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Clarke, A. D.

Publications and source records attributed to Clarke, A. D..

Emissions from Biomass Burning in the Yucatan

In March 2006 two instrumented aircraft made the first detailed field measurements of biomass burning (BB) emissions in the Northern Hemisphere tropics as part of the MILAGRO project. The aircraft were the National Center for Atmospheric Research C-130 and a University of Montana/US Forest Service Twin Otter. The initial emissions of up to 49 trace gas or particle species were measured from 20 deforestation and crop residue fires on the Yucatan peninsula. This included two trace gases useful as indicaters of BB (HCN and acetonitrile) and several rarely, or never before, measured species: OH, peroxyacetic acid, propanoic acid, hydrogen peroxide, methane sulfonic acid, and sulfuric acid. Crop residue fires emitted more organic acids and ammonia than deforestation fires, but the emissions from the main fire types were otherwise fairly similar. The Yucatan fires emitted unusually amounts of SO2 and particle chloride, likely due to a strong marine influence on the peninsula.

Yokelson, R.↗

Characteristics and Influence of Biosmoke on the Fine-Particle Ionic Composition Measured in Asian Outflow during the Transport and Chemical Evolution Over the Pacific (TRACE-P) Experiment

We investigate the sources, prevalence, and fine-particle inorganic composition of biosmoke over the western Pacific Ocean between 24 February and 10 April 2001. The analysis is based on highly time-resolved airborne measurements of gaseous and fine- particle inorganic chemical composition made during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) experiment. At latitudes below approximately 25 deg. N, relatively pure biomass burning plumes of enhanced fine-particle potassium, nitrate, ammonium, light-absorbing aerosols, and CO concentrations were observed in plumes that back trajectories and satellite fire map data suggest originated from biomass burning in southeast Asia. Fine-particle water-soluble potassium (K+) is confirmed to be a unique biosmoke tracer, and its prevalence throughout the experiment indicates that approximately 20% of the TRACE-P Asian outflow plumes were influenced, to some extent, by biomass or biofuel burning emissions. At latitudes above 25 deg. N, highly mixed urban/industrial and biosmoke plumes, indicated by SO(sup 2, sub 4) and K+, were observed in 5 out of 53 plumes. Most plumes were found in the Yellow Sea and generally were associated with much higher fine-particle loadings than plumes lacking a biosmoke influence. The air mass back trajectories of these mixed plumes generally pass through the latitude range of between 34 deg. and 40 deg. N on the eastern China coast, a region that includes the large urban centers of Beijing and Tianjin. A lack of biomass burning emissions based on fire maps and high correlations between K+ and pollution tracers (e.g., S(sup 2, sub 4) suggest biofuel sources. Ratios of fine-particle potassium to sulfate are used to provide an estimate of relative contributions of biosmoke emissions to the mixed Asian plumes. The ratio is highly correlated with fine-particle volume (r(sup 2) = 0.85) and predicts that for the most polluted plume encounter in TRACE-P, approximately 60% of the plume is associated with biosmoke emissions. On average, biosmoke contributes approximately 35-40% to the measured fine inorganic aerosol mass in the mixed TRACE-P plumes intercepted north of 25% latitude.

Ma, Y.↗

New Particle Formation in Anthropogenic Plumes Advecting from Asia Observed During TRACE-P

