Nicholas Meskhidze

Phytoplankton and Cloudiness in the Southern Ocean

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.

Production and Emissions of Marine Isoprene and Monoterpenes: A Review

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 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.

Aerosol-cloud drop concentration closure for clouds sampled during the International Consortium for Atmospheric Research on Transport and Transformation 2004 campaign

This study analyzes 27 cumuliform and stratiform clouds sampled aboard the CIRPAS Twin Otter during the 2004 International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) experiment. The data set was used to assess cloud droplet closure using (1) a detailed adiabatic cloud parcel model and (2) a state-of-the-art cloud droplet activation parameterization. A unique feature of the data set is the sampling of highly polluted clouds within the vicinity of power plant plumes. Remarkable closure was achieved (much less than the 20% measurement uncertainty) for both parcel model and parameterization. The highly variable aerosol did not complicate the cloud droplet closure, since the clouds had low maximum supersaturation and were not sensitive to aerosol variations (which took place at small particle sizes). The error in predicted cloud droplet concentration was mostly sensitive to updraft velocity. Optimal closure is obtained if the water vapor uptake coefficient is equal to 0.06, but can range between 0.03 and 1.0. The sensitivity of cloud droplet prediction error to changes in the uptake coefficient, organic solubility and surface tension depression suggest that organics exhibit limited solubility. These findings can serve as much needed constraints in modeling of aerosol-cloud interactions in the North America; future in situ studies will determine the robustness of our findings.

Acidic processing of mineral dust iron by anthropogenic compounds over the north Pacific Ocean

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 SO2 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.

Comparison between measured tracer fluxes and footprint model predictions over a homogeneous canopy of intermediate roughness

Abstract Fast response tracer flux measurements are compared against flux footprint predictions from both a Lagrangian stochastic simulation and an analytical solution to the equation of diffusion over a canopy of intermediate roughness. A turbulent tracer flux experiment was conducted over a peach orchard for a range of mildly unstable to very unstable conditions. For this purpose, a line source was used to release sulfur hexafluoride at treetop and fast response tracer flux instrumentation placed in the roughness sub-layer was mounted on four towers perpendicular to the line source to measure the vertical tracer flux. There was excellent agreement between Lagrangian simulated fluxes and their experimental counterparts. The analytical solution to the advection–diffusion equation used also shows a good agreement with the tracer fluxes particularly far from the tracer source. These results suggest that for canopies of intermediate roughness, the flux footprint predictions from both models presented work very well, despite their simplifying assumptions.

Effects of Ocean Ecosystem on Marine Aerosol-Cloud Interaction

Using satellite data for the surface ocean, aerosol optical depth (AOD), and cloud microphysical parameters, we show that statistically significant positive correlations exist between ocean ecosystem productivity, the abundance of submicron aerosols, and cloud microphysical properties over different parts of the remote oceans. The correlation coefficient for remotely sensed surface chlorophyll a concentration ([Chl-a]) and liquid cloud effective radii over productive areas of the oceans varies between and . Special attention is given to identifying (and addressing) problems from correlation analysis used in the previous studies that can lead to erroneous conclusions. A new approach (using the difference between retrieved AOD and predicted sea salt aerosol optical depth, ) is developed to explore causal links between ocean physical and biological systems and the abundance of cloud condensation nuclei (CCN) in the remote marine atmosphere. We have found that over multiple time periods, 550 nm (sensitive to accumulation mode aerosol, which is the prime contributor to CCN) correlates well with [Chl-a] over the productive waters of the Southern Ocean. Since [Chl-a] can be used as a proxy of ocean biological productivity, our analysis demonstrates the role of ocean ecology in contributing CCN, thus shaping the microphysical properties of low-level marine clouds.

Correction to “Droplet nucleation: Physically‐based parameterizations and comparative evaluation”

6 1. Atmospheric and Global Change Division, Pacific Northwest National 7 Laboratory, PO Box 999, Richland, Washington, 99352 8 9 2. Department of Mechanical Engineering, Texas A&M University-Kingsville, MSC 10 191, 700 University Blvd, Kingsville, Texas, 78363 11 12 3. Schools of Earth & Atmospheric Sciences and Chemical & Biomolecular 13 Engineering, Georgia Institute of Technology, 311 Ferst Drive, Atlanta, Georgia, 14 30332-0340 15 16 4. Geophysical Fluid Dynamics Laboratory, P. O. Box 308, Princeton, New Jersey, 17 08542 18 19 5. United Kingdom Meteorology Office, Exeter, United Kingdom 20 21 6. Department of Marine, Earth, and Atmospheric Sciences, North Carolina State 22 University, 2800 Faucette Dr, Raleigh, North Carolina, 27695‐8208 23 24 7. Chinese Research Academy of Environment Sciences, No.8 Dayangfang, 25 Beiyuan, Chaoyang District, Beijing 100012, China 26 27 8. Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 10029, 28 China 29 30 31 Submitted to Journal of Advances in Modeling of Earth Systems, April 7, 2011 32

Marine Aerosol-Cloud-Climate Interaction

1Department of Marine Earth and Atmospheric Sciences, North Carolina State University, Raleigh, NC, USA 2NASA/Goddard Space Flight Center, Greenbelt, MD, USA 3 Joint Research Centre Institute for Environment and Sustainability Climate Change Unit, Ispra, VA, Italy 4 Institut f. Atmosphare und Klima, Zurich, Switzerland 5Department of Chemistry, State University of New York, College of Environmental Science and Forestry, New York, USA

Creating Aerosol Types from CHemistry (CATCH): A New Algorithm to Extend the Link Between Remote Sensing and Models

Current remote sensing methods can identify aerosol types within an atmospheric column, presenting an opportunity to incrementally bridge the gap between remote sensing and models. Here a new algorithm was designed for Creating Aerosol Types from CHemistry (CATCH). CATCH-derived aerosol types—dusty mix, maritime, urban, smoke, and fresh smoke—are based on first-generation airborne High Spectral Resolution Lidar (HSRL-1) retrievals during the Ship-Aircraft Bio-Optical Research (SABOR) campaign, July/August 2014. CATCH is designed to derive aerosol types from model output of chemical composition. CATCH-derived aerosol types are determined by multivariate clustering of model-calculated variables that have been trained using retrievals of aerosol types from HSRL-1. CATCH-derived aerosol types (with the exception of smoke) compare well with HSRL-1 retrievals during SABOR with an average difference in aerosol optical depth (AOD) <0.03. Data analysis shows that episodic free tropospheric transport of smoke is underpredicted by the Goddard Earth Observing System- with Chemistry (GEOS-Chem) model. Spatial distributions of CATCH-derived aerosol types for the North American model domain during July/August 2014 show that aerosol type-specific AOD values occurred over representative locations: urban over areas with large population, maritime over oceans, smoke, and fresh smoke over typical biomass burning regions. This study demonstrates that model-generated information on aerosol chemical composition can be translated into aerosol types analogous to those retrieved from remote sensing methods. In the future, spaceborne HSRL-1 and CATCH can be used to gain insight into chemical composition of aerosol types, reducing uncertainties in estimates of aerosol radiative forcing.