of 1996 and the Pacific Exploratory Mission-Tropics B (PEM-Tropics B) campaign in March and April of 1999. Model-predicted values were compared to observations for selected species (e.g., NO2, OH, HO2) with generally good agreement. Predicted values of HO2 were larger than those observed in the upper troposphere, in contrast to previous studies which show a general underprediction of HO2 at upper altitudes. Some characteristics of the budgets of HOx, NOx, and peroxides are discussed. The integrated net tendency for O3 is negative over the remote Pacific during both seasons, with gross formation equal to no more than half of the gross destruction. This suggests that a continual supply of O3 into the Pacific region throughout the year must exist in order to maintain O3 levels. Integrated net tendencies for equatorial O3 showed a seasonality, with a net loss of 1.06×1011 molecules cm-2 s-1 during PEM-Tropics B (March) increasing by 50% to 1.60×1011 molecules cm-2 s-1 during PEM-Tropics A (September). The seasonality over the southern subtropical Pacific was somewhat lower, with losses of 1.21×1011 molecules cm-2 s-1 during PEM-Tropics B (March) increasing by 25% to 1.51×1011 molecules cm-2 s-1 during PEM-Tropics A (September). While the larger net losses during PEM-Tropics A were primarily driven by higher concentrations of O3, the ability of the subtropical atmosphere to destroy O3 was ∼30% less effective during the PEM-Tropics A (September) campaign due to a drier atmosphere and higher overhead O3 column amounts. Copyright 2001 by the American Geophysical Union