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Ultrahigh performance LC/FT-MS non-targeted screening for biomass burning organic aerosol with MZmine2 and MFAssignR

In recent years, ultrahigh performance liquid chromatography Fourier transform mass spectrometry (LC/FT-MS) based non-targeted screening (NTS) methods have become increasingly popular for comprehensive analysis of complex organic mixtures. However, applying these methods for environmental complex mixture analysis is challenging due to the extreme complexity of natural samples and a lack of standard samples or surrogates for environmental complex mixtures. Furthermore, limited molecular markers in the databases and insufficient data processing software workflows make the application of these methods more challenging for environmental complex mixtures. In this work, we implement a new NTS data processing workflow to process data collected from ultrahigh performance liquid chromatography and Fourier transform Orbitrap Elite Mass Spectrometry (LC/FT-MS) by combining MZmine2 and MFAssignR, two opensource data processing tools and commercial Mesquite liquid smoke as a surrogate for biomass burning organic aerosol. MZmine2.53 data extraction followed MFAssignR molecular formula assignment offered noise free and highly accurate 1733 individual molecular formulas presented in liquid smoke with 4906 molecular species, including isomers. The results of this new approach were consistent with the results of direct infusion FT-MS analysis confirming its reliability. Over 90% of the molecular formulas presented in mesquite liquid smoke were matched with the molecular formulas of ambient biomass burning organic aerosol. This suggests the potential use of commercial liquid smoke as a surrogate for biomass burning organic aerosol research. Furthermore, the presented method significantly improves the identification of the molecular composition of biomass burning organic aerosol by successfully addressing some of the limitations related to the data analysis and giving a semi quantitative insight into the analysis.

54 ENVIRONMENTAL SCIENCES↗

Metabolites of Tobacco- and E-Cigarette-Related Nitrosamines Can Drive Cu 2+ -Mediated DNA Oxidation

Nitrosamine metabolites resulting from cigarette smoking and E-cigarette (E-cig) vaping cause DNA damage that can lead to genotoxicity. While DNA adducts of metabolites of nitrosamines 4-(methylnitrosamino)-1-(3-pyridyl)-1-butanone (NNK) and N-nitrosonornicotine (NNN) are well-known tobacco-related cancer biomarkers, only a few studies implicate NNN and NNK in DNA oxidation in humans. NNK and NNN were found in the urine of E-cigarette users who never smoked cigarettes. This paper proposes the first chemical pathways of DNA oxidation driven by NNK and NNN metabolites in redox reactions with Cu 2+ and NADPH leading to reactive oxygen species (ROS). A microfluidic array with thin films of DNA and metabolic enzymes that make metabolites of NNN and NNK in the presence of Cu 2+ and NADPH was used to estimate relative rates of DNA oxidation. Detection by electrochemiluminescence (ECL) employed a new ECL dye [Os(tpy-benz-COOH) 2 ] 2+ that is selective for and sensitive to the primary DNA oxidation product 8-oxo-7,8-dihydro-2-deoxyguanosine (8-oxodG) in DNA. Enzyme–DNA films on magnetic beads were used to produce nitrosamine metabolites that enter ROS-forming redox cycles with Cu 2+ and NADPH, and liquid chromatography–mass spectrometry (LC–MS) was used to quantify 8-oxodG and identify metabolites. ROS were detected by optical sensors. Metabolites of NNK and NNN + Cu 2+ + NADPH generated relatively high rates of DNA oxidation. Lung is the exposure route in smoking and vaping, human lung tissue contains Cu 2+ and NADPH, and lung microsomal enzymes gave the highest rates of DNA oxidation in this study. Furthermore, E-cigarette vapor contains 6-fold more copper than that in cigarette smoke, which could exacerbate DNA oxidation.

