Philip A. Durkee

International Global Atmospheric Chemistry (IGAC) Project's First Aerosol Characterization Experiment (ACE 1): Overview

The southern hemisphere marine Aerosol Characterization Experiment (ACE 1) was the first of a series of experiments that will quantify the chemical and physical processes controlling the evolution and properties of the atmospheric aerosol relevant to radiative forcing and climate. The goals of this series of process studies are to reduce the overall uncertainty in the calculation of climate forcing by aerosols and to understand the multiphase atmospheric chemical system sufficiently to be able to provide a prognostic analysis of future radiative forcing and climate response. ACE 1, which was conducted from November 15 to December 14, 1995, over the southwest Pacific Ocean, south of Australia, quantified the chemical, physical, radiative, and cloud nucleating properties and furthered our understanding of the processes controlling the aerosol properties in this minimally polluted marine atmosphere. The experiment involved the efforts of scientists from 45 research institutes in 11 countries.

Effect of Ship-Stack Effluents on Cloud Reflectivity

Under stable meteorological conditions the effect of ship-stack exhaust on overlying clouds was detected in daytime satellite images as an enhancement in cloud reflectivity at 3.7 micrometers. The exhaust is a source of cloud-condensation nuclei that increases the number of cloud droplets while reducing droplet size. This reduction in droplet size causes the reflectivity at 3.7 micrometers to be greater than the levels for nearby noncontaminated clouds of similar physical characteristics. The increase in droplet number causes the reflectivity at 0.63 micrometer to be significantly higher for the contaminated clouds despite the likelihood that the exhaust is a source of particles that absorb at visible wavelengths. The effect of aerosols on cloud reflectivity is expected to have a larger influence on the earths albedo than that due to the direct scattering and absorption of sunlight by the aerosols alone.

Aerosol-Induced Radiative Flux Changes Off the United States Mid-Atlantic Coast: Comparison of Values Calculated from Sunphotometer and In Situ Data with Those Measured by Airborne Pyranometer

The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) measured a variety of aerosol radiative effects (including flux changes) while simultaneously measuring the chemical, physical, and optical properties of the responsible aerosol particles. Here we use TARFOX-determined aerosol and surface properties to compute shortwave radiative flux changes for a variety of aerosol situations, with midvisible optical depths ranging from 0.06 to 0.55. We calculate flux changes by several techniques with varying degrees of sophistication, in part to investigate the sensitivity of results to computational approach. We then compare computed flux changes to those determined from aircraft measurements. Calculations using several approaches yield downward and upward flux changes that agree with measurements. The agreement demonstrates closure (i.e., consistency) among the TARFOX-derived aerosol properties, modeling techniques, and radiative flux measurements. Agreement between calculated and measured downward flux changes is best when the aerosols are modeled as moderately absorbing (midvisible single-scattering albedos between about 0.89 and 0.93), in accord with independent measurements of the TARFOX aerosol. The calculated values for instantaneous daytime upwelling flux changes are in the range +14 to +48 W m−2 for midvisible optical depths between 0.2 and 0.55. These values are about 30 to 100 times the global-average direct forcing expected for the global-average sulfate aerosol optical depth of 0.04. The reasons for the larger flux changes in TARFOX include the relatively large optical depths and the focus on cloud-free, daytime conditions over the dark ocean surface. These are the conditions that produce major aerosol radiative forcing events and contribute to any global-average climate effect.

Processes controlling the distribution of aerosol particles in the lower marine boundary layer during the First Aerosol Characterization Experiment (ACE 1)

The goals of the International Global Atmospheric Chemistry (IGAC) Programs First Aerosol Characterization Experiment (ACE 1) are to determine and understand the properties and controlling factors of the aerosol in the remote marine atmosphere that are relevant to radiative forcing and climate. A key question in terms of this goal and the overall biogeochemical sulfur cycle is what factors control the formation, growth, and evolution of particles in the marine boundary layer (MBL). To address this question, simultaneous measurements of dimethylsulfide (DMS), sulfur dioxide (SO2), the aerosol chemical mass size distribution, and the aerosol number size distribution from 5 to 10,000 nm diameter were made on the National Oceanic and Atmospheric Administration (NOAA) ship Discoverer. From these data we conclude that the background MBL aerosol during ACE 1 often was composed of four distinct modes: an ultrafine (UF) mode (Dp = 5–20 nm), an Aitken mode (Dp = 20–80 nm), an accumulation mode (Dp = 80–300 nm), and a coarse mode (Dp > 300 nm). The presence of UF mode particles in the MBL could be explained by convective mixing between the free troposphere (FT) and the MBL associated with cloud pumping and subsidence following cold frontal passages. There was no evidence of major new particle production in the MBL. Oceanic emissions of DMS appeared to contribute to the growth of Aitken and accumulation mode particles. Coarse mode particles were comprised primarily of sea salt. Although these particles result from turbulence at the air-sea interface, the instantaneous wind speed accounted for only one third of the variance in the coarse mode number concentration in this region.