The characteristics and sources of what are believed to be newly formed 3 to 4 nm particles in anthropogenic plumes advecting from Asian are reported. Airborne measurements were made from March to April 2001 as part of the NASA TRACE-P experiment at latitudes ranging from North of the Philippines to Northern Japan (20 to 45 deg. N). In the more polluted plumes, high concentrations of 3 to 4 nm diameter particles (less than 100/qu cm) were observed both within and along the upper outer edges of plumes that were identified by enhanced carbon monoxide and fine particulate sulfate concentrations. The results from two research flights are investigated in detail. Three to four-nm particle concentrations are generally correlated with gas phase sulfuric acid and found in regions of low surface areas relative to the immediate surroundings or where there are steep transitions to lower surface areas. Sulfuric acid and surface area concentrations in the most polluted plume reached 6 x l0(exp 7) and 750 micro sq m/qu cm, respectively, in regions of particle formation. In contrast to these anthropogenic plumes, few 3 to 4 nm particles were observed in the clean background and few were detected within a volcanic plume where the studies highest H2SO4 concentrations (less than lO(exp 8)/qu cm) were recorded. Enhanced SO2 concentrations in the range of approximately 2 to 7 ppb, in conjunction with other unidentified, possibly coemitted species, appear to be the driving factor for nucleation. (0345, 4801); 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 0345 Atmospheric Composition and Structure: Pollution-urban and regional (0305); 4801 Oceanography: Biological and Chemical: Aerosols (0305).

Weber, R. J.↗

Backscatter Modeling at 2.1 Micron Wavelength for Space-Based and Airborne Lidars Using Aerosol Physico-Chemical and Lidar Datasets

Space-based and airborne coherent Doppler lidars designed for measuring global tropospheric wind profiles in cloud-free air rely on backscatter, beta from aerosols acting as passive wind tracers. Aerosol beta distribution in the vertical can vary over as much as 5-6 orders of magnitude. Thus, the design of a wave length-specific, space-borne or airborne lidar must account for the magnitude of 8 in the region or features of interest. The SPAce Readiness Coherent Lidar Experiment under development by the National Aeronautics and Space Administration (NASA) and scheduled for launch on the Space Shuttle in 2001, will demonstrate wind measurements from space using a solid-state 2 micrometer coherent Doppler lidar. Consequently, there is a critical need to understand variability of aerosol beta at 2.1 micrometers, to evaluate signal detection under varying aerosol loading conditions. Although few direct measurements of beta at 2.1 micrometers exist, extensive datasets, including climatologies in widely-separated locations, do exist for other wavelengths based on CO2 and Nd:YAG lidars. Datasets also exist for the associated microphysical and chemical properties. An example of a multi-parametric dataset is that of the NASA GLObal Backscatter Experiment (GLOBE) in 1990 in which aerosol chemistry and size distributions were measured concurrently with multi-wavelength lidar backscatter observations. More recently, continuous-wave (CW) lidar backscatter measurements at mid-infrared wavelengths have been made during the Multicenter Airborne Coherent Atmospheric Wind Sensor (MACAWS) experiment in 1995. Using Lorenz-Mie theory, these datasets have been used to develop a method to convert lidar backscatter to the 2.1 micrometer wavelength. This paper presents comparison of modeled backscatter at wavelengths for which backscatter measurements exist including converted beta (sub 2.1).

Srivastava, V.↗

Intercomparison of Pulsed Lidar Data with Flight Level CW Lidar Data and Modeled Backscatter from Measured Aerosol Microphysics Near Japan and Hawaii

Aerosol backscatter coefficient data were examined from two nights near Japan and Hawaii undertaken during NASA's Global Backscatter Experiment (GLOBE) in May-June 1990. During each of these two nights the aircraft traversed different altitudes within a region of the atmosphere defined by the same set of latitude and longitude coordinates. This provided an ideal opportunity to allow flight level focused continuous wave (CW) lidar backscatter measured at 9.11-micron wavelength and modeled aerosol backscatter from two aerosol optical counters to be compared with pulsed lidar aerosol backscatter data at 1.06- and 9.25-micron wavelengths. The best agreement between all sensors was found in the altitude region below 7 km, where backscatter values were moderately high at all three wavelengths. Above this altitude the pulsed lidar backscatter data at 1.06- and 9.25-micron wavelengths were higher than the flight level data obtained from the CW lidar or derived from the optical counters, suggesting sample volume effects were responsible for this. Aerosol microphysics analysis of data near Japan revealed a strong sea-salt aerosol plume extending upward from the marine boundary layer. On the basis of sample volume differences, it was found that large particles were of different composition compared with the small particles for low backscatter conditions.