59 BASIC BIOLOGICAL SCIENCES↗

Vegetable intake and the risk of bladder cancer in the BLadder Cancer Epidemiology and Nutritional Determinants (BLEND) international study

Although a potential inverse association between vegetable intake and bladder cancer risk has been reported, epidemiological evidence is inconsistent. This research aimed to elucidate the association between vegetable intake and bladder cancer risk by conducting a pooled analysis of data from prospective cohort studies. Vegetable intake in relation to bladder cancer risk was examined by pooling individual-level data from 13 cohort studies, comprising 3203 cases among a total of 555,685 participants. Pooled multivariate hazard ratios (HRs), with corresponding 95% confidence intervals (CIs), were estimated using Cox proportional hazards regression models stratified by cohort for intakes of total vegetable, vegetable subtypes (i.e. non-starchy, starchy, green leafy and cruciferous vegetables) and individual vegetable types. In addition, a diet diversity score was used to assess the association of the varied types of vegetable intake on bladder cancer risk. The association between vegetable intake and bladder cancer risk differed by sex ( P -interaction = 0.011) and smoking status ( P -interaction = 0.038); therefore, analyses were stratified by sex and smoking status. With adjustment of age, sex, smoking, energy intake, ethnicity and other potential dietary factors, we found that higher intake of total and non-starchy vegetables were inversely associated with the risk of bladder cancer among women (comparing the highest with lowest intake tertile: HR = 0.79, 95% CI = 0.64–0.98, P = 0.037 for trend, HR per 1 SD increment = 0.89, 95% CI = 0.81–0.99; HR = 0.78, 95% CI = 0.63–0.97, P = 0.034 for trend, HR per 1 SD increment = 0.88, 95% CI = 0.79–0.98, respectively). However, no evidence of association was observed among men, and the intake of vegetable was not found to be associated with bladder cancer when stratified by smoking status. Moreover, we found no evidence of association for diet diversity with bladder cancer risk. Higher intakes of total and non-starchy vegetable are associated with reduced risk of bladder cancer for women. Further studies are needed to clarify whether these results reflect causal processes and potential underlying mechanisms.

59 BASIC BIOLOGICAL SCIENCES↗

Connecting the Radiative Influences of Aerosol upon the Mass Flux Profiles of Shallow Cumuli across the Southeast Atlantic Ocean Basin and its Boundaries (Final Report)

The Atlantic Ocean covers approximately 25% of Earth’s surface and the atmosphere above it is home to a complex array of clouds and aerosols that have important influences on regional and global weather and climate. These influences must be accurately depicted in short range, medium range, seasonal, and climate forecast models. Conditions over the tropical Atlantic are particularly complex due to continental scale plumes of dust from the Sahara Desert and smoke from agricultural burning in Africa that drift across the Atlantic Ocean basin toward the Americas. These plumes are often found meandering in the lower atmosphere above shallow tropical clouds that form above the ocean surface, presumably mingling with these clouds on occasion due to convective mixing processes. Elevated dust and smoke particles absorb incoming sunlight and substantially warm the marine atmosphere in the layer in which they are present. This warming may alter the thermal stability of the marine atmosphere and may throttle or enhance the development of clouds, change their internal structure and the rate at which they precipitate. Alternatively, it may isolate the lower atmosphere from drier layers above enabling water vapor to accumulate near the ocean surface potentially leading to the development of deeper convection. Our study was organized around the principal concept of determining the impact of African smoke and dust plumes upon cloud development at ASI and understanding how a popular shallow convection parameterization used in models responds to the presence of this aerosol. We analyzed observations collected during the US Department of Energy (DOE) Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign using the Atmospheric Radiation Measurement Program’s Mobile Facility #1 (AMF-1), which was deployed to Ascension Island (ASI) in Southeastern Atlantic for a one-year period. Ascension Island is immediately downwind from an African source of these plumes, but far enough removed to enable the lower atmosphere to have reacted to their presence. A main goal of our study was to compute radiative heating rate profiles over Ascension Island and along the trajectory from the biomass burning regions along coastal Africa to Ascension Island. To compute the radiative heating rate due to aerosols and clouds, we employed observed profiles of temperature, humidity, and clouds from LASIC alongside aerosol optical properties from the Modern-era Retrospective analysis for Research and Applications Version 2 (MERRA-2), as input for the Rapid Radiation Transfer Model (RRTM). Radiative heating was also assessed across the southeast Atlantic Ocean using an ensemble of back trajectories from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model. We were successful in this effort and the resulting publication is already being cited despite its relatively short lifetime in the literature. The second part of our study involved the process-level representation of the clouds observed over the Southeastern Atlantic in models. Our initial task, upon which the balance of this portion of the study depended, was to evaluate the representativeness of the clouds observed by AMF-1. What orographic influence did Ascension Island have on the measured cloud structure? We set out to answer this question by trying to separate observations that were clearly indicative of orographic forcing from those that were representative of open ocean. The siting of AMF-1, which was 340-m above sea-level on the slope of a steep escarpment, proved demonstrably problematic for cloud process measurements. Despite considerable effort using multiple approaches including artificial intelligence (AI), we were unable to successfully compensate for the orographic forcing present at the AMF-1 site on ASI and, hence, produce process-level summaries of the convective mass flux representative of open ocean over the Southeastern Atlantic. Even though the project has officially ended, we are making a final attempt using two new types of clustering algorithm (i.e., AI) on the recommendation of a former student, who is an expert in this area. Since we have only recently begun to test these new AI schemes, the recommendations from the second part of our project outlined below are based on our experience at the time of this report.

