Particle production in the outflow of a midlatitude storm

The concentrations of atmospheric gases and condensation nuclei (CN) or aerosol in the outflow of a storm were measured aboard a NASA DC-8 aircraft, as described in a companion paper [Twohy et al., 2002]. The data are used here to study the production of the aerosol. Major fluctuations in CN concentration are observed, in correlation with gas-phase species, but these are shown to arise as the result of the mixing of two distinct air masses. It is deduced that the CN originated in a storm outflow air mass and that its concentration before mixing was approximately uniform over a flight distance of about 200 km. The formation of the aerosol by nucleation followed by growth and coagulation is analyzed assuming that it consists of water and sulphuric acid produced locally by the oxidation of SO2. The analysis uses analytic models, and it is concluded that a 5 min burst of nucleation was followed by growth and coagulation over a period of about 5 hours. Both the mass and number concentrations of the observed aerosol can be reproduced by this analysis within a timescale consistent with that of the storm. The final number concentration is very insensitive to the initial SO2 concentration

Interannual to decadal climate variability of sea salt aerosols in the coupled climate model CESM1.0

This study examines multiyear climate variability associated with sea salt aerosols and their contribution to the variability of shortwave cloud forcing (SWCF) using a 150 year simulation for preindustrial conditions of the Community Earth System Model version 1.0. The results suggest that changes in sea salt and related cloud and radiative properties on interannual timescales are dominated by the El Niño-Southern Oscillation cycle. Sea salt variability on longer (interdecadal) timescales is associated with low-frequency variability in the Pacific Ocean similar to the Interdecadal Pacific Oscillation but does not show a statistically significant spectral peak. A multivariate regression suggests that sea salt aerosol variability may contribute to SWCF variability in the tropical Pacific, explaining up to 20-30% of the variance in that region. Elsewhere, there is only a small sea salt aerosol influence on SWCF through modifying cloud droplet number and liquid water path that contributes to the change of cloud effective radius and cloud optical depth (and hence cloud albedo), producing a multiyear aerosol-cloud-wind interaction

Interannual to decadal climate variability of sea salt aerosols in the coupled climate model CESM1.0

This study examines multiyear climate variability associated with sea salt aerosols and their contribution to the variability of shortwave cloud forcing (SWCF) using a 150 year simulation for preindustrial conditions of the Community Earth System Model version 1.0. The results suggest that changes in sea salt and related cloud and radiative properties on interannual timescales are dominated by the El Niño-Southern Oscillation cycle. Sea salt variability on longer (interdecadal) timescales is associated with low-frequency variability in the Pacific Ocean similar to the Interdecadal Pacific Oscillation but does not show a statistically significant spectral peak. A multivariate regression suggests that sea salt aerosol variability may contribute to SWCF variability in the tropical Pacific, explaining up to 20-30% of the variance in that region. Elsewhere, there is only a small sea salt aerosol influence on SWCF through modifying cloud droplet number and liquid water path that contributes to the change of cloud effective radius and cloud optical depth (and hence cloud albedo), producing a multiyear aerosol-cloud-wind interaction

Interannual to decadal climate variability of sea salt aerosols in the coupled climate model CESM1.0

This study examines multiyear climate variability associated with sea salt aerosols and their contribution to the variability of shortwave cloud forcing (SWCF) using a 150 year simulation for preindustrial conditions of the Community Earth System Model version 1.0. The results suggest that changes in sea salt and related cloud and radiative properties on interannual timescales are dominated by the El Niño-Southern Oscillation cycle. Sea salt variability on longer (interdecadal) timescales is associated with low-frequency variability in the Pacific Ocean similar to the Interdecadal Pacific Oscillation but does not show a statistically significant spectral peak. A multivariate regression suggests that sea salt aerosol variability may contribute to SWCF variability in the tropical Pacific, explaining up to 20-30% of the variance in that region. Elsewhere, there is only a small sea salt aerosol influence on SWCF through modifying cloud droplet number and liquid water path that contributes to the change of cloud effective radius and cloud optical depth (and hence cloud albedo), producing a multiyear aerosol-cloud-wind interaction

Impacts of aerosol particles on the microphysical and radiative properties of stratocumulus clouds over the southeast Pacific Ocean

The southeast Pacific Ocean is covered by the world's largest stratocumulus cloud layer, which has a strong impact on ocean temperatures and climate in the region. The effect of anthropogenic sources of aerosol particles on the stratocumulus deck was investigated during the VOCALS field experiment. Aerosol measurements below and above cloud were made with a ultra-high sensitivity aerosol spectrometer and analytical electron microscopy. In addition to more standard in-cloud measurements, droplets were collected and evaporated using a counterflow virtual impactor (CVI), and the non-volatile residual particles were analyzed. Many flights focused on the gradient in cloud properties on an E-W track along 20° S from near the Chilean coast to remote areas offshore. Mean statistics, including their significance, from eight flights and many individual legs were compiled. Consistent with a continental source of cloud condensation nuclei, below-cloud accumulation-mode aerosol and droplet number concentration generally decreased from near shore to offshore. Single particle analysis was used to reveal types and sources of the enhanced particle number that influence droplet concentration. While a variety of particle types were found throughout the region, the dominant particles near shore were partially neutralized sulfates. Modeling and chemical analysis indicated that the predominant source of these particles in the marine boundary layer along 20° S was anthropogenic pollution from central Chilean sources, with copper smelters a relatively small contribution. Cloud droplets were smaller in regions of enhanced particles near shore. However, physically thinner clouds, and not just higher droplet number concentrations from pollution, both contributed to the smaller droplets. Satellite measurements were used to show that cloud albedo was highest 500–1000 km offshore, and actually slightly lower closer to shore due to the generally thinner clouds and lower liquid water paths there. Thus, larger scale forcings that impact cloud macrophysical properties, as well as enhanced aerosol particles, are important in determining cloud droplet size and cloud albedo. Differences in the size distribution of droplet residual particles and ambient aerosol particles were observed. By progressively excluding small droplets from the CVI sample, we were able to show that the larger drops, some of which may initiate drizzle, contain the largest aerosol particles. Geometric mean diameters of droplet residual particles were larger than those of the below-cloud and above cloud distributions. However, a wide range of particle sizes can act as droplet nuclei in these stratocumulus clouds. A detailed LES microphysical model was used to show that this can occur without invoking differences in chemical composition of cloud-nucleating particles

Observations of clouds, aerosols, precipitation, and surface radiation over the southern ocean

Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation, and radiative processes, and their interactions. Projects between 2016 and 2018 used in situ probes, radar, lidar, and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN), and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF-NCAR G-V aircraft flying north-south gradients south of Tasmania, at Macquarie Island, and on the R/V Investigator and RSV Aurora Australis. Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons. Results show largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multilayered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of dynamics and turbulence that likely drive heterogeneity of cloud phase. Satellite retrievals confirmed low clouds were responsible for radiation biases. The combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets