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Reliable assessment of the impact of aerosols emitted from boreal forest fires on the Arctic climate necessitates improved understanding of emissions and the microphysical properties of carbonaceous (black carbon (BC) and organic aerosols (OA)) and inorganic aerosols. The size distributions of BC were measured by an SP2 based on the laser-induced incandescence technique on board the DC-8 aircraft during the NASA ARCTAS campaign. Aircraft sampling was made in fresh plumes strongly impacted by wildfires in North America (Canada and California) in summer 2008 and in those transported from Asia (Siberia in Russia and Kazakhstan) in spring 2008. We extracted biomass burning plumes using particle and tracer (CO, CH3CN, and CH2Cl2) data. OA constituted the dominant fraction of aerosols mass in the submicron range. The large majority of the emitted particles did not contain BC. We related the combustion phase of the fire as represented by the modified combustion efficiency (MCE) to the emission ratios between BC and other species. In particular, we derived the average emission ratios of BC/CO = 2.3 +/- 2.2 and 8.5 +/- 5.4 ng/cu m/ppbv for BB in North America and Asia, respectively. The difference in the BC/CO emission ratios is likely due to the difference in MCE. The count median diameters and geometric standard deviations of the lognormal size distribution of BC in the BB plumes were 136-141 nm and 1.32-1.36, respectively, and depended little on MCE. These BC particles were thickly coated, with shell/core ratios of 1.3-1.6. These parameters can be used directly for improving model estimates of the impact of BB in the Arctic.

We use aircraft observations of carbon monoxide (CO) from the NASA ARCTAS and NOAA ARCPAC campaigns in April 2008 together with multiyear (2003-2008) CO satellite data from the AIRS instrument and a global chemical transport model (GEOS-Chem) to better understand the sources, transport, and interannual variability of pollution in the Arctic in spring. Model simulation of the aircraft data gives best estimates of CO emissions in April 2008 of 26 Tg month-1 for Asian anthropogenic, 9.1 for European anthropogenic, 4.2 for North American anthropogenic, 9.3 for Russian biomass burning (anomalously large that year), and 21 for Southeast Asian biomass burning. We find that Asian anthropogenic emissions are the dominant source of Arctic CO pollution everywhere except in surface air where European anthropogenic emissions are of similar importance. Synoptic pollution influences in the Arctic free troposphere include contributions of comparable magnitude from Russian biomass burning and from North American, European, and Asian anthropogenic sources. European pollution dominates synoptic variability near the surface. Analysis of two pollution events sampled by the aircraft demonstrates that AIRS is capable of observing pollution transport to the Arctic in the mid-troposphere. The 2003-2008 record of CO from AIRS shows that interannual variability averaged over the Arctic cap is very small. AIRS CO columns over Alaska are highly correlated with the Ocean Nino Index, suggesting a link between El Nino and northward pollution transport. AIRS shows lower-than-average CO columns over Alaska during April 2008, despite the Russian fires, due to a weakened Aleutian Low hindering transport from Asia and associated with the moderate 2007-2008 La Nina. This suggests that Asian pollution influence over the Arctic may be particularly large under strong El Nino conditions.

Aerosol data collected near Asia on the DC-8 aircraft platform during TRACE-P has been examined for evidence of uptake of NO3(-) and SO4(-) on dust surfaces. Data is compared between a sector where dust was predominant and a sector where dust was less of an influence. Coincident with dust were higher mixing ratios of anthropogenic pollutants. HNO3, SO2, and CO were higher in the dust sector than the nondust sector by factors of 2.7, 6.2, and 1.5, respectively. The colocation of dust and pollution sources allowed for the uptake of NO3(-) and nss-SO4(-) on the coarse dust aerosols, increasing the mixing ratios of these particulates by factors of 5.7 and 2.6 on average. There was sufficient nss-SO4(-) to take up all of the NH4(+) present, with enough excess nss-SO4(-) to also react with dust CaCO3. This suggests that the enhanced NO3(-) was not in fine mode NH4NO3. Particulate NO3(-) (p-NO3(-)) constituted 54% of the total NO3(-), (t-NO3(-)) on average, reaching a maximum of 72% in the dust sector. In the nondust sector, p-NO3(-) contributed 37% to t-NO3(-), likely due to the abundance of sea salts there. In two other sectors where the influence of dust and sea salt were minimal, p-NO3(-), accounted for < 15% of t-NO3(-).

