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Methane (CH4) Mixing ratios in the northern Pacific Basin were sampled from two aircraft during the TRACE-P mission (Transport and Chemical Evolution over the Pacific) from late February through early April 2001 using a tunable diode laser system. Described in the more detail by Jacob et al. [2003], the mission was designed to characterize Asian outflow to the Pacific, determine its chemical evolution, and assess changes to the atmosphere resulting from the rapid industrialization and increased energy usage on the Asian continent. The high-resolution, high-precision data set of roughly 13,800 CH4 measurements ranged between 1602 ppbv in stratospherically influenced air and 2149 ppbv in highly polluted air. Overall, CH4 mixing ratios were highly correlated with a variety of other trace gases characteristic of a mix of anthropogenic industrial and combustion sources and were strikingly correlated with ethane (C2H6) in particular. Averages with latitude in the near-surface (0-2 km) show that CH4 was elevated well above background levels north of 15°N close to the Asian continent. In the central and eastern Pacific, levels of CH4 were lower as continental inputs were mixed horizontally and vertically during transport. Overall, the correlation between CH4 and other hydrocarbons such as ethane (C2H6), ethyne (C2H2), and propane (C3H8) as well as the urban/industrial tracer perchloroethene (C2Cl4), suggests that for CH4 colocated sources such as landfills, wastewater treatment, and fossil fuel use associated with urban areas dominate regional inputs at this time. Comparisons between measurements made during TRACE-P and those of PEM-West B, flown during roughly the same time of year and under similar meteorological setting 7 years earlier, suggests that although the TRACE-P CH4 observations are higher, the changes are not significantly greater than the increases seen in backgroound air over this time interval.

We use an inverse model analysis to compare the top-down constraints on Asian sources of carbon monoxide (CO) in spring 2001 from (1) daily MOPITT satellite observations of CO columns over Asia and the neighboring oceans and (2) aircraft observations of CO concentrations in Asian outflow from the TRACE-P aircraft mission over the northwest Pacific. The inversion uses the maximum a posteriori method (MAP) and the GEOS-CHEM chemical transport model (CTM) as the forward model. Detailed error characterization is presented, including spatial correlation of the model transport error. Nighttime MOPITT observations appear to be biased and are excluded from the inverse analysis. We find that MOPITT and TRACE-P observations are independently consistent in the constraints that they provide on Asian CO sources, with the exception of southeast Asia for which the MOPITT observations support a more modest decrease in emissions than suggested by the aircraft observations. Our analysis indicates that the observations do not allow us to differentiate source types (i.e., anthropogenic versus biomass burning) within a region. MOPITT provides ten pieces of information to constrain the geographical distribution of CO sources, while TRACE-P provides only four. The greater information from MOPITT reflects its ability to observe all outflow and source regions. We conducted a number of sensitivity studies for the inverse model analysis using the MOPITT data. Temporal averaging of the MOPITT data (weekly and beyond) degrades the ability to constrain regional sources. Merging source regions beyond what is appropriate after careful selection of the state vector leads to significant aggregation errors. Calculations for an ensemble of realistic assumptions lead to a range of inverse model solutions that has greater uncertainty than the a posteriori errors for the MAP solution. Our best estimate of total Asian CO sources is 361 Tg yr−1, over half of which is attributed to east Asia., Engineering and Applied Sciences

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

The Montreal Protocol restricts production of ozone-depleting halocarbons worldwide. Enforcement of the protocol has relied mainly on annual government statistics of production and consumption of these compounds (bottom-up approach). We show here that aircraft observations of halocarbon:CO enhancement ratios on regional to continental scales can be used to infer halocarbon emissions, providing independent verification of the bottom-up approach. We apply this top-down approach to aircraft observations of Asian outflow from the TRACE-P mission over the western Pacific (March–April 2001) and derive emissions from eastern Asia (China, Japan, and Korea). We derive an eastern Asian carbon tetrachloride (CCl4) source of 21.5 Gg yr−1, several-fold larger than previous estimates and amounting to ≃30% of the global budget for this gas. Our emission estimate for CFC-11 from eastern Asia is 50% higher than inventories derived from manufacturing records. Our emission estimates for methyl chloroform (CH3CCl3) and CFC-12 are in agreement with existing inventories. For halon 1211 we find only a strong local source originating from the Shanghai area. Our emission estimates for the above gases result in a ≃40% increase in the ozone depletion potential (ODP) of Asian emissions relative to previous estimates, corresponding to a ≃10% global increase in ODP., Engineering and Applied Sciences