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Cloud responses to changes in aerosol remain a dominant uncertainty in the radiative forcing of climate. Two main constructs related to aerosol effects on clouds have been postulated: (i) the “albedo effect” whereby anthropogenic aerosol results in increased droplet concentrations that generate increases in cloud albedo, all else (particularly cloud water) being equal; (ii) the “lifetime effect” whereby anthropogenic aerosol suppresses precipitation and results in clouds with more liquid water, higher fractional cloudiness, and longer lifetimes. Based on new observations presented here, and supported by previous fine‐scale modeling studies, we suggest that the balance of evidence shows that non‐precipitating cumulus clouds can experience an evaporation‐entrainment feedback, and respond to aerosol perturbations in a manner inconsistent with the traditional “lifetime effect.” Because most cumulus clouds evaporate without producing significant precipitation, this is particularly relevant to estimates of aerosol indirect effects on climate.

This study examines the role of aerosol in mediating interactions between a warm trade cumulus cloud system and the environment that spawns it. Numerical simulations of the observed and well-studied Rain in Cumulus over the Ocean (RICO) field experiment are performed. The results draw on simulations of 34-h duration so as to avoid conclusions based on transients. Simulations show that, on average, aerosol-perturbed clouds are initially deeper and more vigorous but that after about 14 h there is a reversal in this trend, and unperturbed clouds deepen relative to the perturbed clouds. Differences in cloud depth are about 100 m, and differences in vertical velocity variance are about 30%. After about 20 h, most cloud fields are statistically similar with the exception of rain rate and optical depth, which are lower and higher, respectively, in the high-aerosol conditions. By sampling the model output at various points in the cloud system evolution, the mechanisms responsible for the initial differences and then convergence of most of the cloud field properties are addressed. Sensitivity tests indicate that responses are driven primarily by temperature profiles, rather than by humidity profiles, and that the general trend to homogenization of the bulk cloud field properties is robust for different forcings. Finally, the paper shows that even transient aerosol perturbations may endure beyond the duration of the perturbation itself, provided they persist long enough. Short-duration aerosol perturbations are unlikely to have much influence on the system.

Aircraft measurements during the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) are used to examine the influence of shallow cumulus clouds on vertical profiles of aerosol chemical composition, size distributions, and secondary aerosol precursor gases. The data show signatures of convective transport of particles, gases and moisture from near the surface to higher altitudes, and of aqueous‐phase production of aerosol mass (sulfate and organics) in cloud droplets and aerosol water. In cloudy conditions, the average aerosol volume concentration at an altitude of 2850 m, above typical cloud top levels, was found to be 34% of that at 450 m; for clear conditions, the same ratio was 13%. Both organic and sulfate mass fractions were on average constant with altitude (around 50%); however, the ratio of oxalate to organic mass increased with altitude (from 1% at 450 m to almost 9% at 3450 m), indicative of the influence of in‐cloud production on the vertical abundance and characteristics of secondary organic aerosol (SOA) mass. A new metric termed “residual cloud fraction” is introduced as a way of quantifying the “cloud processing history” of an air parcel. Results of a parcel model simulating aqueous phase production of sulfate and organics reproduce observed trends and point at a potentially important role of SOA production, especially oligomers, in deliquesced aerosols. The observations emphasize the importance of shallow cumulus clouds in altering the vertical distribution of aerosol properties that influence both their direct and indirect effect on climate. Key Points Shallow cumulus convection impacts aerosol vertical abundance Aqueous‐phase processes change aerosol chemical composition with altitude Soluble VOCs exist at cloud‐relevant altitudes

