ALBERT

Description: Atmospheric measurements of aerosol size‐resolved hygroscopicity at submicron sizes are carried out at the United States Army Corps of Engineers Field Research Facility in Duck, North Carolina. The scientific aim of the field deployment is to gain improved understanding of the springtime advection of aerosols from the East Coast of the United States over the Atlantic and help to constrain assessments of anthropogenic particle contributions to the marine boundary layer aerosol budget. Air mass back trajectories show that the aerosol sampled at the coast is largely of continental origin that either gets transported directly from the land or spends some time over the Atlantic Ocean. Aerosol size‐resolved hygroscopicity measurements are consistent with air masses of both continental and marine background that are heavily influenced by the continental outflow. Aitken and accumulation mode mean diameters range from 49.1 ± 1.7 nm to 66.9 ± 0.8 nm and 142.8 ± 1.1 nm to 155.0 ± 2.8 nm, respectively. Hygroscopicity distributions for 96 nm, 188 nm, and 284 nm dry‐sized particles show the mode hygroscopicity parameter range from 0.20 ± 0.01 to 0.54 ± 0.03, suggesting the presence of anthropogenic aerosols. We have used the method described by Royalty et al. (2017) to decompose the hygroscopicity distributions into three distinct classes based on the ambient aerosol hygroscopic properties relative to the hygroscopic properties of a reference compound. The method shows that continental outflow heavily influences aerosol chemical and physical properties at the East Coast, with hygroscopicities of submicron aerosols consistent with sulfate‐containing species (62% to 83%), with small contributions from sodium‐ and carbon‐containing particles (up to 9% and 37%, respectively).

Description: The global marine sources of organic carbon (OC) are estimated here using a physically-based parameterization for the emission of marine isoprene and primary organic matter. The model developed in this study allowed us, for the first time, to explore the relative contributions of sub- and super-micron organic matter and phytoplankton-produced secondary organic aerosol (SOA) to the total OC fraction of marine aerosol. New laboratory measurements of isoprene production by some of the main phytoplankton species under a range of environmental conditions was scaled up, with the help of satellite products, to infer the total annual mean ocean isoprene emissions of 0.92 Tg C yr−1. The sensitivity studies using different schemes for the euphotic zone depth and ocean phytoplankton speciation produced the upper and the lower range of marine-isoprene emissions of 0.31 to 1.09 Tg C yr−1, respectively. Empirical relationships between fluxes of water soluble (WSOM) and water insoluble (WIOM) organic matter (OM) and chlorophyll-a concentration was used to estimate the total primary sources of oceanic sub- and super-micron OC of 1.26 and 19.01 Tg C yr−1, respectively. Using a fixed 3% mass yield for the conversion of isoprene to SOA, our model simulations show minor (less than 0.2%) contribution of ocean produced isoprene to the total marine source of OC. However, our model calculations also indicate that over the tropical waters, marine isoprene-derived SOA could contribute over 40% of the total monthly-averaged sub-micron OC fraction of marine aerosol. The estimated contribution of ocean-isoprene SOA to hourly averaged sub-micron marine OC fluxes is even higher, reaching nearly 100% over the vast regions of the oceans during the midday hours. As it is widely believed that cloud condensation nuclei (CCN) is typically dominated by sub-micron sized particles, our findings suggest that marine sources of SOA could play a critical role in modulating properties of shallow marine clouds and influencing the climate.

