On the relationship between cloud water composition and cloud droplet number concentration.

Aerosol-cloud interactions are the largest source of uncertainty in quantifying anthropogenic radiative forcing. The large uncertainty is, in part, due to the difficulty of predicting cloud microphysical parameters, such as the cloud droplet number concentration (N d). Even though rigorous first-principle approaches exist to calculate N d, the cloud and aerosol research community also relies on empirical approaches such as relating N d to aerosol mass concentration. Here we analyze relationships between N d and cloud water chemical composition, in addition to the effect of environmental factors on the degree of the relationships. Warm, marine, stratocumulus clouds off the California coast were sampled throughout four summer campaigns between 2011 and 2016. A total of 385 cloud water samples were collected and analyzed for 80 chemical species. Single- and multispecies log-log linear regressions were performed to predict N d using chemical composition. Single-species regressions reveal that the species that best predicts N d is total sulfate ( R adj 2 = 0.40 ). Multispecies regressions reveal that adding more species does not necessarily produce a better model, as six or more species yield regressions that are statistically insignificant. A commonality among the multispecies regressions that produce the highest correlation with N d was that most included sulfate (either total or non-sea-salt), an ocean emissions tracer (such as sodium), and an organic tracer (such as oxalate). Binning the data according to turbulence, smoke influence, and in-cloud height allowed for examination of the effect of these environmental factors on the composition-N d correlation. Accounting for turbulence, quantified as the standard deviation of vertical wind speed, showed that the correlation between N d with both total sulfate and sodium increased at higher turbulence conditions, consistent with turbulence promoting the mixing between ocean surface and cloud base. Considering the influence of smoke significantly improved the correlation with N d for two biomass burning tracer species in the study region, specifically oxalate and iron. When binning by in-cloud height, non-sea-salt sulfate and sodium correlated best with N d at cloud top, whereas iron and oxalate correlated best with N d at cloud base.

Stratocumulus cloud clearings: statistics from satellites, reanalysis models, and airborne measurements.

This study provides a detailed characterization of stratocumulus clearings off the US West Coast using remote sensing, reanalysis, and airborne in situ data. Ten years (2009-2018) of Geostationary Operational Environmental Satellite (GOES) imagery data are used to quantify the monthly frequency, growth rate of total area (GRArea), and dimensional characteristics of 306 total clearings. While there is interannual variability, the summer (winter) months experienced the most (least) clearing events, with the lowest cloud fractions being in close proximity to coastal topographical features along the central to northern coast of California, including especially just south of Cape Mendocino and Cape Blanco. From 09:00 to 18:00 (PST), the median length, width, and area of clearings increased from 680 to 1231, 193 to 443, and ~ 67000 to ~ 250000km2, respectively. Machine learning was applied to identify the most influential factors governing the GRArea of clearings between 09:00 and 12:00PST, which is the time frame of most rapid clearing expansion. The results from gradient-boosted regression tree (GBRT) modeling revealed that air temperature at 850 hPa (T 850), specific humidity at 950 hPa (q 950), sea surface temperature (SST), and anomaly in mean sea level pressure (MSLPanom) were probably most impactful in enhancing GRArea using two scoring schemes. Clearings have distinguishing features such as an enhanced Pacific high shifted more towards northern California, offshore air that is warm and dry, stronger coastal surface winds, enhanced lower-tropospheric static stability, and increased subsidence. Although clearings are associated obviously with reduced cloud fraction where they reside, the domain-averaged cloud albedo was actually slightly higher on clearing days as compared to non-clearing days. To validate speculated processes linking environmental parameters to clearing growth rates based on satellite and reanalysis data, airborne data from three case flights were examined. Measurements were compared on both sides of the clear-cloudy border of clearings at multiple altitudes in the boundary layer and free troposphere, with results helping to support links suggested by this study's model simulations. More specifically, airborne data revealed the influence of the coastal low-level jet and extensive horizontal shear at cloud-relevant altitudes that promoted mixing between clear and cloudy air. Vertical profile data provide support for warm and dry air in the free troposphere, additionally promoting expansion of clearings. Airborne data revealed greater evidence of sea salt in clouds on clearing days, pointing to a possible role for, or simply the presence of, this aerosol type in clearing areas coincident with stronger coastal winds.