54 ENVIRONMENTAL SCIENCES↗

Capturing plume behavior in complex terrain: an overview of the Nevada National Security Site Meteorological Experiment (METEX21)

METEX21 was an atmospheric tracer release experiment executed at the Department of Energy’s Nevada National Security Site (NNSS) in the southwestern U.S to study terrain-induced wind and thermodynamic conditions that influence local-scale (<5-km) plume transport under varying atmospheric forcing conditions. Meteorological observations were collected using 10-m tall meteorological towers, 2-m tall tripods with 3-d sonic anemometers, a 3-m tall eddy covariance flux tower, Doppler profiling lidars, Doppler scanning lidars, weather-balloon launched radiosondes, and a tethered balloon equipped with wind, temperature, and aerosol sensors at heights up to 800 m. A smoke tracer was released along three transects in the horizontal and vertical directions and observed with video cameras, aerosol sensors and lidars (via aerosol backscatter). The observations showed evidence of large-scale/synoptic transience as well as local-scale upslope and downslope flows, along-axis valley flows, recirculation eddies on leeward slopes, and periods of strong shear and veer aloft. The release days were classified as either synoptically-driven or locally-driven, and a single case day is presented in detail for each. Synoptically-forced days show relatively narrow smoke plumes traveling down the valley from north to south (with the predominant wind direction), with little deviation in transport direction regardless of the elevation or ground locations of the smoke releases, except near the presence of leeside recirculation eddies. Locally-forced days exhibit a wider range of plume behavior due to the combination of thermally-induced valley and slope flows, which are often flowing in different cardinal directions, and wind shear found aloft at higher altitudes and elevations. We saw evidence of smoke lofting on top of the mesas due to strong upslope flows on these days. A major finding of this experiment was the effectiveness of scanning lidars to measure 2-dimensional plume transport out to a 2–3 km distance; much farther than could be visibly observed. METEX21 was the first of three planned tracer experiments at NNSS, and future experiments will incorporate multiple tracers to improve individual plume identification so that finer resolution flow details can be attained from these measurements, as well as deploy a larger suite of meteorological instrumentation, including more temperature profiling data.

54 ENVIRONMENTAL SCIENCES↗

Biomass burning emission analysis based on MODIS aerosol optical depth and AeroCom multi-model simulations: implications for model constraints and emission inventories

