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The impact of giant sea salt aerosols released from breaking waves on rain formation in marine boundary layer clouds is studied using large-eddy simulations (LES). We perform simulations of marine cumuli and stratocumuli for various concentrations of cloud condensation nuclei (CCN) and giant CCN (GCCN). Cloud microphysics are modeled with a Lagrangian method that provides key improvements in comparison to previous LES of GCCN that used Eulerian bin microphysics. We find that GCCN significantly increase precipitation in stratocumuli. This effect is strongest for low and moderate CCN concentrations. GCCN are found to have a smaller impact on precipitation formation in cumuli. These conclusions are in agreement with field measurements. We develop a simple parameterization of the effect of GCCN on precipitation, accretion, and autoconversion rates in marine stratocumuli. Significance Statement Breaking sea waves release salt particles into the atmosphere. Cloud droplets formed on these salt particles can grow larger than droplets formed on other smaller particles. Therefore, sea salt particles can be important for rain formation over oceans. To investigate this effect, we performed idealized computer simulations of stratocumulus and cumulus clouds. Sea salt particles were modeled with an unprecedented precision thanks to the use of an emerging modeling method. In our simulations sea salt particles significantly enhance rain formation in stratocumuli, but not in cumuli. Our study has implications for climate models, because stratocumuli are important for Earth’s energy budget and for rain enhancement experiments.

The most basic aspect of cloud formation is condensational growth onto cloud condensation nuclei (CCN). As such, condensational growth of cloud drops is often assumed to be a well-understood process described by the drop growth equation. When this process is represented in models, CCN activate into cloud drops at cloud base, and it is often assumed that drops consist of pure water or that the hygroscopic contribution after drop activation is small because of the inclusion of only small CCN. Drop growth rate in adiabatic ascent in such models is proportional to supersaturation and assumed to be inversely proportional to the drop radius, thereby making the drop spectrum narrow with altitude. However, the present study demonstrates that drop growth on giant sea-salt aerosol particles (GCCN; dry radius 0.5 m) behaves differently. For typical marine stratocumulus updrafts and for drops grown on GCCN with sizes m, these drops typically remain concentrated salt solutions. Because of this, their condensational growth is accelerated, and they rapidly attain precipitation drop sizes through condensation only. Additionally, drops formed on GCCN may also grow by condensation in cloudy downdrafts. The strong effect of condensation on GCCN is important when carried through to calculating rain-rate contribution as a function of aerosol size. GCCN larger than 2 m account for most of the rainfall rate in the modeled precipitating marine stratocumulus.

Aerosols influence cloud and precipitation development in complex ways due to myriad feedbacks at a variety of scales from individual clouds through entire storm systems. This paper describes the implementation, testing, and results of a newly modified bulk microphysical parameterization with explicit cloud droplet nucleation and ice activation by aerosols. Idealized tests and a high-resolution, convection-permitting, continental-scale, 72-h simulation with five sensitivity experiments showed that increased aerosol number concentration results in more numerous cloud droplets of overall smaller size and delays precipitation development. Furthermore, the smaller droplet sizes cause the expected increased cloud albedo effect and more subtle longwave radiation effects. Although increased aerosols generally hindered the warm-rain processes, regions of mixed-phase clouds were impacted in slightly unexpected ways with more precipitation falling north of a synoptic-scale warm front. Aerosol impacts to regions of light precipitation, less than approximately 2.5 mm h−1, were far greater than impacts to regions with higher precipitation rates. Comparisons of model forecasts with five different aerosol states versus surface precipitation measurements revealed that even a large-scale storm system with nearly a thousand observing locations did not indicate which experiment produced a more correct final forecast, indicating a need for far longer-duration simulations due to the magnitude of both model forecast error and observational uncertainty. Last, since aerosols affect cloud and precipitation phase and amount, there are resulting implications to a variety of end-user applications such as surface sensible weather and aircraft icing.

The impact of aerosol replenishment in a stratocumulus-topped boundary layer (STBL) on cloud morphology and albedo is examined using a large-eddy simulation (LES) model in conjunction with a prey–predator-type dynamical model following Koren and Feingold. In both the LES and the prey–predator models, the aerosol replenishment is represented as a relaxation term toward an ambient aerosol concentration with a time scale . The LESs suggest the existence of three distinct cloud regimes corresponding to different aerosol relaxation times. Specifically, for a small , the simulations are characterized by a large aerosol concentration, weak precipitation, relatively thick cloud depth, and closed cells. For a moderate , the simulated clouds exhibit open cellular patterns, in accordance with low aerosol concentration and moderate precipitation that oscillates in time. For a large , the aerosol may be depleted by intense drizzling and accordingly the cloud disappears. The critical aerosol relaxation times that separate these regimes vary with the ambient aerosol number concentration and cloud depth. Solutions from the low-order dynamical model with parameters relevant to the LESs are in general consistent with the LES results and provide further insight into the interplay among clouds, aerosol, and precipitation.