We characterize the chemical composition of Asian continental outflow observed during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) mission during February-April 2001 in the western Pacific using data collected on the NASA DC-8 aircraft. A significant anthropogenic impact was present in the free troposphere and as far east as 150degE longitude reflecting rapid uplift and transport of continental emissions. Five-day backward trajectories were utilized to identify five principal Asian source regions of outflow: central, coastal, north-northwest(NNW), southeast (SE), and west-southwest (WSW). The maximum mixing ratios for several species, such as CO, C2Cl4, CH3Cl, and hydrocarbons, were more than a factor of 2 larger in the boundary layer of the central and coastal regions due to industrial activity in East Asia. CO was well correlated with C2H2, C2H6, C2Cl4, and CH3Cl at low altitudes in these two regions (r(sup 2) approx. 0.77-0.97). The NNW, WSW, and SE regions were impacted by anthropogenic sources above the boundary layer presumably due to the longer transport distances of air masses to the western Pacific. Frontal and convective lifting of continental emissions was most likely responsible for the high altitude outflow in these three regions. Photochemical processing was influential in each source region resulting in enhanced mixing ratios of O3, PAN, HNO3, H2O2, and CH3OOH. The air masses encountered in all five regions were composed of a complex mixture of photcrchemically aged air with more recent emissions mixed into the outflow as indicated by enhanced hydrocarbon ratios (C2H2/CO greater than or equal to 3 and C3H8/C2H6 greater than or equal to 0.2). Combustion, industrial activities, and the burning of biofuels and biomass all contributed to the chemical composition of air masses from each source region as demonstrated by the H6, SO2, and C2Cl4 were compared for the TRACE-P and PEM-West B missions. In the more northern regions, O3, CO, and SO2 were higher at low altitudes during TRACE-P. In general, mixing ratios were fairly similar between the two missions in the southern regions. A comparison between CO/CO2, CO/CH4, C2H6/C3H8, NO(x)/SO2, and NO(y)/(SO2 + nss-SO4) ratios for the five source regions and for the 2000 Asian emissions summary showed vay close agreement indicating that Asian emissions were well represented by the TRACE-P data and tbe emissions inventory.

Airborne measurements of aerosol (Condensation Nuclei, CN) and selected trace gases made in the areas of the North Atlantic Ocean during SONEX (October/November 1997), and the south tropical Pacific Ocean during PEM-Tropics A (September/October 1996) and PEM-Tropics B (March/April 1999) have been analyzed. Emphasis is on the interpretations of variations in the number densities of the fine (>17 nm) and ultrafine (>8 nm) CN in the upper troposphere (8-12 km). These data suggest that large number densities of highly volatile CN (10(exp 4)-10(exp 5)/cu cm) are present in the clean upper troposphere with highest values over the tropical1subtropical region. Through marine convection and long-distance horizontal transport, volatile CN originating from the tropical/subtropical regions can frequently impact the abundance of aerosol in the middle and upper troposphere at mid to high latitudes. Nonvolatile aerosol particles behave in a manner similar to tracers of combustion (CO) and photochemical pollution (PAN), implying a source from continental pollution of industrial or biomass burning origin. In the upper troposphere, we find that volatile and nonvolatile partials number densities are inversely correlated. An aerosol microphysical model is used to suggest that coagulation of fine volatile particles with fewer larger nonvolatile particles provides one possible mechanism for this relationship. It appears that nonvolatile particles, of principally anthropogenic origin,provide a highly efficient removal process for the fine volatile aerosol.

Mixing ratios of nonmethane hydrocarbons (NMHCS) were not enhanced in whole air samples collected within the North Atlantic Flight Corridor (NAFC) during the fall of 1997. The investigation was conducted aboard NASA's DC-8 research aircraft, as part of the Subsonic Assessment-Ozone and Nitrogen Experiment (SONEX). NMHC enhancements were not detected within the general Organized Tracking System (OTS) of the NAFC, nor during two tail-chases of the DC-8's own exhaust. Because positive evidence of aircraft emissions was demonstrated by enhancements in both nitrogen oxides and condensation nuclei during SONEX, the NMHC results suggest that the commercial air traffic fleet operating in the North Atlantic region does not contribute significantly to NMHCs in the NAFC.

A significant increase in sulfuric acid aerosol concentration was detected above 10 km pressure altitude during a cross-corridor flight out of Shannon on October 23, 1997. The source of this aerosol is ascribed to commercial aircraft operations in flight corridors above 10 km, because (1) a stable atmosphere prevented vertical air mass exchanges and thus eliminated surface sources, (2) air mass back trajectories documented the absence of remote continental sources, and (3) temperature profiler data showed the tropopause at least one kilometers above flight altitude throughout the flight. Particle volatility identified 70% H2SO4, 20% (NH4)2SO4 and 10% nonvolatile aerosol in the proximity of flight corridors, and (10-30)% H2SO4, up to 50% (NH4)2SO4, and (40-60)% nonvolatile aerosols in air that was not affected by aircraft operations below 10 km. Only a very small fraction of the nonvolatile particles (determined with a condensation nucleus counter) could be morphologically identified as soot aerosol (validated by scanning electron microscopy of wire impactor samples). The newly formed H2SO4 particles did not measurably affect surface area and volume of the background aerosol due to their small size, hence did not affect radiative transfer directly.