Emissions from Ships with respect to Their Effects on Clouds

Emissions of particles, gases, heat, and water vapor from ships are discussed with respect to their potential for changing the microstructure of marine stratiform clouds and producing the phenomenon known as ‘‘ship tracks.’’ Airborne measurements are used to derive emission factors of SO 2 and NO from diesel-powered and steam turbine-powered ships, burning low-grade marine fuel oil (MFO); they were ;15‐89 and ;2‐25 g kg21 of fuel burned, respectively. By contrast a steam turbine‐powered ship burning high-grade navy distillate fuel had an SO2 emission factor of ; 6gk g 21. Various types of ships, burning both MFO and navy distillate fuel, emitted from ;4 3 1015 to 2 3 1016 total particles per kilogram of fuel burned (;4 3 1015‐1.5 3 1016 particles per second). However, diesel-powered ships burning MFO emitted particles with a larger mode radius (;0.03‐0.05 mm) and larger maximum sizes than those powered by steam turbines burning navy distillate fuel (mode radius ;0.02 mm). Consequently, if the particles have similar chemical compositions, those emitted by diesel ships burning MFO will serve as cloud condensation nuclei (CCN) at lower supersaturations (and will therefore be more likely to produce ship tracks) than the particles emitted by steam turbine ships burning distillate fuel. Since steam turbine‐powered ships fueled by MFO emit particles with a mode radius similar to that of diesel-powered ships fueled by MFO, it appears that, for given ambient conditions, the type of fuel burned by a ship is more important than the type of ship engine in determining whether or not a ship will produce a ship track. However, more measurements are needed to test this hypothesis. The particles emitted from ships appear to be primarily organics, possibly combined with sulfuric acid produced by gas-to-particle conversion of SO 2. Comparison of model results with measurements in ship tracks suggests that the particles from ships contain only about 10% water-soluble materials. Measurements of the total particles entering marine stratiform clouds from diesel-powered ships fueled by MFO, and increases in droplet concentrations produced by these particles, show that only about 12% of the particles serve as CCN. The fluxes of heat and water vapor from ships are estimated to be ;2‐22 MW and;0.5‐1.5 kg s21, respectively. These emissions rarely produced measurable temperature perturbations, and never produced detectable perturbations in water vapor, in the plumes from ships. Nuclear-powered ships, which emit heat but negligible particles, do not produce ship tracks. Therefore, it is concluded that heat and water vapor emissions do not play a significant role in ship track formation and that particle emissions, particularly from those burning low-grade fuel oil, are responsible for ship track formation. Subsequent papers in this special issue discuss and test these hypotheses.

Influence of Humidity On the Aerosol Scattering Coefficient and Its Effect on the Upwelling Radiance During ACE-2

Aerosol scattering coefficients (σsp) have been measured over the ocean at different relative humidities (RH) as a function of altitude in the region surrounding the Canary Islands during the Second Aerosol Characterization Experiment (ACE-2) in June and July 1997. The data were collected by the University of Washington passive humidigraph (UWPH) mounted on the Pelican research aircraft. Concurrently, particle size distributions, absorption coefficients and aerosol optical depth were measured throughout 17 flights. A parameterization of σsp as a function of RH was utilized to assess the impact of aerosol hydration on the upwelling radiance (normalized to the solar constant and cosine of zenith angle). The top of the atmosphere radiance signal was simulated at wavelengths corresponding to visible and near-infrared bands of the EOS-AM )“Terra” (detectors, MODIS and MISR. The UWPH measured σsp at 2 RHs, one below and the other above ambient conditions. Ambient σsp was obtained by interpolation of these 2 measurements. The data were stratified in terms of 3 types of aerosols: Saharan dust, clean marine (marine boundary layer background) and polluted marine aerosols (i.e., 2- or 1-day old polluted aerosols advected from Europe). An empirical relation for the dependence of σsp on RH, defined by σsp(RH)=k. (1−RH/100)−γ, was used with the hygroscopic exponent γ derived from the data. The following γ values were obtained for the 3 aerosol types: γ(dust)=0.23±0.05, γ(clean marine)= 0.69±0.06 and γ(polluted marine)=0.57±0.06. Based on the measured γs, the above equation was utilized to derive aerosol models with different hygroscopicities. The satellite simulation signal code 6S was used to compute the upwelling radiance corresponding to each of those aerosol models at several ambient humidities. For the pre-launch estimated precision of the sensors and the assumed viewing geometry of the instrument, the simulations suggest that the spectral and angular dependence of the reflectance measured by MISR is not sufficient to distinguish aerosol models with various different combinations of values for dry composition, γ and ambient RH. A similar behavior is observed for MODIS at visible wavelengths. However, the 2100 nm band of MODIS appears to be able to differentiate between at least same aerosol models with different aerosol hygroscopicity given the MODIS calibration error requirements. This result suggests the possibility of retrieval of aerosol hygroscopicity by MODIS.