Relationships Between Supermicrometer Sea Salt Aerosol and Marine Boundary Layer Conditions: Insights From Repeated Identical Flight Patterns.

The MONterey Aerosol Research Campaign (MONARC) in May-June 2019 featured 14 repeated identical flights off the California coast over the open ocean at the same time each flight day. The objective of this study is to use MONARC data along with machine learning analysis to evaluate relationships between both supermicrometer sea salt aerosol number (N>1) and volume (V>1) concentrations and wind speed, wind direction, sea surface temperature (SST), ambient temperature (Tamb), turbulent kinetic energy (TKE), relative humidity (RH), marine boundary layer (MBL) depth, and drizzle rate. Selected findings from this study include the following: (i) Near surface (<60 m) N>1 and V>1 concentration ranges were 0.1-4.6 cm-3 and 0.3-28.2 µm3 cm-3, respectively; (ii) four meteorological regimes were identified during MONARC with each resulting in different N>1 and V>1 concentrations and also varying horizontal and vertical profiles; (iii) the relative predictive strength of the MBL properties varies depending on predicting N>1 or V>1, with MBL depth being more highly ranked for predicting N>1 and with TKE being higher for predicting V>1; (iv) MBL depths >400 m (<200 m) often correspond to lower (higher) N>1 and V>1 concentrations; (v) enhanced drizzle rates coincide with reduced N>1 and V>1 concentrations; (vi) N>1 and V>1 concentrations exhibit an overall negative relationship with SST and RH and an overall positive relationship with Tamb; and (vii) wind speed and direction were relatively weak predictors of N>1 and V>1.

Effects of Biomass Burning on Stratocumulus Droplet Characteristics, Drizzle Rate, and Composition.

This study reports on airborne measurements of stratocumulus cloud properties under varying degrees of influence from biomass burning (BB) plumes off the California coast. Data are reported from five total airborne campaigns based in Marina, California, with two of them including influence from wildfires in different areas along the coast of the western United States. The results indicate that subcloud cloud condensation nuclei number concentration and mass concentrations of important aerosol species (organics, sulfate, nitrate) were better correlated with cloud droplet number concentration (N d) as compared to respective above-cloud aerosol data. Given that the majority of BB particles resided above cloud tops, this is an important consideration for future work in the region as the data indicate that the subcloud BB particles likely were entrained from the free troposphere. Lower cloud condensation nuclei activation fractions were observed for BB-impacted clouds as compared to non-BB clouds due, at least partly, to less hygroscopic aerosols. Relationships between N d and either droplet effective radius or drizzle rate are preserved regardless of BB influence, indicative of how parameterizations can exhibit consistent skill for varying degrees of BB influence as long as N d is known. Lastly, the composition of both droplet residual particles and cloud water changed significantly when clouds were impacted by BB plumes, with differences observed for different fire sources stemming largely from effects of plume aging time and dust influence.

Aircraft Measurements of Total Mercury and Monomethyl Mercury in Summertime Marine Stratus Cloudwater from Coastal California, USA.

