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Clarke, Antony D.

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

Formaldehyde Distribution over North America: Implications for Satellite Retrievals of Formaldehyde Columns and Isoprene Emission

Formaldehyde (HCHO) columns measured from space provide constraints on emissions of volatile organic compounds (VOCs). Quantitative interpretation requires characterization of errors in HCHO column retrievals and relating these columns to VOC emissions. Retrieval error is mainly in the air mass factor (AMF) which relates fitted backscattered radiances to vertical columns and requires external information on HCHO, aerosols, and clouds. Here we use aircraft data collected over North America and the Atlantic to determine the local relationships between HCHO columns and VOC emissions, calculate AMFs for HCHO retrievals, assess the errors in deriving AMFs with a chemical transport model (GEOS-Chem), and draw conclusions regarding space-based mapping of VOC emissions. We show that isoprene drives observed HCHO column variability over North America; HCHO column data from space can thus be used effectively as a proxy for isoprene emission. From observed HCHO and isoprene profiles we find an HCHO molar yield from isoprene oxidation of 1.6 +/- 0.5, consistent with current chemical mechanisms. Clouds are the primary error source in the AMF calculation; errors in the HCHO vertical profile and aerosols have comparatively little effect. The mean bias and 1Q uncertainty in the GEOS-Chem AMF calculation increase from <1% and 15% for clear skies to 17% and 24% for half-cloudy scenes. With fitting errors, this gives an overall 1 Q error in HCHO satellite measurements of 25-31%. Retrieval errors, combined with uncertainties in the HCHO yield from isoprene oxidation, result in a 40% (1sigma) error in inferring isoprene emissions from HCHO satellite measurements.

Millet, Dylan B.↗

Comparison of Modeled Backscatter using Measured Aerosol Microphysics with Focused CW Lidar Data over Pacific

During NASA's GLObal Backscatter Experiment (GLOBE) II flight mission over the Pacific Ocean in May-June 1990, extensive aerosol backscatter data sets from two continuous wave, focused CO2 Doppler lidars and an aerosol microphysics data set from a laser optical particle counter (LOPC) were obtained. Changes in aerosol loading in various air masses with associated changes in chemical composition, from sulfuric acid and sulfates to dustlike crustal material, significantly affected aerosol backscatter, causing variation of about 3 to 4 orders of magnitude. Some of the significant backscatter features encountered in different air masses were the low backscatter in subtropical air with even lower values in the tropics near the Intertropical Convergence Zone (ITCZ), highly variable backscatter in the ITCZ, mid-tropospheric aerosol backscatter background mode, and high backscatter in an Asian dust plume off the Japanese coast. Differences in aerosol composition and backscatter for northern and southern hemisphere also were observed. Using the LOPC measurements of physical and chemical aerosol properties, we determined the complex refractive index from three different aerosol mixture models to calculate backscatter. These values provided a well-defined envelope of modeled backscatter for various atmospheric conditions, giving good agreement with the lidar data over a horizontal sampling of approximately 18000 km in the mid-troposphere.

Srivastava, Vandana↗

Remote Marine Aerosol: A Characterization of Physical, Chemical and Optical Properties and their Relation to Radiative Transfer in the Troposphere

Our research effort is focused on improving our understanding of aerosol properties needed for optical models for remote marine regions. This includes in-situ and vertical column optical closure and involves a redundancy of approaches to measure and model optical properties that must be self consistent. The model is based upon measured in-situ aerosol properties and will be tested and constrained by the vertically measured spectral differential optical depth of the marine boundary layer, MBL. Both measured and modeled column optical properties for the boundary layer, when added to the free-troposphere and stratospheric optical depth, will be used to establish spectral optical depth over the entire atmospheric column for comparison to and validation of satellite derived radiances (AVHRR).

Clarke, Antony D.↗

Atmospheric nuclei in the Pacific midtroposphere: Their nature, concentration, and evolution

An extensive flight series was carried out during May-June 1990 in the remote North and South Pacific free tropospheric aboard the NASA DC-8. Condensation nuclei counters and optical particle counters provided information on aerosol particles with diameters between 0.003 and 7.0 micrometers. Vertical profiles revealed aerosol layers to be a common feature of the free troposphere. Regions with highest aerosol mass tended to have the highest concentrations of surface-derived nuclei but the lowest concentrations of total nuclei. Regions with lowest aerosol mass tended to have the highest concentrations of the smaller 'ultrafine' condensation nuclei with diameters below 0.02 mircometers. Horizontal transects totaling over 35,000 km at about 9 to 10-km altitude exhibited variability of approximately 3 orders of magnitude in both aerosol mass and number concentrations over spatial scales ranging from 1 to 1000 km. At these altitudes an approximate inverse relationship between ultrafine concentrations and the surface area of the larger aerosol was evident. Regions having lowest aerosol mass were characterized by aerosol thermal volatility, indicative of a predominately sulfuric acid composition, and by very high concentrations of ultrafine nuclei, indicative of recent homogeneous nucleation. These conditions were frequently observed but were conspicuously evident above cloud over the intertropical convergence zone. The clean, free troposphere appears to be a significant source region for new tropospheric nuclei. A simplified model of the lifetime, coagulation, and cycling of these nuclei suggests that they constitute a source of cloud condensation nuclei in the lower troposphere.