The Monterey Area Ship Track Experiment

In June 1994 the Monterey Area Ship Track (MAST) experiment was conducted off the coast of California to investigate the processes behind anthropogenic modification of cloud albedo. The motivation for the MAST experiment is described here, as well as details of the experimental design. Measurement platforms and strategies are explained, and a summary of experiment operations is presented. The experiment produced the largest dataset to date of direct measurements of the effects of ships on the microphysics and radiative properties of marine stratocumulus clouds as an analog for the indirect effects of anthropogenic pollution on cloud albedo.

Snow/Cloud Discrimination with Multispectral Satellite Measurements

Abstract An algorithm is developed and evaluated for discriminating between clouds, snow-covered land and snow-free land in satellite image data. The multispectral technique uses daytime images of NOAA AVHRR channels 1 (0.63 μm), 3 (3.7 μm), and 4 (11.0 μm). Reflectance is derived for channel 3 by using the channel 4 emission temperature to estimate and remove the channel 3 thermal emission. Separation of clouds from snow and land is based primarily on the derived channel 3 reflectance. Observed reflectance in channel 3 is 0.02 to 0.04 for snow, 0.03 to 0.10 for land, 0.02 to 0.27 for ice clouds and 0.08 to 0.36 for liquid clouds. These ranges overlap for thin cirrus and snow, so the routine attempts analysis of cirrus based on differences in transmission between channels 3 and 4. Six case were analyzed and the total cloud cover was verified against a total of 110 surface observations in the standard categories of clear, scattered, broken and overcast. One of the cases is presented in detail to illustrate...

Composite Ship Track Characteristics

Abstract The physical and radiative properties of a composite ship track are described from the analysis of 131 ship–ship track correlation pairs collected during the Monterey Area Ship Track experiment. The significant variability of ship tracks around their average characteristics is also described. The nominal environmental conditions for the ship track set are also described. The composite ship track is 296 ± 233 km long, 7.3 ± 6 h old, and averages 9 ± 5 km wide. The ship is, on the average, 16 ± 8 km from of the head of the ship track along the relative wind vector and corresponds to a time of 25 ± 15 min. The set of ship tracks examined in this study formed in marine boundary layers that were between 300 and 750 m deep, and no tracks formed in boundary layers above 800 m. The tracks form in regions of high relative humidity, small air–sea temperature differences, and moderate winds (average of 7.7 ± 3.1 m s−1). The ambient cloud reflectance in advanced very high resolution radiometer channel 3 (3.7...

The Role of Background Cloud Microphysics in the Radiative Formation of Ship Tracks

The authors investigate the extent to which the contrast brightness of ship tracks, that is, the relative change in observed solar reflectance, in visible and near-infrared imagery can be explained by the microphysics of the background cloud in which they form. The sensitivity of visible and near-infrared wavelengths for detecting reflectance changes in ship tracks is discussed, including the use of a modified cloud susceptibility parameter, termed the ‘‘contrast susceptibility,’’ for assessing the sensitivity of background cloud microphysics on potential track development. It is shown that the relative change in cloud reflectance for ship tracks is expected to be larger in the near-infrared than in the visible and that 3.7- mm channels, widely known to be useful for detecting tracks, have the greatest sensitivity. The usefulness of contrast susceptibility as a predictor of ship track contrast is tested with airborne and satellite remote sensing retrievals of background cloud parameters and track contrast. Retrievals are made with the high spatial resolution Moderate Resolution Imaging Spectroradiometer Airborne Simulator flown on the National Aeronautics and Space Administration’s high-altitude ER-2 aircraft, and with the larger-scale perspective of the advanced very high resolution radiometer. Observed modifications in cloud droplet effective radius, optical thickness, liquid water path, contrast susceptibility, and reflectance contrast are presented for several ship tracks formed in background clouds with both small and large droplet sizes. The remote sensing results are augmented with in situ measurements of cloud microphysics that provide data at the smaller spatial scales.