Cutten, D. R.↗

Distribution of Halon-1211 in the Upper Troposphere and Lower Stratosphere and the 1994 Total Bromine Budget

We report here on the details of the first, in situ, real-time measurements of H-1211 (CBrClF2) and sulfur hexafluoride (SF6) mixing ratios in the stratosphere up to 20 km. Stratospheric air was analyzed for these gases and others with a new gas chromatograph, flown aboard a National Aeronautics and Space Administration ER-2 aircraft as part of the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft mission conducted in 1994. The mixing ratio of SF6, with its nearly linear increase in the troposphere, was used to estimate the mean age of stratospheric air parcels along the ER-2 flight path. Measurements of H-1211 and mean age estimates were then combined with simultaneous measurements of CFC-11 (CCl3F), measurements of brominated compounds in stratospheric whole air samples, and records of tropospheric organic bromine mixing ratios to calculate the dry mixing ratio of total bromine in the lower stratosphere and its partitioning between organic and inorganic forms. We estimate that the organic bromine-containing species were almost completely photolyzed to inorganic species in the oldest air parcels sampled. Our results for inorganic bromine are consistent with those obtained from a photochemical, steady state model for stratospheric air parcels with CFC- I I mixing ratios greater than 150 ppt. For stratospheric air parcels with CFC-11 mixing ratios less than 50 ppt (mean age greater than or equal to 5 years) we calculate inorganic bromine mixing ratios that are approximately 20% less than the photo-chemical, steady state model. There is a 20% reduction in calculated ozone loss resulting from bromine chemistry in old air relative to some previous estimates as a result of the lower bromine levels.

Wamsley, P. R.↗

Intercomparison of Remote and Flight Level Measured Aerosol Backscatter Coefficient During GLOBE 2 Pacific Survey Mission

Aerosol backscatter coefficient data are examined from two local flights undertaken during NASA's GLObal Backscatter Experiment (GLOBE) in May - June, 1990. During each of these two flights the aircraft traversed different altitudes within a region of the atmosphere defined by the same set of latitude and longitude coordinates. This provides an ideal opportunity to allow flight level measured or modeled aerosol backscafter to be compared with pulsed lidar aerosol backscafter data that were obtained at these same altitudes either earlier or later than the flight level measurements. Aerosol backscafter comparisons were made at 1.06-, 9.11- and 9.25-mm wavelengths, using data from three lidar systems and two aerosol optical counters. The best agreement between all sensor's was found in the altitude region below 7 km where backscafter values were moderately high at all three wavelengths. Above this altitude the pulsed lidar backscafter data at 1.06- and 9.25-mm wavelengths were higher than the flight level data obtained from the CW lidar or derived from the optical counters. Possible reasons are offered to explain this discrepancy. During the Japan local flight, microphysics analysis revealed: (1) evidence of a strong advected seasalt aerosol plume from the marine boundary layer, and (2) where backscatter was low, the large lidar sampling volume included many large particles which were of different chemical composition to the small particle category sampled by the particle counters.

Cutten, D. R.↗

Multiwavelength Comparison of Modeled and Measured Remote Tropospheric Aerosol Backscatter Over Pacific Ocean

Aerosol concentrations and size distributions in the middle and upper troposphere over the remote Pacific Ocean were measured with a forward scattering spectrometer probe (FSSP) on the NASA DC-8 aircraft during NASA's Global Backscatter Experiment (GLOBE) in May-June 1990. The FSSP size channels were recalibrated based on refractive index estimates from flight-level aerosol volatility measurements with a collocated laser optical particle counter (LOPC). The recalibrated FSSP size distributions were averaged over 100-s intervals, fitted with lo-normal distributions and used to calculate aerosol backscatter coefficients at selected wavelengths. The FSSP-derived backscatter estimates were averaged over 300-s intervals to reduce large random fluctuations. The smoothed FSSP aerosol backscatter coefficients were then compared with LOPC-derived backscatter values and with backscatter measured at or near flight level from four lidar systems operating at 0.53, 1.06, 9.11, 9.25, and 10.59 micrometers. Agreement between FSSP-derived and lidar-measured backscatter was generally best at flight level in homogeneous aerosol fields and at high backscatter values. FSSP data often underestimated low backscatter values especially at the longer wavelengths due to poor counting statistics for larger particles (greater than 0.8 micrometers diameter) that usually dominate aerosol backscatter at these wavelengths. FSSP data also underestimated backscatter at shorter wavelengths when particles smaller than the FSSP lower cutoff diameter (0.35 micrometers) made significant contributions to the total backscatter.