Description: The supply of bioavailable iron to the high-nitrate low-chlorophyll (HNLC) waters of the Southern Ocean through atmospheric pathways could stimulate phytoplankton blooms and have major implications for the global carbon cycle. In this study, model results and remotely-sensed data are analyzed to examine the horizontal and vertical transport pathways of Patagonian dust and quantify the effect of iron-laden mineral dust deposition on marine biological productivity in the surface waters of the South Atlantic Ocean (SAO). Model simulations for the atmospheric transport and deposition of mineral dust and bioavailable iron are carried out for two large dust outbreaks originated at the source regions of Northern Patagonia during the austral summer of 2009. Model-simulated horizontal and vertical transport pathways of Patagonian dust plumes are in reasonable agreement with remotely-sensed data. Simulations indicate that the synoptic meteorological patterns of high and low pressure systems are largely accountable for dust transport trajectories over the SAO. According to model results and retrievals from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO), synoptic flows caused by opposing pressure systems (a high pressure system located to the east or north-east of a low pressure system) elevate the South American dust plumes well above the marine boundary layer. Under such conditions, the bulk concentration of mineral dust can quickly be transported around the low pressure system in a clockwise manner, follow the southeasterly advection pathway, and reach the HNLC waters of the SAO and Antarctica in ~3–4 days after emission from the source regions of Northern Patagonia. Two different mechanisms for dust-iron mobilization into a bioavailable form are considered in this study. A global 3-D chemical transport model (GEOS-Chem), implemented with an iron dissolution scheme, is employed to estimate the atmospheric fluxes of soluble iron, while a dust/biota assessment tool (Boyd et al., 2010) is applied to evaluate the amount of bioavailable iron formed through the slow and sustained leaching of dust in the ocean mixed layer. The effect of iron-laden mineral dust supply on surface ocean biomass is investigated by comparing predicted surface chlorophyll-a concentration ([Chl-a]) to remotely-sensed data. As the dust transport episodes examined here represent large summertime outflows of mineral dust from South American continental sources, this study suggests that (1) atmospheric fluxes of mineral dust from Patagonia are not likely to be the major source of bioavailable iron to ocean regions characterized by high primary productivity; (2) even if Patagonian dust plumes may not cause visible algae blooms, they could still influence background [Chl-a] in the South Atlantic sector of the Southern Ocean.

Description: The aerosol-cloud interaction in different parts of the globe is examined here using multi-year statistics of remotely sensed data from two MODIS sensors aboard NASA's Terra (morning) and Aqua (afternoon) satellites. Simultaneous retrievals of aerosol loadings and cloud properties by the MODIS sensor allowed us to explore morning-to-afternoon variation of liquid cloud fraction (CF) and optical thickness (COT) for clean, moderately polluted and heavily polluted clouds in different seasons. Data analysis for seven-years of MODIS retrievals revealed strong temporal and spatial patterns in morning-to-afternoon variation of cloud fraction and optical thickness over different parts of the global oceans and the land. For the vast areas of stratocumulus cloud regions, the data shows that the days with elevated aerosol abundance were also associated with enhanced afternoon reduction of CF and COT pointing to the possible reduction of the indirect climate forcing. A positive correlation between aerosol optical depth and morning-to-afternoon variation of trade wind cumulus cloud cover was also found over the northern Indian Ocean, though no clear relationship between the concentration of Indo-Asian haze and morning-to-afternoon variation of COT was established. Over the Amazon region during wet conditions, aerosols are associated with an enhanced convective process in which morning shallow warm clouds are organized into afternoon deep convection with greater ice cloud coverage. Analysis presented here demonstrates that the new technique for exploring morning-to-afternoon variability in cloud properties by using the differences in data products from the two daily MODIS overpasses is capable of capturing some of the major features of diurnal variations in cloud properties and can be used for better understanding of aerosol radiative effects.

Description: The contribution of marine organic emissions to the air quality in coastal areas of the western United States is studied using the latest version of the US Environmental Protection Agency (EPA) regional-scale Community Multiscale Air Quality (CMAQv4.7) modeling system. Emissions of marine isoprene, monoterpenes, and primary organic matter (POM) from the ocean are implemented into the model to provide a comprehensive view of the connection between ocean biology and atmospheric chemistry and air pollution. Model simulations show that marine organics can increase the concentration of PM2.5 by 0.1–0.3 μg m−3 (up to 5%) in some coastal cities such as San Francisco, CA. This increase in the PM2.5 concentration is primarily attributed to the POM emissions, with small contributions from the marine isoprene and monoterpenes. When marine organic emissions are included, organic carbon (OC) concentrations over the remote ocean are increased by up to 50% (25% in coastal areas), values consistent with recent observational findings. This study is the first to quantify the air quality impacts from marine POM and monoterpenes for the United States, and it highlights the need for inclusion of marine organic emissions in air quality models.