Water samples from marine stratus clouds were collected during 16 aircraft flights above the Pacific Ocean near the Central California coast during the summer of 2016. These samples were analyzed for total mercury (THg), monomethyl mercury (MMHg), and 32 other chemical species in addition to aerosol physical parameters. The mean concentrations of THg and MMHg in the cloudwater samples were 9.2 ± 6.0 ng L-1 (2.3-33.8 ng L-1) ( N = 97) and 0.87 ± 0.66 ng L-1 (0.17-2.9 ng L-1) ( N = 22), respectively. This corresponds to 9.5% (3-21%) MMHg as a fraction of THg. Low and high nonsea salt calcium ion (nss-Ca2+) concentrations in cloudwater were used to classify flights as "marine" and "continental", respectively. Mean [MMHg]marine was significantly higher ( p < 0.05) than [MMHg]continental consistent with an ocean source of dimethyl Hg (DMHg) to the atmosphere. Mean THg in cloudwater was not significantly different between the two categories, indicating multiple emissions sources. Mean [THg]continental was correlated with pH, CO, NO3-, NH4+, and other trace metals, whereas [THg]marine was correlated with MMHg and Na+. THg concentrations were negatively correlated with altitude, consistent with ocean and land emissions, coupled with removal at the cloud-top due to drizzle formation.

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.

Observations of sharp oxalate reductions in stratocumulus clouds at variable altitudes: organic acid and metal measurements during the 2011 E-PEACE campaign.

This work examines organic acid and metal concentrations in northeastern Pacific Ocean stratocumulus cloudwater samples collected by the CIRPAS Twin Otter between July and August 2011. Correlations between a suite of various monocarboxylic and dicarboxylic acid concentrations are consistent with documented aqueous-phase mechanistic relationships leading up to oxalate production. Monocarboxylic and dicarboxylic acids exhibited contrasting spatial profiles reflecting their different sources; the former were higher in concentration near the continent due to fresh organic emissions. Concentrations of sea salt crustal tracer species, oxalate, and malonate were positively correlated with low-level wind speed suggesting that an important route for oxalate and malonate entry in cloudwater is via some combination of association with coarse particles and gaseous precursors emitted from the ocean surface. Three case flights show that oxalate (and no other organic acid) concentrations drop by nearly an order of magnitude relative to samples in the same vicinity. A consistent feature in these cases was an inverse relationship between oxalate and several metals (Fe, Mn, K, Na, Mg, Ca), especially Fe. By means of box model studies we show that the loss of oxalate due to the photolysis of iron oxalato complexes is likely a significant oxalate sink in the study region due to the ubiquity of oxalate precursors, clouds, and metal emissions from ships, the ocean, and continental sources.

Worldwide data sets constrain the water vapor uptake coefficient in cloud formation.

Cloud droplet formation depends on the condensation of water vapor on ambient aerosols, the rate of which is strongly affected by the kinetics of water uptake as expressed by the condensation (or mass accommodation) coefficient, αc. Estimates of αc for droplet growth from activation of ambient particles vary considerably and represent a critical source of uncertainty in estimates of global cloud droplet distributions and the aerosol indirect forcing of climate. We present an analysis of 10 globally relevant data sets of cloud condensation nuclei to constrain the value of αc for ambient aerosol. We find that rapid activation kinetics (αc > 0.1) is uniformly prevalent. This finding resolves a long-standing issue in cloud physics, as the uncertainty in water vapor accommodation on droplets is considerably less than previously thought.

Comprehensive simultaneous shipboard and airborne characterization of exhaust from a modern container ship at sea.