The global chemical transport model GEOS‐Chem, implemented with a dust‐iron dissolution scheme, was used to analyze the magnitude and spatial distribution of mineral dust and soluble‐iron (sol‐Fe) deposition to the South Atlantic Ocean (SAO). The comparison of model results with remotely sensed data shows that GEOS‐Chem can capture dust source regions in Patagonia and characterize the temporal variability of dust outflow. For a year‐long model simulation, 22 Tg of mineral dust and 4 Gg of sol‐Fe were deposited to the surface waters of the entire SAO region, with roughly 30% of this dust and sol‐Fe predicted to be deposited to possible high nitrate low chlorophyll oceanic regions. Model‐predicted dissolved iron fraction of mineral dust over the SAO was small, on average only accounting for 0.57% of total iron. Simulations suggest that the primary reason for such a small fraction of sol‐Fe is the low ambient concentrations of acidic trace gases available for mixing with dust plumes. Overall, the amount of acid added to the deliquesced aerosol solution was not enough to overcome the alkalinity buffer of Patagonian dust and initiate considerable acid dissolution of mineral‐iron. Sensitivity studies show that the amount of sol‐Fe deposited to the SAO was largely controlled by the initial amount of sol‐Fe at the source region, with limited contribution from the spatial variability of Patagonian‐desert topsoil mineralogy and natural sources of acidic trace gases. Simulations suggest that Patagonian dust should have a minor effect on biological productivity in the SAO.

We analyse the cloud microphysical response to entrainment mixing in warm cumulus clouds observed from the CIRPAS Twin Otter during the GoMACCS field campaign near Houston, Texas, in summer 2006. Cloud drop size distributions and cloud liquid water contents from the Artium Flight phase-Doppler interferometer in conjunction with meteorological observations are used to investigate the degree to which inhomogeneous versus homogeneous mixing is preferred as a function of height above cloud base, distance from cloud edge and aerosol concentration. Using four complete days of data with 101 cloud penetrations (minimum 300 m in length), we find that inhomogeneous mixing primarily explains liquid water variability in these clouds. Furthermore, we show that there is a tendency for mixing to be more homogeneous towards the cloud top, which we attribute to the combination of increased turbulent kinetic energy and cloud drop size with altitude which together cause the Damköhler number to increase by a factor of between 10 and 30 from cloud base to cloud top. We also find that cloud edges appear to be air from cloud centres that have been diluted solely through inhomogeneous mixing. Theory predicts the potential for aerosol to affect mixing type via changes in drop size over the range of aerosol concentrations experienced (moderately polluted rural sites to highly polluted urban sites). However, the observations, while consistent with this hypothesis, do not show a statistically significant effect of aerosol on mixing type.

Cloud drop number concentration (Nd) can be retrieved through passive satellite observation. These retrievals are useful due to their wide spatial and temporal coverage. However, the accuracy of the retrieved values is not well understood. In this study, we seek to understand why the retrievals agree or disagree with in situ measurements by examining the various cloud properties that underlie the retrievals. To do so, we compare satellite Nd derived from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument with in situ aircraft measurements made using a phase Doppler interferometer on board three flight campaigns sampling marine stratocumulus clouds. Intercomparison of Nd values shows that the discrepancy between retrieved and in situ Nd can be ± 50 % or more. In the mean, there is evidence of an overestimation bias by MODIS retrievals, although the sample size is insufficient for statistical certainty. We find that MODIS Nd is best interpreted as representative of the mid-cloud region, as there is almost always a greater discrepancy from in situ values near the cloud top and cloud base. We also find evidence of cases where Nd is accurately retrieved but the effective radius is not, presumably due to offsetting errors in other retrieval parameters. Vertical profiles of the extinction coefficient β, liquid water content L, and effective radius re measured during sawtooth-pattern flight legs through the cloud top are also compared to implicit MODIS retrieval profiles. For the two cases with Nd agreement, all profiles match well. For the six cases with significant disagreement, there is no consistent underlying cause. The discrepancy originates from one of the following: (a) discrepancy in the re profile, (b) discrepancy in the β and L profiles, or (c) discrepancy in both.