Clarke, Antony D.↗

Aerosol chemistry in GLOBE

This task addresses the measurement and understanding of the physical and chemical properties of aerosol in remote regions that are responsible for aerosol backscatter at infrared wavelengths. Because it is representative of other clean areas, the remote Pacific is of extreme interest. Emphasis is on the determination size dependent aerosol properties that are required for modeling backscatter at various wavelengths and upon those features that may be used to help understand the nature, origin, cycling and climatology of these aerosols in the remote troposphere. Empirical relationships will be established between lidar measurements and backscatter derived from the aerosol microphysics as required by the NASA Doppler Lidar Program. This will include the analysis of results from the NASA GLOBE Survey Mission Flight Program. Additional instrument development and deployment will be carried out in order to extend and refine this data base. Identified activities include participation in groundbased and airborne experiments. Progress to date includes participation in, analysis of, and publication of results from Mauna Loa Backscatter Intercomparison Experiment (MABIE) and Global Backscatter Experiment (GLOBE).

Clarke, Antony D.↗

Atmospheric nuclei in the remote free-troposphere

An extensive flight series to survey aerosol present in the upper-troposphere was undertaken aboard the NASA DC-8 as part of the Global Backscatter Experiment. Aerosol with diameters greater than 3 nm were counted and sized with a combination of condensation nuclei counters and optical particle counters. Aerosol number and mass concentrations were separately identified with regard to both refractory and volatile components. Regions of the free-troposphere with the lowest mass concentrations were generally found to have the highest number concentrations and appeared to be effective regions for new particle production. These new particle concentrations appear inversely related to available aerosol surface area, and their volatility suggests a sulfuric acid composition. The long lifetime of these new particles aloft can result in their growth to sizes effective as CN and CCN that can be mixed throughout the troposphere.

Clarke, Antony D.↗

Aerosol size distribution, composition, and CO2 backscatter

The aerosol size distribution, composition, and CO2 backscatter at 10.6 microns (beta-CO2) were measured continuosly at the Mauna Loa Observatory (Hawaii) during January-March and November-December, 1988 periods to compare the characteristics of periods associated with appreciable Asian dust transport to that site (January-March) with those of periods characterized by low-dust condition. The aerosol size distribution in the range 0.15 micron to 7.6 microns was measured at temperatures of 40, 150, and 340 C to differentiate between volatile and nonvolatile aerosols. Large ranges of variability was found in measurements of aerosol size distribution during both periods, but the average distributions were similar for both the high-dust and the low-dust periods. However, values for beta-CO2 were more elevated (by about six times) during periods associated with active Asian dust transport to the observatory site than during the low-dust periods.

Clarke, Antony D.↗

Comparison of CO2 backscatter using Mie theory from aerosol measurements over Pacific Basin with lidar data

Results of a comparison of aerosol backscatter with measurements over the Pacific Basin obtained from the CW CO2 lidars are presented. Both the Laser Optical Particle Counter (POPC) and CW CO2 lidars performed measurements at the flight level close to the aircraft and measured the same air mass. From the number distributions measured during a flight over Tokyo in June 1990, the backscatter coefficient for each component is calculated by integrating the differential backscatter. Fifteen sets of number distributions measured by the LOPC during the flight are used to predict aerosol backscatter. The backscatter from microphysics of the aerosols obtained from the LOPC and from the lidar measurements are in good agreement. It is concluded that the size distribution and composition of the aerosols can change dramatically as a function of altitude and location. The magnitude of the aerosol backscatter can vary by over three orders of magnitude from clear air to an aerosol layer.

Srivastava, Vandana↗

Aerosol in the Pacific troposphere

The use of near real-time optical techniques is emphasized for the measurement of mid-tropospheric aerosol over the Central Pacific. The primary focus is on measurement of the aerosol size distribution over the range of particle diameters from 0.15 to 5.0 microns that are essential for modeling CO2 backscatter values in support of the laser atmospheric wind sounder (LAWS) program. The measurement system employs a LAS-X (Laser Aerosol Spectrometer-PMS, Boulder, CO) with a custom 256 channel pulse height analyzer and software for detailed measurement and analysis of aerosol size distributions. A thermal preheater system (Thermo Optic Aerosol Descriminator (TOAD) conditions the aerosol in a manner that allows the discrimination of the size distribution of individual aerosol components such as sulfuric acid, sulfates and refractory species. This allows assessment of the relative contribution of each component to the BCO2 signal. This is necessary since the different components have different sources, exhibit independent variability and provide different BCO2 signals for a given mass and particle size. Field activities involve experiments designed to examine both temporal and spatial variability of these aerosol components from ground based and aircraft platforms.

Clarke, Antony D.↗

Mauna Loa Aerosol Backscatter Intecomparison Experiment (MABIE)

Measurements of CO2 aerosol backscatter coefficients and other aerosol physicochemical properties were obtained in remote Pacific free tropospheric airmasses at the Mauna Loa Observatory in Hawaii. The experiment used an attenuated total reflection impactor (Johnson et al., 1983), a dispersive infrared spectrophotometer, and a high-resolution optical particle counter. Preliminary results suggest that sulfate compounds dominate background backscatter properties at CO2 wavelengths between 9 and 10 microns.

Bowdle, David A.↗