Coastal and island Aerosol Robotic Network (AERONET) sites are used to determine characteristic aerosol modes over marine environments. They are compared with the assumed modes used in the operational Moderate Resolution Imaging Spectroradiometer (MODIS) ocean aerosol algorithm, and the results show that 1) the standard deviation values of three fine aerosol modes (0.6) and one dustlike aerosol mode (0.8) are much higher than the corresponding statistical AERONET modal values (0.45 and 0.6, respectively). The values of three sea salt aerosol modes (0.6) are somewhat lower than the corresponding statistical AERONET modal value (0.675). 2) The number median radius of the current fine and dustlike aerosol modes cannot span the dynamic range of corresponding aerosol distribution properly. 3) AERONET products show that the standard deviation and the number median radius exhibit an obvious negative correlation, especially for sea salt and dustlike aerosol modes. According to this, a refinement of the current aerosol modes is made. These revised modes are used in a version of the MODIS retrieval over ocean. Compared with the current aerosol modes: 1) more retrieved aerosol optical depths (AODs) from the revised aerosol modes lie within the expected error bars and 2) the linear regression lines of the retrievals from the revised aerosol modes and AERONET are closer to the 1:1 line.

A large fraction of the atmospheric aerosol load reaching the free troposphere is frequently located above low clouds. Most commonly observed aerosols above clouds are carbonaceous particles generally associated with biomass burning and boreal forest fires, and mineral aerosols originating in arid and semiarid regions and transported across large distances, often above clouds. Because these aerosols absorb solar radiation, their role in the radiative transfer balance of the earth–atmosphere system is especially important. The generally negative (cooling) top-of-the-atmosphere direct effect of absorbing aerosols may turn into warming when the light-absorbing particles are located above clouds. The actual effect depends on the aerosol load and the single scattering albedo, and on the geometric cloud fraction. In spite of its potential significance, the role of aerosols above clouds is not adequately accounted for in the assessment of aerosol radiative forcing effects due to the lack of measurements. This paper discusses the basis of a simple technique that uses near-UV observations to simultaneously derive the optical depth of both the aerosol layer and the underlying cloud for overcast conditions. The two-parameter retrieval method described here makes use of the UV aerosol index and reflectance measurements at 388 nm. A detailed sensitivity analysis indicates that the measured radiances depend mainly on the aerosol absorption exponent and aerosol–cloud separation. The technique was applied to above-cloud aerosol events over the southern Atlantic Ocean, yielding realistic results as indicated by indirect evaluation methods. An error analysis indicates that for typical overcast cloudy conditions and aerosol loads, the aerosol optical depth can be retrieved with an accuracy of approximately 54% whereas the cloud optical depth can be derived within 17% of the true value.

The impacts of urban aerosols on clouds and precipitation are investigated using a spectral (bin) microphysics cloud model. For this purpose, extensive numerical experiments with various aerosol concentrations are performed under different environmental moisture conditions. To take into account the urban heat island and urban air pollution, it is considered that there is low-level heating in the urban area and that the aerosol concentration in the urban area is higher than that in the surrounding rural area. Simulation results show that a low-level updraft induced by the urban heat island leads to the formation of a low-level cloud and then a deep convective cloud downwind of the urban area. The onset of precipitation produced by the low-level cloud is delayed at higher aerosol concentrations. This is because when the aerosol concentration is high, a narrow drop size distribution results in a suppressed collision–coalescence process and hence in late raindrop formation. However, after the deep convective cloud develops, a higher aerosol concentration generally leads to the development of a stronger convective cloud. This is mainly due to increased release of latent heat resulting from the enhanced condensation process with increasing aerosol concentration. The low collision efficiency of smaller cloud drops and the resulting stronger updraft at higher aerosol concentrations result in higher liquid water content at higher levels, leading to the enhanced riming process to produce large ice particles. The melting of a larger amount of hail leads to precipitation enhancement downwind of the urban area with increasing urban aerosol concentration in all moisture environments considered.