Description: In this study, several marine primary organic aerosol (POA) emission schemes have been evaluated using the GEOS-Chem chemical transport model in order to provide guidance for their implementation in air quality and climate models. These emission schemes, based on varying dependencies of chlorophyll a concentration ([chl a]) and 10 m wind speed (U10), have large differences in their magnitude, spatial distribution, and seasonality. Model comparison with weekly and monthly mean values of the organic aerosol mass concentration at two coastal sites shows that the source function exclusively related to [chl a] does a better job replicating surface observations. Sensitivity simulations in which the negative U10 and positive [chl a] dependence of the organic mass fraction of sea spray aerosol are enhanced show improved prediction of the seasonality of the marine POA concentrations. A top-down estimate of submicron marine POA emissions based on the parameterization that compares best to the observed weekly and monthly mean values of marine organic aerosol surface concentrations has a global average emission rate of 6.3 Tg yr−1. Evaluation of existing marine POA source functions against a case study during which marine POA contributed the major fraction of submicron aerosol mass shows that none of the existing parameterizations are able to reproduce the hourly-averaged observations. Our calculations suggest that in order to capture episodic events and short-term variability in submicron marine POA concentration over the ocean, new source functions need to be developed that are grounded in the physical processes unique to the organic fraction of sea spray aerosol.

Description: Marine organic aerosol emissions have been implemented and evaluated within the National Center of Atmospheric Research (NCAR)'s Community Atmosphere Model (CAM5) with the Pacific Northwest National Laboratory's 7-mode Modal Aerosol Module (MAM-7). Emissions of marine primary organic aerosols (POA), phytoplankton-produced isoprene- and monoterpenes-derived secondary organic aerosols (SOA) and methane sulfonate (MS−) are shown to affect surface concentrations of organic aerosols in remote marine regions. Global emissions of submicron marine POA is estimated to be 7.9 and 9.4 Tg yr−1, for the Gantt et al. (2011) and Vignati et al. (2010) emission parameterizations, respectively. Marine sources of SOA and particulate MS− (containing both sulfur and carbon atoms) contribute an additional 0.2 and 5.1 Tg yr−1, respectively. Widespread areas over productive waters of the Northern Atlantic, Northern Pacific, and the Southern Ocean show marine-source submicron organic aerosol surface concentrations of 100 ng m−3, with values up to 400 ng m−3 over biologically productive areas. Comparison of long-term surface observations of water insoluble organic matter (WIOM) with POA concentrations from the two emission parameterizations shows that despite revealed discrepancies (often more than a factor of 2), both Gantt et al. (2011) and Vignati et al. (2010) formulations are able to capture the magnitude of marine organic aerosol concentrations, with the Gantt et al. (2011) parameterization attaining better seasonality. Model simulations show that the mixing state of the marine POA can impact the surface number concentration of cloud condensation nuclei (CCN). The largest increases (up to 20%) in CCN (at a supersaturation (S) of 0.2%) number concentration are obtained over biologically productive ocean waters when marine organic aerosol is assumed to be externally mixed with sea-salt. Assuming marine organics are internally-mixed with sea-salt provides diverse results with increases and decreases in the concentration of CCN over different parts of the ocean. The sign of the CCN change due to the addition of marine organics to sea-salt aerosol is determined by the relative significance of the increase in mean modal diameter due to addition of mass, and the decrease in particle hygroscopicity due to compositional changes in marine aerosol. Based on emerging evidence for increased CCN concentration over biologically active surface ocean areas/periods, our study suggests that treatment of sea spray in global climate models (GCMs) as an internal mixture of marine organic aerosols and sea-salt will likely lead to an underestimation in CCN number concentration.