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The effect of ocean biological productivity on marine clouds is explored over a large phytoplankton bloom in the Southern Ocean with the use of remotely sensed data. Cloud droplet number concentration over the bloom was twice what it was away from the bloom, and cloud effective radius was reduced by 30%. The resulting change in the short-wave radiative flux at the top of the atmosphere was -15 watts per square meter, comparable to the aerosol indirect effect over highly polluted regions. This observed impact of phytoplankton on clouds is attributed to changes in the size distribution and chemical composition of cloud condensation nuclei. We propose that secondary organic aerosol, formed from the oxidation of phytoplankton-produced isoprene, can affect chemical composition of marine cloud condensation nuclei and influence cloud droplet number. Model simulations support this hypothesis, indicating that 100% of the observed changes in cloud properties can be attributed to the isoprene secondary organic aerosol.

One pathway by which the oceans influence climate is via the emission of sea spray that may subsequently influence cloud properties. Sea spray emissions are known to be dependent on atmospheric and oceanic physicochemical parameters, but the potential role of ocean biology on sea spray fluxes remains poorly characterized. Here we show a consistent significant relationship between seawater nanophytoplankton cell abundances and sea-spray derived Cloud Condensation Nuclei (CCN) number fluxes, generated using water from three different oceanic regions. This sensitivity of CCN number fluxes to ocean biology is currently unaccounted for in climate models yet our measurements indicate that it influences fluxes by more than one order of magnitude over the range of phytoplankton investigated.

Terrestrial and marine photosynthetic organisms emit trace gases, including isoprene and monoterpenes. The resulting emissions can impact the atmosphere through oxidative chemistry and formation of secondary organic aerosol. Large uncertainty exists as to the magnitude of the marine sources of these compounds, their controlling factors, and contribution to marine aerosol. In recent years, the number of relevant studies has increased substantially, necessitating the review of this topic. Isoprene emissions vary with plankton species, chlorophyll concentration, light, and other factors. Remote marine boundary layer isoprene mixing ratios can reach >300 pptv, and extrapolated global ocean fluxes range from <1 to >10 Tg C year-1. Modeling studies using surface chlorophyll concentration as an isoprene emissions proxy suggest variable atmospheric impacts. More information is needed, including emission fluxes of isoprene and monoterpenes from various biogeographical areas, the effects of species and nutrient limitation on emissions, and the aerosol yields via condensation and nucleation, in order to better quantify the atmospheric impacts of marine isoprene and monoterpenes.

The formation of inorganic fine particulate matter (i.e., iPM2.5) is controlled by the thermodynamic equilibrium partitioning of NH3-NH4+. To develop effective control strategies of PM2.5, we aim to understand the impacts of changes in different precursor gases on iPM2.5 concentrations and partitioning of NH3-NH4+. To understand partitioning of NH3-NH4+ in the southeastern U.S., responses of iPM2.5 to precursor gases in four seasons were investigated using field measurements of iPM2.5, precursor gases, and meteorological conditions. The ISORROPIA II model was used to examine the effects of changes in total ammonia (gas + aerosol), total sulfuric acid (aerosol), and total nitric acid (gas + aerosol) on iPM2.5 concentrations and partitioning of NH3-NH4+. The results indicate that reduction in total H2SO4 is more effective than reduction in total HNO3 and total NH3 to reduce iPM2.5 especially under NH3-rich condition. The reduction in total H2SO4 may change partitioning of NH3-NH4+ towards gas-phase and may also lead to an increase in NO3− under NH3-rich conditions, which does not necessarily lead to full neutralization of acidic gases (pH < 7). Thus, future reduction in iPM2.5 may necessitate the coordinated reduction in both H2SO4 and HNO3 in the southeastern U.S. It is also found that the response of iPM2.5 to the change in total H2SO4 is more sensitive in summer than winter due to the dominance of SO42− salts in iPM2.5 and the high temperature in summer. The NH3 emissions from Animal Feeding Operations (AFOs) at an agricultural rural site (YRK) had great impacts on partitioning of NH3-NH4+. The Multiple Linear Regression (MLR) model revealed a strong positive correlation between cation-NH4+ and anions-SO42− and NO3−. This research provides an insight into iPM2.5 formation mechanism for the advancement of PM2.5 control and regulation in the southeastern U.S.

