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Airborne whole air samples collected over the western Pacific in spring, 2001 showed depletion of tetrachloroethene (C2Cl4) in every upper tropospheric (UT) air parcel that had interacted with large areas of cirrus less than three days upwind. The amount of C2Cl4 depletion showed a negative correlation with time since the interaction, consistent with the C2Cl4-depleted air parcels mixing with the ambient air as they moved downwind of the cirrus. Ethane and C2Cl4 both react relatively quickly with atomic chlorine (Cl) but ethane was not significantly depleted in these same air parcels, indicating that the C2Cl4 depletion cannot be attributed to Cl chemistry alone. Based on the minimum ethane depletion that can be detected by our measurements, a daytime upper limit of roughly 3 × 104 atom Cl cm-3 is indirectly estimated for heterogeneous chlorine activation by cirrus clouds in the UT in tropical- and mid-latitudes during spring. © 2003 by the American Geophysical Union.

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.

NASA's Pacific Exploratory Mission-Tropics (PEM-T) experiment investigated the atmospheric chemistry of a large portion of the tropical and subtropical Pacific Basin during August to October 1996. This paper summarizes meteorological conditions over the PEM-T domain. Mean flow patterns during PEM-T are described. Important circulation systems near the surface include subtropical anticyclones, the South Pacific Convergence Zone (SPCZ), the Intertropical Convergence Zone (ITCZ), and middle latitude transient cyclones. The SPCZ and ITCZ are areas of widespread ascent and deep convection; however, there is relatively little lightning in these oceanic regions. A large area of subsidence is associated with the subtropical anticyclone centered near Easter Island. PEM-T occurred during a period of near normal sea surface temperatures. When compared to an 11 year climatology (1986-1996), relatively minor circulation anomalies are observed during PEM-T. Some of these circulation anomalies are consistent with much stronger anomalies observed during previous La Nina events. In general, however, the 1996 PEM-T period appears to be climatologically representative. Meteorological conditions for specific flights from each major operations area are summarized. The vertical distribution of ozone along selected DC-8 flights is described using the DIAL remote sensing system. These ozone distributions are related to thermodynamic soundings obtained during aircraft maneuvers and to backward trajectories that arrived at locations along the flight tracks. Most locations in the deep tropics are found to have relatively small values of tropospheric ozone. Backward trajectories calculated from global gridded analyses show that much of this air originates from the east and has not passed over land within 10 days. The deep convection associated with the ITCZ and SPCZ also influences the atmospheric chemistry of these regions. Flights over portions of the subtropics and middle latitudes document layers of greatly enhanced tropospheric ozone, sometimes exceeding 80 ppbv. In situ carbon monoxide in these layers often exceeds 90 ppbv. These regions are located near, and especially south of Tahiti, Easter Island, and Fiji. The layers of enhanced ozone usually correspond to layers of dry air, associated with widespread subsiding air. The backward trajectories show that air parcels arriving in these regions originate from the west, passing over Australia and even extending back to southern Africa. These are regions of biomass burning. The in situ chemical measurements support the trajectory-derived origins of these ozone plumes. Thus the enhanced tropospheric ozone over the central Pacific Basin may be due to biomass burning many thousands of kilometers away. Middle-latitude portions of the PEM-T area are influenced by transient cyclones, and the DC-8 traversed tropopause folds during several flights. The flight area just west of Ecuador experiences outflow from South America. Thus the biomass burning that is prevalent over portions of Brazil influences this area. Copyright 1999 by the American Geophysical Union.

Satellite observations of carbon monoxide (CO) from the Measurements of Pollution in the Troposphere (MOPITT) instrument are combined with measurements from the Transport and Chemical Evolution Over the Pacific (TRACE-P) aircraft mission over the northwest Pacific and with a global three-dimensional chemical transport model (GEOS-CHEM) to quantify Asian pollution outflow and its trans-Pacific transport during spring 2001. Global CO column distributions in MOPITT and GEOS-CHEM are highly correlated (R2 = 0.87), with no significant model bias. The largest regional bias is over Southeast Asia, where the model is 18% too high. A 60% decrease of regional biomass burning emissions in the model (to 39 Tg yr−1) would correct the discrepancy; this result is consistent with TRACE-P observations. MOPITT and TRACE-P also give consistent constraints on the Chinese source of CO from fuel combustion (181 Tg CO yr−1). Four major events of trans-Pacific transport of Asian pollution in spring 2001 were seen by MOPITT, in situ platforms, and GEOS-CHEM. One of them was sampled by TRACE-P (26–27 February) as a succession of pollution layers over the northeast Pacific. These layers all originated from one single event of Asian outflow that split into northern and southern plumes over the central Pacific. The northern plume (sampled at 6–8 km off California) had no ozone enhancement. The southern subsiding plume (sampled at 2–4 km west of Hawaii) contained a 8–17 ppbv ozone enhancement, driven by decomposition of peroxyacetylnitrate (PAN) to nitrogen oxides (NOx). This result suggests that PAN decomposition in trans-Pacific pollution plumes subsiding over the United States could lead to significant enhancements of surface ozone., Engineering and Applied Sciences