Hossein Dadashazar

Relationships between giant sea salt particles and clouds inferred from aircraft physicochemical data

NASA [NNX14AM02G]; Office of Naval Research [N00014-10-1-0811, N00014-11-1-0783, N00014-10-1-0200, N00014-04-1-0118, N00014-16-1-2567]

Contrasting cloud composition between coupled and decoupled marine boundary layer clouds

Marine stratocumulus clouds often become decoupled from the vertical layer immediately above the ocean surface. This study contrasts cloud chemical composition between coupled and decoupled marine stratocumulus clouds for dissolved nonwater substances. Cloud water and droplet residual particle composition were measured in clouds off the California coast during three airborne experiments in July–August of separate years (Eastern Pacific Emitted Aerosol Cloud Experiment 2011, Nucleation in California Experiment 2013, and Biological and Oceanic Atmospheric Study 2015). Decoupled clouds exhibited significantly lower air-equivalent mass concentrations in both cloud water and droplet residual particles, consistent with reduced cloud droplet number concentration and subcloud aerosol (D_p > 100 nm) number concentration, owing to detachment from surface sources. Nonrefractory submicrometer aerosol measurements show that coupled clouds exhibit higher sulfate mass fractions in droplet residual particles, owing to more abundant precursor emissions from the ocean and ships. Consequently, decoupled clouds exhibited higher mass fractions of organics, nitrate, and ammonium in droplet residual particles, owing to effects of long-range transport from more distant sources. Sodium and chloride dominated in terms of air-equivalent concentration in cloud water for coupled clouds, and their mass fractions and concentrations exceeded those in decoupled clouds. Conversely, with the exception of sea-salt constituents (e.g., Cl, Na, Mg, and K), cloud water mass fractions of all species examined were higher in decoupled clouds relative to coupled clouds. Satellite and Navy Aerosol Analysis and Prediction System-based reanalysis data are compared with each other, and the airborne data to conclude that limitations in resolving boundary layer processes in a global model prevent it from accurately quantifying observed differences between coupled and decoupled cloud composition.

Impact of Wildfire Emissions on Chloride and Bromide Depletion in Marine Aerosol Particles

This work examines particulate chloride (Cl-) and bromide (Br-) depletion in marine aerosol particles influenced by wildfires at a coastal California site in the summers of 2013 and 2016. Chloride exhibited a dominant coarse mode due to sea salt influence, with substantially diminished concentrations during fire periods as compared to nonfire periods. Bromide exhibited a peak in the submicrometer range during fire and nonfire periods, with an additional supermicrometer peak in the latter periods. Chloride and Br- depletions were enhanced during fire periods as compared to nonfire periods. The highest observed %Cl- depletion occurred in the submicrometer range, with maximum values of 98.9% (0.32-0.56 μm) and 85.6% (0.56-1 μm) during fire and nonfire periods, respectively. The highest %Br- depletion occurred in the supermicrometer range during fire and nonfire periods with peak depletion between 1.8-3.2 μm (78.8% and 58.6%, respectively). When accounting for the neutralization of sulfate by ammonium, organic acid particles showed the greatest influence on Cl- depletion in the submicrometer range. These results have implications for aerosol hygroscopicity and radiative forcing in areas with wildfire influence owing to depletion effects on composition.

Analysis of aerosol composition data for western United States wildfires between 2005 and 2015: Dust emissions, chloride depletion, and most enhanced aerosol constituents

This study examines major wildfires in the western United States between 2005 and 2015 to determine which species exhibit the highest percent change in mass concentration on day of peak fire influence relative to preceding nonfire days. Forty-one fires were examined using the Environmental Protection Agency (EPA) Interagency Monitoring of Protected Visual Environments (IMPROVE) data set. Organic carbon (OC) and elemental carbon (EC) constituents exhibited the highest percent change increase. The sharpest enhancements were for the volatile (OC1) and semivolatile (OC2) OC fractions, suggestive of secondary organic aerosol formation during plume transport. Of the noncarbonaceous constituents, Cl, P, K, NO3-, and Zn levels exhibited the highest percent change. Dust was significantly enhanced in wildfire plumes, based on significant enhancements in fine soil components (i.e., Si, Ca, Al, Fe, and Ti) and PMcoarse (i.e., PM10-PM2.5). A case study emphasized how transport of wildfire plumes significantly impacted downwind states, with higher levels of fine soil and PMcoarse at the downwind state (Arizona) as compared to the source of the fires (California). A global model (Navy Aerosol Analysis and Prediction System, NAAPS) did not capture the dust influence over California or Arizona during this case event because it is not designed to resolve dust dynamics in fires, which motivates improved treatment of such processes. Significant chloride depletion was observed on the peak EC day for almost a half of the fires examined. Size-resolved measurements during two specific fires at a coastal California site revealed significant chloride reductions for particle aerodynamic diameters between 1 and 10 μm.

