ALBERT

Description: Observed correlations between atmospheric concentrations of CO2 and CO represent potentially powerful information for improving CO2 surface flux estimates through coupled CO2-CO inverse analyses. We explore the value of these correlations in improving estimates of regional CO2 fluxes in east Asia by using aircraft observations of CO2 and CO from the TRACE-P campaign over the NW Pacific in March 2001. Our inverse model uses regional CO2 and CO surface fluxes as the state vector, separating biospheric and combustion contributions to CO2. CO2-CO error correlation coefficients are included in the inversion as off-diagonal entries in the a priori and observation error covariance matrices. We derive error correlations in a priori combustion source estimates of CO2 and CO by propagating error estimates of fuel consumption rates and emission factors. However, we find that these correlations are weak because CO source uncertainties are mostly determined by emission factors. Observed correlations between atmospheric CO2 and CO concentrations imply corresponding error correlations in the chemical transport model used as the forward model for the inversion. These error correlations in excess of 0.7, as derived from the TRACE-P data, enable a coupled CO2-CO inversion to achieve significant improvement over a CO2-only inversion for quantifying regional fluxes of CO2.

Description: The meteorological pathways contributing to Asian pollution outflow over the Pacific are examined with a global three-dimensional model analysis of CO observations from the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission (February-April 2001). The model is used also to place the TRACE-P observations in an interannual (1994-2001) and seasonal context. The major process driving Asian pollution outflow in spring is frontal lifting ahead of southeastward-moving cold fronts (the leading edge of cold surges) and transport in the boundary layer behind the cold fronts. Orographic lifting over central and eastern China combines with the cold fronts to promote the transport of Chinese pollution to the free troposphere. Outflow of seasonal biomass burning in Southeast Asia during spring takes place mostly by deep convection but also by northeastward transport and frontal lifting, mixing with the anthropogenic outflow. Boundary layer outflow over the western Pacific is largely devoid of biomass burning influence. European and African (biomass burning) plumes in Asian outflow during TRACE-P were weak (less than 60 ppbv and 20 ppbv CO, respectively) and were not detectable in the observations because of superposition of the much larger Asian pollution signal. Spring 2001 (La Nina) was characterized by unusually frequent cold surge events in the Asian Pacific rim and strong convection in Southeast Asia, leading to unusually strong boundary layer outflow of anthropogenic emissions and convective outflow of biomass burning emissions in the upper troposphere. The Asian outflow flux of CO to the Pacific is found to vary seasonally by a factor of 3-4 (maximum in March and minimum in summer). The March maximum results from frequent cold surge events and seasonal biomass burning emissions.

Description: 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 ha1ocarbon: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 topdown approach to aircraft observations of Asian outflow &om 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(sup -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 (CH3CC13) 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 approximately equal to 40% increase in the ozone depletion potential (ODP) of Asian emissions relative to previous estimates, corresponding to a approximately equal to 10% global increase in ODP.

Description: The NASA Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission was conducted in February-April 2001 over the NW Pacific (1) to characterize the Asian chemical outflow and relate it quantitatively to its sources and (2) to determine its chemical evolution. It used two aircraft, a DC-8 and a P-3B, operating out of Hong Kong and Yokota Air Force Base (near Tokyo), with secondary sites in Hawaii, Wake Island, Guam, Okinawa, and Midway. The aircraft carried instrumentation for measurements of long-lived greenhouse gases, ozone and its precursors, aerosols and their precursors, related species, and chemical tracers. Five chemical transport models (CTMs) were used for chemical forecasting. Customized bottom-up emission inventories for East Asia were generated prior to the mission to support chemical forecasting and to serve as a priori for evaluation with the aircraft data. Validation flights were conducted for the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument and revealed little bias (6 plus or minus 2%) in the MOPITT measurements of CO columns. A major event of transpacific Asian pollution was characterized through combined analysis of TRACE-P and MOPITT data. The TRACE-P observations showed that cold fronts sweeping across East Asia and the associated warm conveyor belts (WCBs) are the dominant pathway for Asian outflow to the Pacific in spring. The WCBs lift both anthropogenic and biomass burning (SE Asia) effluents to the free troposphere, resulting in complex chemical signatures. The TRACE-P data are in general consistent with a priori emission inventories, lending confidence in our ability to quantify Asian emissions from socioeconomic data and emission factors. However, the residential combustion source in rural China was found to be much larger than the a priori, and there were also unexplained chemical enhancements (HCN, CH3Cl, OCS, alkylnitrates) in Chinese urban plumes. The Asian source of CCl4 was found to be much higher than government estimates. Measurements of HCN and CH3CN indicated a dominant biomass burning source and ocean sink for both gases. Large fractions of sulfate and nitrate were found to be present in dust aerosols. Photochemical activity in the Asian outflow was strongly reduced by aerosol attenuation of UV radiation, with major implications for the concentrations of HOx, radicals. New particle formation, apparently from ternary nucleation involving NH3, was observed in Chinese urban plumes.

Description: The Pacific Exploratory Mission-West B (PEM-West B) explored atmospheric layer structure using measurements of O3, H2O, CO, and CH4 from the NASA DC-8 fast-response instruments. The mission took place in February-March 1994 over the western Pacific, mainly in the northern hemisphere. Results were compared with similar measurements made during the Pacific Exploratory Mission-West A (PEM-West A) in September-October 1991. PEM-West B sampled 94 vertical profiles, with an average atmospheric depth per profile of 6.4 km, and this sampling yielded 254 discrete layers. PEM-West A sampled 105 profiles, also with a 6.4 km average depth, yielding 538 layers. Both missions revealed that layers containing high ozone and low water vapor were the most abundant, and low ozone and high water vapor layers were the next most abundant. Lidar images and potential vorticity cross sections showed the former associated with subsidence from the stratosphere in middle latitudes, spreading into the tropics. The latter was associated with convection from the boundary layer. The partition among different types of layers only changed slightly in the two missions, although PEM-West B had half as many layers. Compared to PEM-West A, PEM-West B showed only one-third the number of layers associated with polluted continental air. However, PEM-West B revealed significantly more layers showing characteristics of descended clean marine air. In some cases these layers originated from the southern hemisphere. For ozone- and water-vapor-rich layers, the ozone deviation amplitude was higher in low latitudes and lower in high latitudes in PEM-West B. The mean thickness of layers increased from about 450 m in PEM-West A to 680 in in PEM-West B. Layers also existed in the Intertropical Convergence Zone. CO2 measurements had sufficient vertical resolution to show layer structure as well.

Description: With aircraft-mounted in-situ and remote sensing instruments for dynamical, thermal. and chemical measurements, we studied two cases of tropopause folding. In both folds we found Kelvin-Helmholtz billows with horizontal wavelength of about 900 m and thickness of about 120 m. In one case the instability was effectively mixing the bottomside of the fold, leading to the transfer of stratospheric air into the troposphere. Also we discovered in both cases small-scale secondary ozone maxima shortly after the aircraft ascended past the topside of the fold that corresponded to regions of convective instability. We interpreted this phenomenon as convectively breaking gravity waves. Therefore, we posit that convectively breaking gravity waves acting on tropopause folds must be added to the list of important irreversible mixing mechanisms leading to stratosphere-troposphere exchange.