Cloud condensation nuclei activity, closure, and droplet growth kinetics of Houston aerosol during the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS)

In situ cloud condensation nuclei (CCN) measurements were obtained in the boundary layer over Houston, Texas, during the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) campaign onboard the CIRPAS Twin Otter. Polluted air masses in and out of cloudy regions were sampled for a total of 22 flights, with CCN measurements obtained for 17 of these flights. In this paper, we focus on CCN closure during two flights, within and downwind of the Houston regional plume and over the Houston Ship Channel. During both flights, air was sampled with particle concentrations exceeding 25,000 cm^(−3) and CCN concentrations exceeding 10,000 cm^(−3). CCN closure is evaluated by comparing measured concentrations with those predicted on the basis of measured aerosol size distributions and aerosol mass spectrometer particle composition. Different assumptions concerning the internally mixed chemical composition result in average CCN overprediction ranging from 3% to 36% (based on a linear fit). It is hypothesized that the externally mixed fraction of the aerosol contributes much of the CCN closure scatter, while the internally mixed fraction largely controls the overprediction bias. On the basis of the droplet sizes of activated CCN, organics do not seem to impact, on average, the CCN activation kinetics

Comprehensive Simultaneous Shipboard and Airborne Characterization of Exhaust from a Modern Container Ship at Sea

We report the first joint shipboard and airborne study focused on the chemical composition and water-uptake behavior of particulate ship emissions. The study focuses on emissions from the main propulsion engine of a Post-Panamax class container ship cruising off the central coast of California and burning heavy fuel oil. Shipboard sampling included micro-orifice uniform deposit impactors (MOUDI) with subsequent off-line analysis, whereas airborne measurements involved a number of real-time analyzers to characterize the plume aerosol, aged from a few seconds to over an hour. The mass ratio of particulate organic carbon to sulfate at the base of the ship stack was 0.23 ± 0.03, and increased to 0.30 ± 0.01 in the airborne exhaust plume, with the additional organic mass in the airborne plume being concentrated largely in particles below 100 nm in diameter. The organic to sulfate mass ratio in the exhaust aerosol remained constant during the first hour of plume dilution into the marine boundary layer. The mass spectrum of the organic fraction of the exhaust aerosol strongly resembles that of emissions from other diesel sources and appears to be predominantly hydrocarbon-like organic (HOA) material. Background aerosol which, based on air mass back trajectories, probably consisted of aged ship emissions and marine aerosol, contained a lower organic mass fraction than the fresh plume and had a much more oxidized organic component. A volume-weighted mixing rule is able to accurately predict hygroscopic growth factors in the background aerosol but measured and calculated growth factors do not agree for aerosols in the ship exhaust plume. Calculated CCN concentrations, at supersaturations ranging from 0.1 to 0.33%, agree well with measurements in the ship-exhaust plume. Using size-resolved chemical composition instead of bulk submicrometer composition has little effect on the predicted CCN concentrations because the cutoff diameter for CCN activation is larger than the diameter where the mass fraction of organic aerosol begins to increase significantly. The particle number emission factor estimated from this study is 1.3 × 10^(16) (kg fuel)^(−1), with less than 1/10 of the particles having diameters above 100 nm; 24% of particles (>10 nm in diameter) activate into cloud droplets at 0.3% supersaturation

On the link between ocean biota emissions, aerosol, and maritime clouds: Airborne, ground, and satellite measurements off the coast of California

Surface, airborne, and satellite measurements over the eastern Pacific Ocean off the coast of California during the period between 2005 and 2007 are used to explore the relationship between ocean chlorophyll a, aerosol, and marine clouds. Periods of enhanced chlorophyll a and wind speed are coincident with increases in particulate diethylamine and methanesulfonate concentrations. The measurements indicate that amines are a source of secondary organic aerosol in the marine atmosphere. Subsaturated aerosol hygroscopic growth measurements indicate that the organic component during periods of high chlorophyll a and wind speed exhibit considerable water uptake ability. Increased average cloud condensation nucleus (CCN) activity during periods of increased chlorophyll a levels likely results from both size distribution and aerosol composition changes. The available data over the period of measurements indicate that the cloud microphysical response, as represented by either cloud droplet number concentration or cloud droplet effective radius, is likely influenced by a combination of atmospheric dynamics and aerosol perturbations during periods of high chlorophyll a concentrations

Aerosol-cloud relationships in continental shallow cumulus

Aerosol-cloud relationships are derived from 14 warm continental cumuli cases sampled during the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) by the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. Cloud droplet number concentration is clearly proportional to the subcloud accumulation mode aerosol number concentration. An inverse correlation between cloud top effective radius and subcloud aerosol number concentration is observed when cloud depth variations are accounted for. There are no discernable aerosol effects on cloud droplet spectral dispersion; the averaged spectral relative dispersion is 0.30 ± 0.04. Aerosol-cloud relationships are also identified from comparison of two isolated cloud cases that occurred under different degrees of anthropogenic influence. Cloud liquid water content, cloud droplet number concentration, and cloud top effective radius exhibit subadiabaticity resulting from entrainment mixing processes. The degree of LWC subadiabaticity is found to increase with cloud depth. Impacts of subadiabaticity on cloud optical properties are assessed. It is estimated that owing to entrainment mixing, cloud LWP, effective radius, and cloud albedo are decreased by 50–85%, 5–35%, and 2–26%, respectively, relative to adiabatic values of a plane-parallel cloud. The impact of subadiabaticity on cloud albedo is largest for shallow clouds. Results suggest that the effect of entrainment mixing must be accounted for when evaluating the aerosol indirect effect

CCN Activity, Closure and Droplet Growth Kinetics of Houston Aerosol During the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS)

For Publication in Journal of Geophysical Research – Atmospheres TexAQS/GoMACCS special issueIn-situ Cloud Condensation Nuclei (CCN) measurements were obtained in the boundary layer over Houston, TX during the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) campaign onboard the CIRPAS Twin Otter. Polluted air masses in and out of cloudy regions were sampled for a total of 22 flights, with CCN measurements obtained for 17 of these flights. In this paper, we focus on CCN closure during two flights, within and downwind of the Houston regional plume and over the Houston Ship Channel. During both flights, air was sampled with particle concentrations exceeding 25,000 cm-3 and CCN concentrations exceeding 10,000 cm-3. CCN closure was evaluated by comparing measured CCN concentrations with those predicted on the basis of measured aerosol size distributions and Aerosol Mass Spectrometer particle composition. Different assumptions concerning the internally mixed chemical composition result in average CCN overprediction ranging from 3% to 36% (based on a linear fit). It is hypothesized that the externally-mixed fraction of the aerosol contributes much of the CCN closure scatter, while the internally-mixed fraction largely controls the overprediction bias. Finally, based on the droplet sizes of activated CCN, organics do not seem to impact, on average, the CCN activation kinetics.We acknowledge support from the National Oceanic and Atmospheric Administration (NOAA) under contracts NA05OAR4310101 and NA06OAR4310082, the support of an NSF CAREER grant, and the Office of Naval Research. SL would like to acknowledge the support of a Georgia Institute of Technology (Georgia Tech) Presidential Fellowship and a National Center for Atmospheric Research (NCAR) Advanced Study Program (ASP) Graduate Fellowship