We assessed the biomass burning (BB) smoke aerosol optical depth (AOD) simulations of 11 global models that participated in the AeroCom phase III BB emission experiment. By comparing multi-model simulations and satellite observations in the vicinity of fires over 13 regions globally, we (1) assess model-simulated BB AOD performance as an indication of smoke source–strength, (2) identify regions where the common emission dataset used by the models might underestimate or overestimate smoke sources, and (3) assess model diversity and identify underlying causes as much as possible. Using satellite-derived AOD snapshots to constrain source strength works best where BB smoke from active sources dominates background non-BB aerosol, such as in boreal forest regions and over South America and southern hemispheric Africa. The comparison is inconclusive where the total AOD is low, as in many agricultural burning areas, and where the background is high, such as parts of India and China. Many inter-model BB AOD differences can be traced to differences in values for the mass ratio of organic aerosol to organic carbon, the BB aerosol mass extinction efficiency, and the aerosol loss rate from each model. The results point to a need for increased numbers of available BB cases for study in some regions and especially to a need for more extensive regional-to-global-scale measurements of aerosol loss rates and of detailed particle microphysical and optical properties; this would both better constrain models and help distinguish BB from other aerosol types in satellite retrievals. More generally, there is the need for additional efforts at constraining aerosol source strength and other model attributes with multi-platform observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Particulate exhaust emissions from an experimental combustor

The concentration of dry particulates (carbon) in the exhaust of an experimental gas turbine combustor was measured at simulated takeoff operating conditions and correlated with the standard smoke-number measurement. Carbon was determined quantitatively from a sample collected on a fiberglass filter by converting the carbon in the smoke sample to carbon dioxide and then measuring the volume of carbon dioxide formed by gas chromatography. At a smoke of 25 (threshold of visibility of the smoke plume for large turbojets) the carbon concentration was 2.8 mg carbon/cu m exhaust gas, which is equivalent to an emission index of 0.17 g carbon/kg fuel.

Norgren, C. T.↗

Combustor exhaust emissions with air-atomizing splash-groove fuel injectors burning Jet A and Diesel number 2 fuels

Air-atomizing, splash-groove injectors were shown to improve primary-zone fuel spreading and reduce combustor exhaust emissions for Jet A and diesel number 2 fuels. With Jet A fuel large-orifice, splash-groove injectors the oxides-of-nitrogen emission index was reduced, but emissions of carbon monoxide, unburned hydrocarbons, or smoke were unaffected. Small-orifice, splash-groove injectors did not reduce oxides of nitrogen, but reduced the smoke number and carbon monoxide and unburned-hydrocarbon emission indices. With diesel number 2 fuel, the small-orifice, splash-groove injectors reduced oxides of nitrogen by 19 percent, smoke number by 28 percent, carbon monoxide by 75 percent, and unburned hydrocarbons by 50 percent. Smoke number and unburned hydrocarbons were twice as high with diesel number 2 as with Jet A fuel. Combustor blowout limits were similar for diesel number 2 and Jet A fuels.

Ingebo, R. D.↗

Satellite detection of air pollutants

NASA's ERTS-1 satellite, with its high resolution and multispectral capabilities, has been found useful in the detection and analysis of smoke from large point sources (power plants, steel mills, etc.), and widespread atmospheric turbidity associated with atmospheric stagnations. Smoke plumes from the Chicago-Northern Indiana industrial complex have been tracked over Lake Michigan for over 100 km. Experience has shown that smoke plumes are relatively easy to detect over water (in the 0.6-0.7 micrometer band) but much more difficult over land surfaces. Pattern recognition techniques (cluster analysis) were applied to the digital ERTS data, and it was found that the smoke plumes indeed had a unique spectral signature. Studies are currently underway to use measured plume geometries to obtain quantitative estimates of diffusion over water surfaces.

Lyons, W. A.↗

Effect of primary-zone equivalence ratio on pollutant formation

Test were conducted to determine the effect of primary-zone equivalence ratio on the formation of smoke and other gaseous pollutants in an experimental can combustor. Several fuel injection techniques were examined at primary-zone equivalence ratios from 0.8 to 2.0. The main emphasis was on reducing fuel-rich-combustion smoke levels. Two of the four fuel injection configurations studied produced smoke levels below a smoke number of 20 at a primary-zone equivalence ratio of about 1.7. As the fuel mixing and atomization were recorded at primary-zone equivalence ratios as high as 2.0. The gaseous emissions of unburned hydrocarbons, carbon monoxide, and oxides of nitrogen were quite sensitive to the fuel injection configuration as well as to the primary-zone equilvalence ratio.