The net shortwave radiative impact of aerosol on simulations of two shallow marine cloud cases is investigated using a Monte Carlo radiative transfer model. For a shallow cumulus case, increased aerosol concentrations are associated not only with smaller droplet sizes but also reduced cloud fractions and cloud dimensions, a result of evaporation-induced mixing and a lack of precipitation. Three-dimensional radiative transfer (3DRT) effects alter the fluxes by 10%–20% from values calculated using the independent column approximation for these simulations. The first (Twomey) aerosol indirect effect is dominant but the decreased cloud fraction reduces the magnitude of the shortwave cloud forcing substantially. The 3DRT effects slightly decrease the sensitivity of the cloud albedo to changes in droplet size under an overhead sun for the two ranges of cloud liquid water paths examined, but not strongly so. A popular two-stream radiative transfer approximation to the cloud susceptibility overestimates the more directly calculated values for the low liquid-water-path clouds within pristine aerosol conditions by a factor of 2 despite performing well otherwise, suggesting caution in its application to the cloud albedos within broken cloud fields. An evaluation of the influence of cloud susceptibility and cloud fraction changes to a “domain” area-weighted cloud susceptibility found that the domain cloud albedo is more likely to increase under aerosol loading at intermediate aerosol concentrations than under the most pristine conditions, contrary to traditional expectations. The second simulation (cumulus penetrating into stratus) is characterized by higher cloud fractions and more precipitation. This case has two regimes: a clean, precipitating regime where cloud fraction increases with increasing aerosol, and a more polluted regime where cloud fraction decreases with increasing aerosol. For this case the domain-mean cloud albedo increases steadily with aerosol loading under clean conditions, but increases only slightly after the cloud coverage decreases. Three-dimensional radiative transfer effects are mostly negligible for this case. Both sets of simulations suggest that aerosol-induced cloud fraction changes must be considered in tandem with the Twomey effect for clouds of small dimensions when assessing the net radiative impact, because both effects are drop size dependent and radiatively significant.

The effects of aerosol on warm trade cumulus clouds are investigated using a large-eddy simulation with size-resolved cloud microphysics. It is shown that, as expected, increases in aerosols cause a reduction in precipitation and an increase in the cloud-averaged liquid water path (LWP). However, for the case under study, cloud fraction, cloud size, cloud-top height, and depth decrease in response to increasing aerosol concentration, contrary to accepted hypotheses associated with the second aerosol indirect effect. It is found that the complex responses of clouds to aerosols are determined by competing effects of precipitation and droplet evaporation associated with entrainment. As aerosol concentration increases, precipitation suppression tends to maintain the clouds and lead to higher cloud LWP, whereas cloud droplets become smaller and evaporate more readily, which tends to dissipate the clouds and leads to lower cloud fraction, cloud size, and depth. An additional set of experiments with higher surface latent heat flux, and hence higher LWP and drizzle rate, was also performed. Changes in cloud properties due to aerosols have the same trends as in the base runs, although the magnitudes of the changes are larger. Evidence for significant stabilization (or destabilization) of the subcloud layer due to drizzle is not found, mainly because drizzling clouds cover only a small fraction of the domain. It is suggested that cloud fraction may only increase with increasing aerosol loading for larger clouds that are less susceptible to entrainment and evaporation. Finally, it is noted that at any given aerosol concentration the dynamical variability in bulk cloud parameters such as LWP tends to be larger than the aerosol-induced changes in these parameters, indicating that the second aerosol indirect effect may be hard to measure in this cloud type. The variability in cloud optical depth is, however, dominated by changes in aerosol, rather than dynamics.

Large concentrations of small aerosols have been previously observed in the vicinity of anvils of convective clouds. A 3D cloud-resolving model (CRM) including an explicit size-resolving aerosol module has been used to examine the origin of these aerosols. Five different types of aerosols are considered: nucleation mode sulfate aerosols (here defined by 0 ≤ d ≤5.84 nm), Aitken mode sulfate aerosols (here defined by 5.84 nm ≤ d ≤ 31.0 nm), accumulation mode sulfate aerosols (here defined by d ≥ 31.0 nm), mixed aerosols, and black carbon aerosols. The model results suggest that approximately 10% of the initial boundary layer number concentration of Aitken mode aerosols and black carbon aerosols are present at the top of the convective cloud as the cloud reaches its decaying state. The simulated average number concentration of Aitken mode aerosols in the cloud anvil (∼1.6 × 104 cm−3) is in the same order of magnitude as observations. Thus, the model results strongly suggest that vertical convective transport, particularly during the active period of the convection, is responsible for a major part of the appearance of high concentrations of small aerosols (corresponding to the Aitken mode in the model) observed in the vicinity of cloud anvils. There is some formation of new aerosols within the cloud, but the formation is small. Nucleation mode aerosols are also efficiently scavenged through impaction scavenging by precipitation. Accumulation mode and mixed mode aerosols are efficiently scavenged through nucleation scavenging and their concentrations in the cloud anvil are either very low (mixed mode) or practically zero (accumulation mode). In addition to the 3D CRM, a box model, including important features of the aerosol module of the 3D model, has been used to study the formation of new aerosols after the cloud has evaporated. The possibility of these aerosols to grow to suitable cloud condensation or ice nuclei size is also examined. Concentrations of nucleation mode aerosols up to 3 × 104 cm−3 are obtained. The box model simulations thus suggest that new particle formation is a substantial source of small aerosols in the upper troposphere during and after the dissipation of the convective cloud. Nucleation mode and Aitken mode aerosols grow due to coagulation and condensation of H2SO4 on the aerosols, but the growth rate is low. Provided that there is enough OH available to oxidize SO2, parts of the aerosol population (∼400 cm−3) can reach the accumulation mode size bin of the box model after 46 h of simulation.