Sub-cloud rain evaporation in the trade wind region significantly influences the boundary layer mass and energy budgets. Parameterizing it is, however, difficult due to the sparsity of well-resolved rain observations and the challenges of sampling short-lived marine cumulus clouds. In this study, sub-cloud rain evaporation is analyzed using a steady-state, one-dimensional model that simulates changes in drop sizes, relative humidity, and rain isotopic composition. The model is initialized with relative humidity, raindrop size distributions, and water vapor isotope ratios (e.g., δDv, δ18Ov) sampled by the NOAA P3 aircraft during the Atlantic Tradewind Ocean–Atmosphere Mesoscale Interaction Campaign (ATOMIC), which was part of the larger EUREC4A (ElUcidating the RolE of Clouds–Circulation Coupling in ClimAte) field program. The modeled surface precipitation isotope ratios closely match the observations from EUREC4A ground-based and ship-based platforms, lending credibility to our model. The model suggests that 63 % of the rain mass evaporates in the sub-cloud layer across 22 P3 cases. The vertical distribution of the evaporated rain flux is top heavy for a narrow (σ) raindrop size distribution (RSD) centered over a small geometric mean diameter (Dg) at the cloud base. A top-heavy profile has a higher rain-evaporated fraction (REF) and larger changes in the rain deuterium excess (d=δD-8×δ18O) between the cloud base and the surface than a bottom-heavy profile, which results from a wider RSD with larger Dg. The modeled REF and change in d are also more strongly influenced by cloud base Dg and σ rather than the concentration of raindrops. The model results are accurate as long as the variations in the relative humidity conditions are accounted for. Relative humidity alone, however, is a poor indicator of sub-cloud rain evaporation. Overall, our analysis indicates the intricate dependence of sub-cloud rain evaporation on both thermodynamic and microphysical processes in the trade wind region.

Two case studies of marine stratocumulus (one nocturnal and drizzling, the other daytime and nonprecipitating) are simulated by the UCLA large-eddy simulation model with bin microphysics for comparison with aircraft in situ observations. A high-bin-resolution variant of the microphysics is implemented for closer comparison with cloud drop size distribution (DSD) observations and a turbulent collision–coalescence kernel to evaluate the role of turbulence on drizzle formation. Simulations agree well with observational constraints, reproducing observed thermodynamic profiles (i.e., liquid water potential temperature and total moisture mixing ratio) as well as liquid water path. Cloud drop number concentration and liquid water content profiles also agree well insofar as the thermodynamic profiles match observations, but there are significant differences in DSD shape among simulations that cause discrepancies in higher-order moments such as sedimentation flux, especially as a function of bin resolution. Counterintuitively, high-bin-resolution simulations produce broader DSDs than standard resolution for both cases. Examination of several metrics of DSD width and percentile drop sizes shows that various discrepancies of model output with respect to the observations can be attributed to specific microphysical processes: condensation spuriously creates DSDs that are too wide as measured by standard deviation, which leads to collisional production of too many large drops. The turbulent kernel has the greatest impact on the low-bin-resolution simulation of the drizzling case, which exhibits greater surface precipitation accumulation and broader DSDs than the control (quiescent kernel) simulations. Turbulence effects on precipitation formation cannot be definitively evaluated using bin microphysics until the artificial condensation broadening issue has been addressed.

This study uses airborne data from two field campaigns off the California coast to characterize aerosol size distribution characteristics in the entrainment interface layer (EIL), a thin and turbulent layer above marine stratocumulus cloud tops, which separates the stratocumulus-topped boundary layer (STBL) from the free troposphere (FT). The vertical bounds of the EIL are defined in this work based on considerations of buoyancy and turbulence using thermodynamic and dynamic data. Aerosol number concentrations are examined from three different probes with varying particle diameter (Dp) ranges: > 3 nm, > 10 nm, and 0.11–3.4 µm. Relative to the EIL and FT layers, the sub-cloud (SUB) layer exhibited lower aerosol number concentrations and higher surface area concentrations. High particle number concentrations between 3 and 10 nm in the EIL are indicative of enhanced nucleation, assisted by high actinic fluxes, cool and moist air, and much lower surface area concentrations than the STBL. Slopes of number concentration versus altitude in the EIL were correlated with the particle number concentration difference between the SUB and lower FT layers. The EIL aerosol size distribution was influenced by varying degrees from STBL aerosol versus subsiding FT aerosol depending on the case examined. These results emphasize the important role of the EIL in influencing nucleation and aerosol–cloud–climate interactions.

Measuring emissions from stacks is challenging due to accessibility and safety concerns and requires techniques to address a broad range of conditions and measurement challenges. One way to facilitate such measurements is to build an instrument package and then use a crane to hold the package over the emissions source. Here we describe such an instrument package that is used to characterize both wet droplet and dried aerosol emissions from cooling tower spray drift. In this application, the instrument package characterizes the velocity, size distribution, and concentration of the wet droplet emissions and the mass concentration and elemental composition of the dried PM2.5 and PM10 emissions. Subsequent papers will present and analyze the wet and dried emissions from individual towers.