Atmospheric processing of mineral aerosol by anthropogenic pollutants may be an important process by which insoluble iron can be transformed into soluble forms and become available to oceanic biota. Observations of the soluble iron fraction in atmospheric aerosol exhibit large variability, which is poorly represented in models. In this study, we implemented a dust iron dissolution scheme in a global chemistry transport model (GEOS‐Chem). The model is applied over the North Pacific Ocean during April 2001, a period when concentrations of dust and pollution within the east Asia outflow were high. Simulated fields of many key chemical constituents compare reasonably well with available observations, although some discrepancies are identified and discussed. In our simulations, the production of soluble iron varies temporally and regionally depending on pollution‐to‐dust ratio, primarily due to strong buffering by calcite. Overall, we show that the chemical processing mechanism produces significant amounts of dissolved iron reaching and being deposited in remote regions of the Pacific basin, with some seasonal variability. Simulated enhancements in particulate soluble iron fraction range from 0.5% to 6%, which is consistent with the observations. According to our simulations, ∼30% to 70% of particulate soluble iron over the North Pacific Ocean basin can be attributed to atmospheric processing. On the basis of April 2001 monthly simulations, sensitivity tests suggest that doubling SO 2 emissions can induce a significant increase (13% on average, up to 40% during specific events) in dissolved iron production and deposition to the remote Pacific. We roughly estimate that half of the primary productivity induced by iron deposition in a north Pacific high‐nutrient low‐chlorophyll region is due to soluble iron derived from anthropogenic chemical processing of Asian aerosol.
This study uses airborne cloud water composition measurements to characterize the vertical structure of air-equivalent mass concentrations of water-soluble species in marine stratocumulus clouds off the California coast. A total of 385 cloud water samples were collected in the months of July and August between 2011 and 2016 and analyzed for water-soluble ionic and elemental composition. Three characteristic profiles emerge: (i) a reduction of concentration with in-cloud altitude for particulate species directly emitted from sources below cloud without in-cloud sources (e.g., Cl- and Na+), (ii) an increase of concentration with in-cloud altitude (e.g., NO2- and formate), and (iii) species exhibiting a peak in concentration in the middle of cloud (e.g., non-sea-salt SO42-, NO3-, and organic acids). Vertical profiles of rainout parameters such as loss frequency, lifetime, and change in concentration with respect to time show that the scavenging efficiency throughout the cloud depth depends strongly on the thickness of the cloud. Thin clouds exhibit a greater scavenging loss frequency at cloud top, while thick clouds have a greater scavenging loss frequency at cloud base. The implications of these results for treatment of wet scavenging in models are discussed.
Abstract. The science guiding the EUREC4A campaign and its measurements is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. Through its ability to characterize processes operating across a wide range of scales, EUREC4A marked a turning point in our ability to observationally study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper-ocean processes or the life cycle of particulate matter. This characterization was made possible by thousands (2500) of sondes distributed to measure circulations on meso- (200 km) and larger (500 km) scales, roughly 400 h of flight time by four heavily instrumented research aircraft; four global-class research vessels; an advanced ground-based cloud observatory; scores of autonomous observing platforms operating in the upper ocean (nearly 10 000 profiles), lower atmosphere (continuous profiling), and along the air–sea interface; a network of water stable isotopologue measurements; targeted tasking of satellite remote sensing; and modeling with a new generation of weather and climate models. In addition to providing an outline of the novel measurements and their composition into a unified and coordinated campaign, the six distinct scientific facets that EUREC4A explored – from North Brazil Current rings to turbulence-induced clustering of cloud droplets and its influence on warm-rain formation – are presented along with an overview of EUREC4A's outreach activities, environmental impact, and guidelines for scientific practice. Track data for all platforms are standardized and accessible at https://doi.org/10.25326/165 (Stevens, 2021), and a film documenting the campaign is provided as a video supplement.
The ability of airborne particles to take up water may be enhanced by surface‐active components, but the importance of this effect is controversial because direct measurement of the surface tension of microscopic droplets has not been possible. Here we infer droplet surface tension from water uptake measurements of mixed organic‐inorganic particles at relative humidities just below saturation (99.3–99.9%). The surface tension of droplets formed on particles composed of NaCl and α ‐pinene ozonolysis products was reduced by 50–75%, but only when enough organic material was present to form a film on the droplet surface at least 0.8 nm thick. This study suggests that if atmospheric particles are predominantly (≳80%) composed of surface‐active material, their influence on cloud properties and thus climate could be enhanced, and their atmospheric lifetimes could be reduced.