A Multi-Year Data Set on Aerosol-Cloud-Precipitation-Meteorology Interactions for Marine Stratocumulus Clouds

Airborne measurements of meteorological, aerosol, and stratocumulus cloud properties have been harmonized from six field campaigns during July-August months between 2005 and 2016 off the California coast. A consistent set of core instruments was deployed on the Center for Interdisciplinary Remotely-Piloted Aircraft Studies Twin Otter for 113 flight days, amounting to 514 flight hours. A unique aspect of the compiled data set is detailed measurements of aerosol microphysical properties (size distribution, composition, bioaerosol detection, hygroscopicity, optical), cloud water composition, and different sampling inlets to distinguish between clear air aerosol, interstitial in-cloud aerosol, and droplet residual particles in cloud. Measurements and data analysis follow documented methods for quality assurance. The data set is suitable for studies associated with aerosol-cloud-precipitation-meteorology-radiation interactions, especially owing to sharp aerosol perturbations from ship traffic and biomass burning. The data set can be used for model initialization and synergistic application with meteorological models and remote sensing data to improve understanding of the very interactions that comprise the largest uncertainty in the effect of anthropogenic emissions on radiative forcing.

Characteristic Vertical Profiles of Cloud Water Composition in Marine Stratocumulus Clouds and Relationships With Precipitation

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 SO4 2-, 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.

Sources of pollution and interrelationships between aerosol and precipitation chemistry at a central California site

This study examines co-located aerosol and precipitation chemistry data between 2010 and 2016 at Pinnacles National Monument ~65 km east of the coastline in central California. Positive matrix factorization analysis of the aerosol composition data revealed seven distinct pollutant sources: aged sea salt (25.7% of PM2.5), biomass burning (24.2% of PM2.5), fresh sea salt (15.0% of PM2.5), secondary sulfate (11.7% of PM2.5), dust (10.0% of PM2.5), vehicle emissions (8.2% of PM2.5), and secondary nitrate (5.2% of PM2.5). The influence of meteorology and transport on monthly patterns of PM2.5 composition is discussed. Only secondary sulfate exhibited a statistically significant change (a reduction) over time among the PM2.5 source factors. In contrast, PMcoarse exhibited a significant increase most likely due to dust influence. Monthly profiles of precipitation chemistry are summarized showing that the most abundant species in each month was either SO42-, NO3-, or Cl-. Intercomparisons between the precipitation and aerosol data revealed several features: (i) precipitation pH was inversely related to factors associated with more acidic aerosol constituents such as secondary sulfate and aged sea salt, in addition to being reduced by uptake of HNO3 in the liquid phase; (ii) two aerosol source factors (dust and aged sea salt) and PMcoarse exhibited a positive association with Ca2+ in precipitation, suggestive of directly emitted aerosol types with larger sizes promoting precipitation; and (iii) sulfate levels in both the aerosol and precipitation samples analyzed were significantly correlated with dust and aged sea salt PMF factors, pointing to the partitioning of secondary sulfate to dust and sea salt particles. The results of this work have implications for the regions air quality and hydrological cycle, in addition to demonstrating that the use of co-located aerosol and precipitation chemistry data can provide insights relevant to aerosol-precipitation interactions.

Characterization of the Real Part of Dry Aerosol Refractive Index Over North America From the Surface to 12 km

National Aeronautics and Space Administration [NNX12AC10G, NNX14AP75G]; United States Navy Office of Naval Research [N00014-10-1-0811]; NASA Earth and Space Science Fellowship [NNX14AK79H]; NASA [NNX12AC03G, NNX15AT96G]; Visiting Scientist Program at the National Institute of Aerospace (NIA)