One of the greatest sources of uncertainty in simulations of climate and climate change is the influence of aerosols on the optical properties of clouds. The root of this influence is the droplet nucleation process, which involves the spontaneous growth of aerosol into cloud droplets at cloud edges, during the early stages of cloud formation, and in some cases within the interior of mature clouds. Numerical models of droplet nucleation represent much of the complexity of the process, but at a computational cost that limits their application to simulations of hours or days. Physically‐based parameterizations of droplet nucleation are designed to quickly estimate the number nucleated as a function of the primary controlling parameters: the aerosol number size distribution, hygroscopicity and cooling rate. Here we compare and contrast the key assumptions used in developing each of the most popular parameterizations and compare their performances under a variety of conditions. We find that the more complex parameterizations perform well under a wider variety of nucleation conditions, but all parameterizations perform well under the most common conditions. We then discuss the various applications of the parameterizations to cloud‐resolving, regional and global models to study aerosol effects on clouds at a wide range of spatial and temporal scales. We compare estimates of anthropogenic aerosol indirect effects using two different parameterizations applied to the same global climate model, and find that the estimates of indirect effects differ by only 10%. We conclude with a summary of the outstanding challenges remaining for further development and application.

[...]uncertainty in the origin, number size distribution, and chemical composition of background aerosol complicates the assessments of direct and indirect anthropogenic aerosol forcing and makes it difficult for Earth system science models to accurately predict 21st century climate change. Because effects on climate are estimated from the differences between model simulations with present-day and preindustrial aerosol and precursor emissions, concerns over the global aerosol budget in the absence of anthropogenic influence have sparked renewed interest in the natural emissions of trace gases (acting as particle precursors) and aerosols. A reduction of the uncertainties in the representation of natural aerosols in climate models requires an improved quantification of their number, size distribution, chemical composition, and hygroscopic properties in the marine boundary layer (MBL). Studies have shown that the production rates and physiological properties of SSA and the resulting efficacy to act as CCN or INP can be strongly influenced by the ocean’s biogeochemical state (nutrient availability, pH, bacterial and phytoplankton abundance, eco-physiological factors, and evolutionary drivers). By combining Moderate Resolution Imaging Spectroradiometer (MODIS) and Aerosol Robotic Network (AERONET) AOD retrievals with 2 m wind speed data, the study develops a new power–law relationship between AOD and surface–wind over the oceans.

The global chemical transport model GEOS‐Chem, implemented with a dust‐iron dissolution scheme, was used to analyze the magnitude and spatial distribution of mineral dust and soluble‐iron (sol‐Fe) deposition to the South Atlantic Ocean (SAO). The comparison of model results with remotely sensed data shows that GEOS‐Chem can capture dust source regions in Patagonia and characterize the temporal variability of dust outflow. For a year‐long model simulation, 22 Tg of mineral dust and 4 Gg of sol‐Fe were deposited to the surface waters of the entire SAO region, with roughly 30% of this dust and sol‐Fe predicted to be deposited to possible high nitrate low chlorophyll oceanic regions. Model‐predicted dissolved iron fraction of mineral dust over the SAO was small, on average only accounting for 0.57% of total iron. Simulations suggest that the primary reason for such a small fraction of sol‐Fe is the low ambient concentrations of acidic trace gases available for mixing with dust plumes. Overall, the amount of acid added to the deliquesced aerosol solution was not enough to overcome the alkalinity buffer of Patagonian dust and initiate considerable acid dissolution of mineral‐iron. Sensitivity studies show that the amount of sol‐Fe deposited to the SAO was largely controlled by the initial amount of sol‐Fe at the source region, with limited contribution from the spatial variability of Patagonian‐desert topsoil mineralogy and natural sources of acidic trace gases. Simulations suggest that Patagonian dust should have a minor effect on biological productivity in the SAO.