The indirect effect of aerosols on water clouds, whereby aerosol particles change cloud optical properties, is caused by aerosol-induced changes of the size and number of cloud droplets. This affects the lifetime of the water clouds as well as their shortwave radiative properties. In addition, anthropogenic aerosols may change the properties of ice-forming nuclei. To investigate the potential effect of aerosol–ice cloud interactions by contact freezing, a prognostic equation for the number concentration of ice crystals is introduced into the ECMWF–Hamburg (ECHAM4) GCM. A simulation in which the number of contact ice nuclei is considered to be only temperature dependent is compared to simulations in which contact ice nuclei are considered to be dust aerosols. If dust aerosols are assumed to lose their nucleability by forming an internally mixed aerosol with sulfate, then the ice formation is slightly inhibited. On the contrary, if all contact nuclei are assumed to be insoluble carbonaceous aerosol...

The influence of sea salt on the cloud droplet activation of sulfate particles is investigated using a size-resolving model of the aerosol activation process. The authors found that the total number concentration of activated cloud droplets increases with increasing sea salt concentration if the sulfate number concentrations are relatively low and updrafts are strong, but it decreases with higher sea salt if sulfate number concentrations are high and cloud updrafts are weak. The increase is due to the activation of accumulation mode sea salt particles, while the decrease is due to the reduction in maximum cloud supersaturation due to competition with coarse mode sea salt particles. These conclusions are insensitive to the sulfate size distribution and surface wind speed.

By increasing droplet concentration and thereby the optical thickness of a cloud, pollution acts to increase the reflectance (albedo) of clouds; by increasing the absorption coefficient it acts to decrease the reflectance. Calculations suggest that the former effect (brightening of the clouds in reflection, hence climatically a cooling effect) dominates for thin to moderately thick clouds, whereas for sufficiently thick clouds the latter effect (climatically a warming effect) can become dominant.

An atmospheric boundary layer (ABL) model is used to address problems involving the generation, turbulent transport, and deposition of giant sized (1–25 μm) sea-salt aerosol. The surface aerosol generation rate is taken from the production flux expressions developed by Monahan. A simplified second-moment closure formulation for turbulent transport is used, while dry deposition fluxes are computed as functions of Stokes' settling speed and the rate of inertial impaction of particles across the viscous sublayer. Initially we investigate, starting from first principles, whether the model can develop reasonable sea-salt volume distributions at several different Beaufort wind forces Using the empirical expressions for generation and deposition fluxes, we permit an initially aerosol-free ABL to fill by diffusion until the volume distributions approach equilibrium., we then compare these distributions with the classic Woodcock observations. Further experiments are conducted in which we explore the dynam...

Numerical computations have been performed to study the effect on the characteristics of a condensationally produced droplet size distribution of a variability in the kind and fraction of soluble material among atmospheric aerosol particles. The model aerosol used in the study is assumed to be comprised only of nuclei containing 1, 10, 50 and 90% soluble material and to have a particle size distribution equal to the mean of the model continental and maritime aerosol size distributions described by Junge and McLaren. The soluble constituent of the nuclei is taken to be ammonium sulfate. Droplet size distributions are computed for a height of 150 m above cloud base. The computations show that the droplet size distribution resulting from condensation upon a population of mixed nuclei (i.e., nuclei composed of both soluble and insoluble components) is not broader than that produced by condensation upon a population of pure salt nuclei. Further, the dispersion of cloud droplet sizes is found to be qui...

Cloud nuclei spectra have been calculated as a function of aerosol size distribution and soluble salt content. Size distribution of the nucleating aerosol is shown to be the most important factor in determining the cloud nuclei spectra, with compositional variations being significant only for aerosols with less than 10% soluble material. Variations in the physical parameters entering into the calculations do not affect the results for normal aerosols. Comparison with some observed spectra shows both similarities and differences which should be useful in gaining more understanding of cloud nuclei spectra and unusual aerosol distributions.

Changes in aerosol concentrations could imply changes in cloud condensation nuclei concentrations, which could in turn affect cloud optical properties. Calculations made with a one-dimensional radiative-convective model show that this can be a significant mechanism for climate change.