ALBERT

Description: This paper presents airborne measurements of multiple atmospheric trace constituents including greenhouse gases (such as CO2, CH4, O3) and biomass burning tracers (such as CO, CH3CN) downwind of an exceptionally large wildfire. In summer 2013, the Rim wildfire, ignited just west of the Yosemite National Park, California, and burned over 250,000 acres of the forest during the 2-month period (17 August to 24 October) before it was extinguished. The Rim wildfire plume was intercepted by flights carried out by the NASA Ames Alpha Jet Atmospheric eXperiment (AJAX) on 29 August and the NASA DC-8, as part of SEAC4RS (Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys), on 26 and 27 August during its intense, primary burning period. AJAX revisited the wildfire on 10 September when the conditions were increasingly smoldering, with slower growth. The more extensive payload of the DC-8 helped to bridge key measurements that were not available as part of AJAX (e. g. CO). Data analyses are presented in terms of emission ratios (ER), emission factors (EF) and combustion efficiency and are compared with previous wildfire studies. ERs were 8.0 ppb CH4/(ppm CO2) on 26 August, 6.5 ppb CH4 (ppm CO2)1 on 29 August and 18.3 ppb CH4 (ppm CO2)1 on 10 September 2013. The increase in CH4 ER from 6.5 to 8.0 ppb CH4/(ppm CO2) during the primary burning period to 18.3 ppb CH4/(ppm CO2) during the fire's slower growth period likely indicates enhanced CH4 emissions from increased smoldering combustion relative to flaming combustion. Given the magnitude of the Rim wildfire, the impacts it had on regional air quality and the limited sampling of wildfire emissions in the western United States to date, this study provides a valuable dataset to support forestry and regional air quality management, including observations of ERs of a wide number of species from the Rim wildfire.

Description: A comprehensive group of reactive nitrogen species (NO, NOz, HN03, HOzN02, PANs, alkyl nitrates, and aerosol-NO3) were measured over North America during July/August 2004 from the NASA DC-8 platform (0.1 - 12 km). Nitrogen containing tracers of biomass combustion (HCN and CH3CN) were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, convection, lightning, and the stratosphere was sampled over the continental United States, the Atlantic, and the Pacific. The North American upper troposphere (UT) was found to be greatly influenced by both lightning NO, and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO,. Observational data suggest that lightning was a far greater contributor to NO, in the UT than previously believed. PAN provided a dominant reservoir of reactive nitrogen in the UT while nitric acid dominated in the lower troposphere (LT). Peroxynitric acid (H02N02) was present in sizable concentrations peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the LT. Plumes from Alaskan fires contained large amounts of PAN and aerosol nitrate but little enhancement in ozone. A comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.

Description: We analyze aircraft observations obtained during INTEX-A (1 July 14 - August 2004) to examine the summertime influence of Asian pollution in the free troposphere over North America. By applying correlation analysis and Principal Component Analysis (PCA) to the observations between 6-12 km, we find dominant influences from recent convection and lightning (13 percent of observations), Asia (7 percent), the lower stratosphere (7 percent), and boreal forest fires (2 percent), with the remaining 71 percent assigned to background. Asian airmasses are marked by high levels of CO, O3, HCN, PAN, acetylene, benzene, methanol, and SO4(2-). The partitioning of reactive nitrogen species in the Asian plumes is dominated by peroxyacetyl nitrate (PAN) (approximately 600 pptv), with varying NO(x)/HNO3 ratios in individual plumes consistent with different plumes ages ranging from 3 to 9 days. Export of Asian pollution in warm conveyor belts of mid-latitude cyclones, deep convection, and lifting in typhoons all contributed to the five major Asian pollution plumes. Compared to past measurement campaigns of Asian outflow during spring, INTEX-A observations display unique characteristics: lower levels of anthropogenic pollutants (CO, propane, ethane, benzene) due to their shorter summer lifetimes; higher levels of biogenic tracers (methanol and acetone) because of a more active biosphere; as well as higher levels of PAN, NO(x), HNO3, and O3 (more active photochemistry possibly enhanced by injection of lightning NO(x)). The high delta O3/delta CO ratio (0.76 mol mol(exp -1)) of Asian plumes during INTEX-A is due to a combination of strong photochemical production and mixing with stratospheric air along isentropic surfaces. The GEOS-Chem global chemical transport model captures the timing and location of the Asian plumes remarkably well. However, it significantly underestimates the magnitude of the enhancements.

Description: We use observations from two aircraft during the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) campaign over the eastern United States and North Atlantic during summer 2004, interpreted with a global 3-D model of tropospheric chemistry (GEOS-Chem) to test current understanding of the regional sources, chemical evolution, and export of nitrogen oxides. The boundary layer NO(x) data provide top-down verification of a 50% decrease in power plant and industry NO(x) emissions over the eastern United States between 1999 and 2004. Observed 8-12 8 km NO(x) concentrations in ICARTT were 0.55 +/- 36 ppbv, much larger than in previous United States aircraft campaigns (ELCHEM, SUCCESS, SONEX). We show that regional lightning was the dominant source of this NO(x) and increased upper tropospheric ozone by 10 ppbv. Simulating the ICARTT upper tropospheric NO(x) observations with GEOS-Chem require a factor of 4 increase in the model NO(x) yield per flash (to 500 mol/flash). Observed OH concentrations were a factor of 2 lower than can be explained from current photochemical models, and if correct would imply a broader lightning influence in the upper troposphere than presently thought.An NO(y)-CO correlation analysis of the fraction f of North American NO(x) emissions vented to the free troposphere as NO(y) (sum of NO(x) and its oxidation products PAN and HNO3) s shows observed f=16+/-10 percent and modeled f=14 +/- 8 percent, consistent with previous studies. Export to the lower free troposphere is mostly HNO3 but at higher altitudes is mostly PAN. The model successfully simulates NO(y) export efficiency and speciation, supporting previous model estimates of a large U.S. contribution to tropospheric ozone through NO(x) and PAN export.