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Crawford, James H.

Publications and source records attributed to Crawford, James H..

22 records · Page 2

A Reevaluation of Airborne HO(x) Observations from NASA Field Campaigns

In-situ observations of tropospheric HO(x) (OH and HO2) obtained during four NASA airborne campaigns (SUCCESS, SONEX, PEM-Tropics B and TRACE-P) are reevaluated using the NASA Langley time-dependent photochemical box model. Special attention is given to previously diagnosed discrepancies between observed and predicted HO2 which increase with higher NO(x) levels and at high solar zenith angles. This analysis shows that much of the model discrepancy at high NO(x) during SUCCESS can be attributed to modeling observations at time-scales too long to capture the nonlinearity of HO(x) chemistry under highly variable conditions for NO(x). Discrepancies at high NO(x) during SONEX can be moderated to a large extent by complete use of all available precursor observations. Differences in kinetic rate coefficients and photolysis frequencies available for previous studies versus current recommendations also explain some of the disparity. Each of these causes is shown to exert greater influence with increasing NO(x) due to both the chemical nonlinearity between HO(x) and NO(x) and the increased sensitivity of HO(x) to changes in sources at high NO(x). In contrast, discrepancies at high solar zenith angles will persist until an adequate nighttime source of HO(x) can be identified. It is important to note that this analysis falls short of fully eliminating the issue of discrepancies between observed and predicted HO(x) for high NO(x) environments. These discrepancies are not resolved with the above causes in other data sets from ground-based field studies. Nevertheless, these results highlight important considerations in the application of box models to observationally based predictions of HO(x) radicals.

Olson, Jennifer↗

Airborne Observations and Satellite Validation: INTEX-A Experience and INTEX-B Plans

Intercontinental Chemical Transport Experiment (INTEX; http://cloudl.arc.nasa.gov) is an ongoing two-phase integrated atmospheric field experiment being performed over North America (NA). Its first phase (INTEX-A) was performed in the summer of 2004 and the second phase (INTEX-B) is planned for the early spring of 2006. The main goal of INTEX-NA is to understand the transport and transformation of gases and aerosols on transcontinental/intercontinental scales and to assess their impact on air quality and climate. Central to achieving this goal is the need to relate space-based observations with those from airborne and surface platforms. During INTEX-A, NASA s DC-8 was joined by some dozen other aircraft from a large number of European and North American partners to focus on the outflow of pollution from NA to the Atlantic. Several instances of Asian pollution over NA were also encountered. INTEX-A flight planning extensively relied on satellite observations and in turn Satellite validation (Terra, Aqua, and Envisat) was given high priority. Over 20 validation profiles were successfully carried out. DC-8 sampling of smoke from Alaskan fires and formaldehyde over forested regions, and simultaneous satellite observations of these provided excellent opportunities for the interplay of these platforms. The planning for INTEX-5 is currently underway, and a vast majority of "standard" and "research" products to be retrieved from Aura instruments will be measured during INTEX-B throughout the troposphere. INTEX-B will focus on the inflow of pollution from Asia to North America and validation of satellite observations with emphasis on Aura. Several national and international partners are expected to coordinate activities with INTEX-B, and we expect its scope to expand in the coming months. An important new development involves partnership with an NSF-sponsored campaign called MIRAGE (Megacity Impacts on Regional and Global Environments- Mexico City Pollution Outflow Field Campaign; http://mirage- mex.acd.ucar.edu/index.html). This partnership will utilize both the NASA-DC-8 mad NCAR C-130 aircrafts and greatly expand the temporal and spatial coverage of these experiments. We will briefly describe our INTEX-A experience and discuss plans for INTEX-B activities especially as they relate to validation and interpretation of Aura observations.

Crawford, James H.↗

Asian Outflow and Trans-Pacific Transport of Carbon Monoxide and Ozone Pollution: An Integrated Satellite, Aircraft, and Model Perspective

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 (R(exp 2) = 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) 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). 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.

Heald, Colette L.↗

Transport and Chemical Evolution over the Pacific (TRACE-P)Aircraft Mission: Design, Execution, and First Results

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.

Jacob, Daniel J.↗