Claus, R. W.↗

Low NOx heavy fuel combustor concept program addendum: Low/mid heating value gaseous fuel evaluation

The combustion performance of a rich/quench/lean (RQL) combustor was evaluated when operated on low and mid heating value gaseous fuels. Two synthesized fuels were prepared having lower heating values of 10.2 MJ/cu m. (274 Btu/scf) and 6.6 MJ/cu m (176 Btu/scf). These fuels were configured to be representative of actual fuels, being composed primarily of nitrogen, hydrogen, carbon monoxide, and carbon dioxide. A liquid fuel air assist fuel nozzle was modified to inject both of the gaseous fuels. The RQL combustor liner was not changed from the configuration used when the liquid fuels were tested. Both gaseous fuels were tested over a range of power levels from 50 percent load to maximum rated power of the DDN Model 570-K industrial gas turbine engine. Exhaust emissions were recorded for four power level at several rich zone equivalence ratios to determine NOx sensitivity to the rich zone operating point. For the mid Btu heating value gas, ammonia was added to the fuel to simulate a fuel bound nitrogen type gaseous fuel. Results at the testing showed that for the low heating value fuel NOx emissions were all below 20 ppmc and smoke was below a 10 smoke number. For the mid heating value fuel, NOx emissions were in the 50 to 70 ppmc range with the smoke below a 10 smoke number.

Novick, A. S.↗

Experimental studies of circumstellar, interstellar and interplanetary refractory grain analogs

Experimental techniques for studying the processes which occur during the life cycle of a refractory grain are reviewed. Consideration is given to the construction of a differentially-pumped beam-mass spectrometer which is expected to determine the relative stability of small clusters in the Fe-Mg-Si-O and Ca-Ti-Al-O systems as a function of temperature and pressure. Also, a smoke generator has been constructed to produce gram quantities of amorphous grains for use in thermal annealing and hydrous alteration studies of smokes containing Fe-Mg-Al-Ti-Ca-Si-O and Cl. Topics of the studies include the properties of grains produced in a flow condensation apparatus, the sorption efficiency of Si2O3 smokes for AR gas, the processing of ices containing refractory precursors such as SiH4 or Fe(CO)5 plus water, and the residue from 1 MeV bombardment and warming of an amorphous Fe-SiO smoke.

Nuth, J. A.↗

The Kuwait oil fires as seen by Landsat

A mosaic of two Landsat thematic mapper images acquired May 30, 1991, reveals a dark smoke plume 30-60 km wide extending hundreds of kilometers south of Kuwait City along the Persian Gulf. Smoke coming from the Raudhatain and Sabriyah oil fields blew across the Gulf of Kuwait and over Kuwait City, joined with smoke from the Greater Burgan and Minagish fields, and continued southward over smaller villages and regions of desert agriculture consisting of hundreds of axially irrigated fields in both Kuwait and Saudi Arabia. One agricultural region in Kuwait was completely obscured by the smoke. The light colored limestone gravel and sand surface was darkened by oil lakes near the wells, and by oil drizzling out of the plume downwind of the wells. Most fires produced either a light or dark plume, and the separate plumes mixed to form a combined plume much darker than the land surface, but slightly more reflective than the Gulf waters. A few of the hottest fires had no visible plume, and are presumably associated with methane combustion. The last of the Kuwait fires was reportedly extinguished in November of 1991. Continued monitoring is needed to assess the impact of emissions from both burning and nonburning oil wells on the region's climate, as well as on the agriculture, fishing, and other activities essential to life in the region.

Cahalan, Robert F.↗

Thermal degradation of polytetrafluoroethylene in tube reactors

We have studied the thermal degradation of polytetrafluoroethylene (PTFE) in wet air, dry air and nitrogen gas at temperatures ranging from 310 to 520 C. The principal gas product was tetrafluoroethylene (TFE). The nitrogen experiments yielded only TFE, but experiments in dry and wet air also produced several other minor gas products. The dry air experiments produced the most smoke and the least gas products, with the nitrogen experiments giving no smoke and the highest amounts of gas products. Wet air experiments gave intermediate results for smoke and gas formation. The rate of degradation in wet air showed an apparent activation energy of 103 kca/mol. We also performed FTIR analyses of the smoke particulate, determining that the particulate formed in dry air is different than that formed in wet air.