Dust aerosol optical depth (AOD) and vertical distribution of aerosol extinction predicted by a global chemical transport model (GEOS‐Chem) are compared to space‐borne data from the Moderate‐resolution Imaging Spectroradiometer (MODIS), Multi‐Angle Imaging SpectroRadiometer (MISR), and Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) for March 2009 to February 2010. Model‐predicted and remotely‐sensed AOD/aerosol extinction profiles are compared over six regions where aerosol abundances are dominated by mineral dust. Calculations indicate that over the regions examined in this study (with the exception of Middle Eastern dust sources) GEOS‐Chem predicts higher AOD values compared to MODIS and MISR. The positive bias is particularly pronounced over the Saharan dust source regions, where model‐predicted AOD values are a factor of 2 to 3 higher. The comparison with CALIPSO‐derived dust aerosol extinction profiles revealed that the model overestimations of dust abundances over the study regions primarily occur below ∼4 km, suggesting excessive emissions of mineral dust and/or uncertainties in dust optical properties. The implementation of a new dust size distribution scheme into GEOS‐Chem reduced the yearly‐mean positive bias in model‐predicted AOD values over the study regions. The results were most noticeable over the Saharan dust source regions where the differences between model‐predicted and MODIS/MISR retrieved AOD values were reduced from 0.22 and 0.17 to 0.02 and −0.04, respectively. Our results suggest that positive/negative biases between satellite and model‐predicted aerosol extinction values at different altitudes can sometimes even out, giving a false impression for the agreement between remotely‐sensed and model‐predicted column‐integrated AOD data. Key Points Modeled dust AOD and extinction profiles are compared to remotely‐sensed data Baseline model captures horizontal and vertical distribution of mineral dust New dust mass size distribution improves simulated magnitudes of dust AODs

We apply principles of Gibbs phase plane chemistry across the entire ocean-atmosphere interface to investigate aerosol generation and geophysical transfer issues. Marine surface tension differences comprise a tangential pressure field controlling trace gas fluxes, primary organic inputs, and sea spray salt injections, in addition to heat and momentum fluxes. Mapping follows from the organic microlayer composition, now represented in ocean system models. Organic functional variations drive the microforcing, leading to (1) reduced turbulence and (by extension) laminar gas-energy diffusion; plus (2) altered bubble film mass emission into the boundary layer. Interfacial chemical behaviors are, therefore, closely reviewed as the background. We focus on phase transitions among two dimensional “solid, liquid, and gaseous” states serving as elasticity indicators. From the pool of dissolved organic carbon (DOC) only proteins and lipids appear to occupy significant atmospheric interfacial areas. The literature suggests albumin and stearic acid as the best proxies, and we distribute them through ecodynamic simulation. Consensus bulk distributions are obtained to control their adsorptive equilibria. We devise parameterizations for both the planar free energy and equation of state, relating excess coverage to the surface pressure and its modulus. Constant settings for the molecular surrogates are drawn from laboratory study and successfully reproduce surfactant solid-to-gas occurrence in compression experiments. Since DOC functionality measurements are rare, we group them into super-ecological province tables to verify aqueous concentration estimates. Outputs are then fed into a coverage, tension, elasticity code. The resulting two dimensional pressure contours cross a critical range for the regulation of precursor piston velocity, bubble breakage, and primary aerosol sources plus ripple damping. Concepts extend the water-air adsorption theory currently embodied in our OCEANFILMS aerosol emissions package, and the two approaches could be inserted into Earth System Models together. Uncertainties in the logic include kinetic and thermochemical factors operating at multiple scales.

The vertical distribution of freshly nucleated aerosol particles in the marine boundary layer remains poorly constrained, limiting our ability to represent new particle formation in climate models. Here we characterize 3–10 nm particle events, termed small particle events (SPEs), by deriving their vertical turbulent fluxes from aircraft measurements during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. To overcome stationarity limitations of traditional eddy covariance methods, we applied continuous wavelet transform analysis to data collected during June–July 2017 and January–February 2018 flights over the Azores. Our flux-based analysis revealed two distinct SPE scenarios with different vertical structures and spatial extents. The first featured nucleation in the entrainment zone, where free tropospheric air entrains into the boundary layer. The second showed nucleation in the decoupled layer, a stratified region between the well-mixed surface layer and cloud-topped upper boundary layer. In both cases, convergence of air masses from different layers diluted preexisting aerosol surface area to very low levels, creating conditions favorable for nucleation and generating strong downward particle fluxes. SPEs occurred in 15 % of flights, challenging prevailing theoretical expectations that new particle formation should rarely occur in marine boundary layers due to high condensation and coagulation sink capacity of sea spray aerosols. Aircraft-derived particle fluxes provide first observational constraints on the vertical location and source strength of likely nucleation regions in the remote marine boundary layer, improving aerosol source representations in climate models and reducing uncertainties in aerosol-cloud interactions.