Cutten, D. R.↗

Aircraft studies of size-dependent aerosol sampling through inlets

Representative measurement of aerosol from aircraft-aspirated systems requires special efforts in order to maintain near isokinetic sampling conditions, estimate aerosol losses in the sample system, and obtain a measurement of sufficient duration to be statistically significant for all sizes of interest. This last point is especially critical for aircraft measurements which typically require fast response times while sampling in clean remote regions. This paper presents size-resolved tests, intercomparisons, and analysis of aerosol inlet performance as determined by a custom laser optical particle counter. Measurements discussed here took place during the Global Backscatter Experiment (1988-1989) and the Central Pacific Atmospheric Chemistry Experiment (1988). System configurations are discussed including (1) nozzle design and performance, (2) system transmission efficiency, (3) nonadiabatic effects in the sample line and its effect on the sample-line relative humidity, and (4) the use and calibration of a virtual impactor.

Porter, J. N.↗

Measurements of the light-absorbing material inside cloud droplets and its effect on cloud albedo

Most of the measurements of light-absorbing aerosol particles made previously have been in non-cloudy air and therefore provide no insight into aerosol effects on cloud properties. Here, researchers describe an experiment designed to measure light absorption exclusively due to substances inside cloud droplets, compare the results to related light absorption measurements, and evaluate possible effects on the albedo of clouds. The results of this study validate those of Twomey and Cocks and show that the measured levels of light-absorbing material are negligible for the radiative properties of realistic clouds. For the measured clouds, which appear to have been moderately polluted, the amount of elemental carbon (EC) present was insufficient to affect albedo. Much higher contaminant levels or much larger droplets than those measured would be necessary to significantly alter the radiative properties. The effect of the concentrations of EC actually measured on the albedo of snow, however, would be much more pronounced since, in contrast to clouds, snowpacks are usually optically semi-infinite and have large particle sizes.

Twohy, C. H.↗

Stratospheric aerosol light absorption before and after El Chichon

Direct in-situ measurements of aerosol light absorption before, during, and after the eruption of Mt. St. Helens and El Chichon reveal the presence of light absorbing species at all times. Large enhancements which appear to drop rapidly with time are found at certain locations immediately following volcanic events. Although a general patchiness is present in the aerosol and its associated absorption coefficient, post eruption values appear to remain elevated in the mean when compared to early 1979 data prior to the El Chichon eruption. From the data collected for this period, lower bounds for the single scatter albedo are presented along with implications for associated radiative effects.

Clarke, A. D.↗

Measurements of the absorption coefficient of stratospheric aerosols

The absorption coefficients of stratospheric aerosols are measured using a variation on the integrating plate method. The technique is based on the decrease in the transparency of a substrate when an absorbing aerosol is deposited on it. A Lambert scatterer is placed behind the substrate to integrate forward scattered light and minimize the effect of scattering on the measurement. The low pressure in the stratosphere is used for the direct impaction of particles onto a narrow strip of opal glass. The eight samples collected had a median value of 4 x 10 to the -9th m with an uncertainty of + or - 5 x 10 to the -9th m. If this absorption is due to graphitic carbon, then its concentration is estimated at about 0.4 ng/cu m, or about 0.25% of the total aerosol mass concentration. Estimates of the aerosol scattering coefficients based on satellite extinction inversions result in an aerosol single-scattering albedo in the range of 0.96-1.0.

Ogren, J. A.↗