Mckinnon, J. Thomas↗

Characterization of Aircraft Produced Soot and Contrails Near the Tropopause

Participation in the SUCCESS project primarily involved development and deployment of specific instruments for characterizing jet aircraft exhaust emissions as particulates and their subsequent evolution as contrail particles, either liquid or solid, as cirrus. Observations can be conveniently considered in two categories - close or distant from the aircraft. Thus close to the aircraft the exhaust is mixing through the engine turbulence with a much drier and colder environment and developing water/ ice supersaturation along the trail depending on circumstances (near field), whereas distant from the aircraft (far field) the exhaust has cooled essentially to ambient temperature, the turbulence has decayed and any particle growth or evaporation is controlled by the prevailing ambient conditions. Intermediate between these two regions the main aircraft vortices form (one on each side of the aircraft) which tend to inhibit mixing under some conditions, a region extending from a few aircraft lengths to sometimes a hundred times this distance. Our approach to the problem lay in experience gained in characterizing the smoke from hydrocarbon combustion in terms of its cloud forming properties and its potential influence on the radiation properties of the smoke and subsequent cloud from the viewpoint of reduction (absorbtion and scattering ) of solar radiation flux leading to significant global cooling (Hudson et al 1991; Hallett and Hudson 1991). Engine exhaust contains a much smaller proportion of the fuel carbon than is sometimes present in ordinary combustion (less than 0.01% compared with 10%) and influences condensation in quite different ways, to be characterized by the Cloud Condensation Nucleus, CCN - supersaturation spectrum. The transition to ice is to be related to the dilution of solution droplets to freeze by homogeneous nucleation at temperatures somewhat below -40C (Pueschel et al 1998). The subsequent growth of ice particles depends critically on temperature, supersaturation and to some extent pressure, as is demonstrated in an NSF funded project being carried out in parallel with the work reported here. As will be discussed below, nucleation processes themselves and also exhaust impurities also influence the growth of ice particles and may control some aspects of growth of ice in contrails. Instrumentation was designed to give insight into these questions and to be flown on the NASA DC- 8 as a platform. In addition a modest program was undertaken to investigate the properties of laboratory produced smoke produced under controlled conditions from the viewpoint of forming both CCN and CN. The composition of the smoke could inferred from a thermal characterization technique; larger particles were captured by formvar replicator for detailed analysis; ice particles were captured and evaporated in flight on a new instrument, the cloudscope, to give their mass, density and impurity content.

Hallett, John↗

How Well Will MODIS Measure Top of Atmosphere Aerosol Direct Radiative Forcing?

The new generation of satellite sensors such as the Moderate Resolution Imaging Spectroradiometer (MODIS) will be able to detect and characterize global aerosols with an unprecedented accuracy. The question remains whether this accuracy will be sufficient to narrow the uncertainties in our estimates of aerosol radiative forcing at the top of the atmosphere. Satellite remote sensing detects aerosol optical thickness with the least amount of relative error when aerosol loading is high. Satellites are less effective when aerosol loading is low. We use the monthly mean results of two global aerosol transport models to simulate the spatial distribution of smoke aerosol in the Southern Hemisphere during the tropical biomass burning season. This spatial distribution allows us to determine that 87-94% of the smoke aerosol forcing at the top of the atmosphere occurs in grid squares with sufficient signal to noise ratio to be detectable from space. The uncertainty of quantifying the smoke aerosol forcing in the Southern Hemisphere depends on the uncertainty introduced by errors in estimating the background aerosol, errors resulting from uncertainties in surface properties and errors resulting from uncertainties in assumptions of aerosol properties. These three errors combine to give overall uncertainties of 1.5 to 2.2 Wm-2 (21-56%) in determining the Southern Hemisphere smoke aerosol forcing at the top of the atmosphere. The range of values depend on which estimate of MODIS retrieval uncertainty is used, either the theoretical calculation (upper bound) or the empirical estimate (lower bound). Strategies that use the satellite data to derive flux directly or use the data in conjunction with ground-based remote sensing and aerosol transport models can reduce these uncertainties.