Atmospheric flow patterns are examined over the South Atlantic Ocean where a maximum of tropospheric ozone has been observed just west of southern Africa. We investigate the flow climatology during October and perform a case study for six days during October 1989. Horizontal and vertical motions are examined and used to prepare 3D backward trajectories from the region of greatest ozone. An initially zonally symmetric distribution of ozone is treated as a passive tracer and advected by 3D flows forecast by the global model. Results from the passive tracer simulation indicate that 3D advection alone can produce a maximum of tropospheric ozone in the observed location. In addition, the trajectories suggest that by-products of biomass burning could be transported to the area of maximum ozone. Low-level flow from commonly observed regions of burning in Africa streams westward to the area of interest. Over Brazil, if the burning by-products are carried into the upper troposphere by convective process, they then could be transported eastward to the ozone feature in approximately five days. There is considerable subsidence over the tropical southern Atlantic, such that stratospheric influences also are a factor in producing the ozone maximum. Both planetary-scale and transient synoptic-scale circulation features play major roles in the various transport processes that influence the region. In summary, the observed tropospheric ozone maximum appears to be caused by a complex set of horizontal and vertical advections, transport from regions of biomass burning, and stratospheric influences.

The derivations of the energy budget equations for divergent and rotational components of kinetic energy are provided. The intense convection periods studied are: (1) synoptic scale data of 3 or 6 hour intervals and (2) mesoalphascale data every 3 hours. Composite energies and averaged budgets for the periods are presented; the effects of random data errors on derived energy parameters is investigated. The divergent kinetic energy and rotational kinetic energy budgets are compared; good correlation of the data is observed. The kinetic energies and budget terms increase with convective development; however, the conversion of the divergent and rotational energies are opposite.

Mesoscale sounding data from a truth rawinsonde network and a VAS from March 6-7, 1982 are statistically studied. The parameters of temperature, geopotential height, and mixing ratio at 850, 700, 500, 300, and 200 mb levels, and thickness and precipitable water are examined. The VAS retrieval gradients derived from a physical algorithm and from a regression technique are analyzed; the analysis reveals that both techniques have similar error characteristics and capabilities for calculating gradients of mesoscale temperature and geopotential height. Ground-truth rawinsonde data and VAS retrievals are compared; it is observed that VAS data describes weaker gradients than rawinsonde data.

Researchers goals are to describe the information content of Vertical Atmospheric Sounder (VAS) radiance data, especially the 6.7 micrometers water vapor channel, to better interpret the atmosphere's water vapor structure from 6.7 micrometers imagery, and to investigate new analysis and forecasting techniques utilizing retrieved VAS soundings. Researchers made major progress toward these goals during FY-85. They are investigating 6.7 micrometer imagery on 6 to 7 March 1982, a day when special mesoscale ground truth data were collected during the 1982 atmospheric variability experiment/vertical amospheric sounder (AVE/VAS) field experiment. A dark (dry) image streak having mesoscale details was located over the special data region, and it provides the major focus of the case study. Mesoscale radiosonde-derived humidity data are found to verify fine scale features of the image that are not evident from the standard National Weather Service network. Thus, VAS imagery is a reliable detector of mesoscale moisture structure during this case. To investigate causes for the image streak, researchers are calculating water vapor budgets. Subsidence is found to be a factor in the current case as well; however, patterns of descent are not related to the jet streak according to traditional conceptual models. Thus, it appears that more research into jet stream dynamics is needed in order to better interpret 6.7 micrometer imagery.

The goals of this research were to better understand interactions between areas of intense convection and their surrounding mesoscale environments by using diagnostic budgets of kinetic (KE) and available potential energy (APE). Three cases of intense convection were examined in detail. 1) Atmospheric Variability Experiments (AVE) carried out on 24 to 25 April 1975 were studied. Synoptic scale data at 3 to 6 hour intervals, contained two mesoscale convective complexes (MCCs). Analyses included total KE budgets and budgets of divergent and rotational components of KE. 2) AVE-Severe Environmental Storms and Mesoscale Experiments (SESAME)-4 carried out on 10 to 11 April 1979 were studied. Synotpic and meso alpha-scale data (250 km spacing, 3 hour intervals), contained the Red River Valley tornado outbreak. Analyses included total KE budgets (separate synoptic and mesoscale version), budgets for the divergent and rotational components, and the generation of APE by diabatic processes. 3) AVE-SESAME 5 studies were carried out on 20 to 31 May 1979. Synoptic and meso beta-scale data (75 km spacing, 1 1/2 to 3 hour intervals), contained a small MCC. Analyses include separate KE budgets for the synotic and meso beta-scales and a water vapor budget. Major findings of these investigations are: (1) The synoptic scale storm environment contains energy conversions and transports that are comparable to those of mature midlatitude cyclones. (2) Energetic in the mesoscale storm environment are often an order of magnitude larger than those in an undisturbed region. (3) Mesoscale wind maxima form in the upper troposphere on the poleward sides of convective areas, whereas speeds decrease south of storm regions.

GOES-VAS satellite retrievals are used to investigate an intense convective outbreak over the Mississippi River Valley on 21-22 July 1982. The primary goals are to assess the strengths and weaknesses of three methods for computing vertical motion using satellite retrievals and to determine the effects of short interval observations on the calculations. Then, the vertical motions are incorporated with thermodynamic parameters to assess the usefulness of VAS data in delineating factors leading to storm formation. Results indicate that the quasi-geotrophic omega equation provided patterns and magnitudes most consistent with observed weather events and the 12 h radiosonde-derived motions. The vorticity method generally produced reasonable patterns, especially over the convective outbreak, although magnitudes were large due to its time derivative.