We report the first joint shipboard and airborne study focused on the chemical composition and water-uptake behavior of particulate ship emissions. The study focuses on emissions from the main propulsion engine of a Post-Panamax class container ship cruising off the central coast of California and burning heavy fuel oil. Shipboard sampling included micro-orifice uniform deposit impactors (MOUDI) with subsequent off-line analysis, whereas airborne measurements involved a number of real-time analyzers to characterize the plume aerosol, aged from a few seconds to over an hour. The mass ratio of particulate organic carbon to sulfate at the base of the ship stack was 0.23 +/- 0.03, and increased to 0.30 +/- 0.01 in the airborne exhaust plume, with the additional organic mass in the airborne plume being concentrated largely in particles below 100 nm in diameter. The organic to sulfate mass ratio in the exhaust aerosol remained constant during the first hour of plume dilution into the marine boundary layer. The mass spectrum of the organic fraction of the exhaust aerosol strongly resembles that of emissions from other diesel sources and appears to be predominantly hydrocarbon-like organic (HOA) material. Background aerosol which, based on air mass back trajectories, probably consisted of aged ship emissions and marine aerosol, contained a lower organic mass fraction than the fresh plume and had a much more oxidized organic component. A volume-weighted mixing rule is able to accurately predict hygroscopic growth factors in the background aerosol but measured and calculated growth factors do not agree for aerosols in the ship exhaust plume. Calculated CCN concentrations, at supersaturations ranging from 0.1 to 0.33%, agree well with measurements in the ship-exhaust plume. Using size-resolved chemical composition instead of bulk submicrometer composition has little effect on the predicted CCN concentrations because the cutoff diameter for CCN activation is larger than the diameter where the mass fraction of organic aerosol begins to increase significantly. The particle number emission factor estimated from this study is 1.3 x 10(16) (kg fuel)(-1), with less than 1/10 of the particles having diameters above 100 nm; 24% of particles (>10 nm in diameter) activate into cloud droplets at 0.3% supersaturation.

On the source of organic acid aerosol layers above clouds.

During the July 2005 Marine Stratus/Stratocumulus Experiment (MASE) and the August-September 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter probed aerosols and cumulus clouds in the eastern Pacific Ocean off the coast of northern California and in southeastern Texas, respectively. An on-board particle-into-liquid sampler (PILS) quantified inorganic and organic acid species with < or = 5-min time resolution. Ubiquitous organic aerosol layers above cloud with enhanced organic acid levels were observed in both locations. The data suggest that aqueous-phase reactions to produce organic acids, mainly oxalic acid, followed by droplet evaporation is a source of elevated organic acid aerosol levels above cloud. Oxalic acid is observed to be produced more efficiently relative to sulfate as the cloud liquid water content increases, corresponding to larger and less acidic droplets. As derived from large eddy simulations of stratocumulus underthe conditions of MASE, both Lagrangian trajectory analysis and diurnal cloudtop evolution provide evidence that a significant fraction of the aerosol mass concentration above cloud can be accounted for by evaporated droplet residual particles. Methanesulfonate data suggest that entrainment of free tropospheric aerosol can also be a source of organic acids above boundary layer clouds.

Thunderstorm asthma.

Thunderstorms have often been linked to epidemics of asthma, especially during the grass flowering season; however, the precise mechanisms explaining this phenomenon are unknown. Evidence of high respirable allergen loadings in the air associated with specific meteorologic events combined with an analysis of pollen physiology suggests that rupture of airborne pollen can occur. Strong downdrafts and dry, cold outflows distinguish thunderstorm rain from frontal rain. The weather system of a mature thunderstorm likely entrains grass pollen into the cloud base, where pollen rupture would be enhanced, then transports the respirable-sized fragments of pollen debris to ground level where outflows distribute them ahead of the rain. The conditions occurring at the onset of a thunderstorm might expose susceptible people to a rapid increase in concentrations of pollen allergens in the air that can readily deposit in the lower airways and initiate asthmatic reactions.

Evidence for the predominance of mid-tropospheric aerosols as subtropical anvil cloud nuclei.

NASA's recent Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment focused on anvil cirrus clouds, an important but poorly understood element of our climate system. The data obtained included the first comprehensive measurements of aerosols and cloud particles throughout the atmospheric column during the evolution of multiple deep convective storm systems. Coupling these new measurements with detailed cloud simulations that resolve the size distributions of aerosols and cloud particles, we found several lines of evidence indicating that most anvil crystals form on mid-tropospheric rather than boundary-layer aerosols. This result defies conventional wisdom and suggests that distant pollution sources may have a greater effect on anvil clouds than do local sources.