Remer, Lorraine A.↗

Flame Shapes of Nonbuoyant Laminar Jet Diffusion Flames

The shapes (flame-sheet and luminous-flame boundaries) of steady nonbuoyant round hydrocarbon-fueled laminar-jet diffusion flames in still and coflowing air were studied both experimentally and theoretically. Flame-sheet shapes were measured from photographs using a CH optical filter to distinguish flame-sheet boundaries in the presence of blue C02 and OH emissions and yellow continuum radiation from soot. Present experimental conditions included acetylene-, methane-, propane-, and ethylene-fueled flames having initial reactant temperatures of 300 K, ambient pressures of 4-50 kPa, jet exit Reynolds number of 3-54, initial air/fuel velocity ratios of 0-9 and luminous flame lengths of 5-55 mm; earlier measurements for propylene- and 1,3-butadiene-fueled flames for similar conditions were considered as well. Nonbuoyant flames in still air were observed at micro-gravity conditions; essentially nonbuoyant flames in coflowing air were observed at small pressures to control effects of buoyancy. Predictions of luminous flame boundaries from soot luminosity were limited to laminar smoke-point conditions, whereas predictions of flame-sheet boundaries ranged from soot-free to smoke-point conditions. Flame-shape predictions were based on simplified analyses using the boundary layer approximations along with empirical parameters to distinguish flame-sheet and luminous-flame (at the laminar smoke point) boundaries. The comparison between measurements and predictions was remarkably good and showed that both flame-sheet and luminous-flame lengths are primarily controlled by fuel flow rates with lengths in coflowing air approaching 2/3 lengths in still air as coflowing air velocities are increased. Finally, luminous flame lengths at laminar smoke-point conditions were roughly twice as long as flame-sheet lengths at comparable conditions due to the presence of luminous soot particles in the fuel-lean region of the flames.

Xu, F.↗

MODIS Observation of Aerosols over Southern Africa During SAFARI 2000: Data, Validation, and Estimation of Aerosol Radiative Forcing

Aerosol properties, including optical thickness and size parameters, are retrieved operationally from the MODIS sensor onboard the Terra satellite launched on 18 December 1999. The predominant aerosol type over the Southern African region is smoke, which is generated from biomass burning on land and transported over the southern Atlantic Ocean. The SAFARI-2000 period experienced smoke aerosol emissions from the regular biomass burning activities as well as from the prescribed burns administered on the auspices of the experiment. The MODIS Aerosol Science Team (MAST) formulates and implements strategies for the retrieval of aerosol products from MODIS, as well as for validating and analyzing them in order to estimate aerosol effects in the radiative forcing of climate as accurately as possible. These activities are carried out not only from a global perspective, but also with a focus on specific regions identified as having interesting characteristics, such as the biomass burning phenomenon in southern Africa and the associated smoke aerosol, particulate, and trace gas emissions. Indeed, the SAFARI-2000 aerosol measurements from the ground and from aircraft, along with MODIS, provide excellent data sources for a more intensive validation and a closer study of the aerosol characteristics over Southern Africa. The SAFARI-2000 ground-based measurements of aerosol optical thickness (AOT) from both the automatic Aerosol Robotic Network (AERONET) and handheld Sun photometers have been used to validate MODIS retrievals, based on a sophisticated spatio-temporal technique. The average global monthly distribution of aerosol from MODIS has been combined with other data to calculate the southern African aerosol daily averaged (24 hr) radiative forcing over the ocean for September 2000. It is estimated that on the average, for cloud free conditions over an area of 9 million square kin, this predominantly smoke aerosol exerts a forcing of -30 W/square m C lose to the terrestrial surface and -10 W/square m at the top of the atmosphere (TOA). While cooling the surface and Earth system, the difference of 20 W/square m is energy that heats the atmosphere.

Ichoku, Charles↗