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At least 91 records · Page 5

The Association Between Cloud Droplet Number over the Summer Southern Ocean and Air Mass History

The cloud properties and governing processes in Southern Ocean marine boundary layer clouds have emerged as a central issue in understanding the Earth's climate sensitivity. While our understanding of Southern Ocean cloud feedbacks have evolved in the most recent climate model intercomparison, the background properties of simulated summertime clouds in the Southern Ocean are not consistent with measurements due to known biases in simulating cloud condensation nuclei concentrations. This paper presents several case studies collected during the Capricorn 2 and Marcus campaigns held aboard Australian research vessels in the Austral Summer of 2018. Combining the surface–observed cases with MODIS data along forward and backward air mass trajectories, we demonstrate the evolution of cloud properties with time. These cases are consistent with multi–year statistics showing that long trajectories of air masses over the Antarctic ice sheet are critical to creating high droplet number clouds in the high latitude summer Southern Ocean. We speculate that secondary aerosol production via the oxidation of biogenically derived aerosol precursor gasses over the high actinic flux region of the high latitude ice sheets is fundamental to maintaining relatively high droplet numbers in Southern Ocean clouds during Summer.

54 ENVIRONMENTAL SCIENCES↗

Global Distribution of Cloud Droplet Number Concentration, Autoconversion Rate, and Aerosol Indirect Effect Under Diabatic Droplet Activation

This study presents a global assessment of the sensitivity of droplet number to diabatic activation (i.e., including effects from entrainment of dry air) and its first-order tendency on indirect forcing and autoconversion. Simulations were carried out with the NASA Global Modeling Initiative (GMI) atmospheric and transport model using climatological metereorological fields derived from the former NASA Data Assimilation Office (DAO), the NASA Finite volume GCM (FVGCM) and the Goddard Institute for Space Studies version II (GISS) GCM. Cloud droplet number concentration (CDNC) is calculated using a physically based prognostic parameterization that explicitly includes entrainment effects on droplet formation. Diabatic activation results in lower CDNC, compared to adiabatic treatment of the process. The largest decrease in CDNC (by up to 75 percent) was found in the tropics and in zones of moderate CCN concentration. This leads to a global mean effective radius increase between 0.2-0.5 micrometers (up to 3.5 micrometers over the tropics), a global mean autoconversion rate increase by a factor of 1.1 to 1.7 (up to a factor of 4 in the tropics), and a 0.2-0.4 W m(exp -2) decrease in indirect forcing. The spatial patterns of entrainment effects on droplet activation tend to reduce biases in effective radius (particularly in the tropics) when compared to satellite retrievals. Considering the diabatic nature of ambient clouds, entrainment effects on CDNC need to be considered in GCM studies of the aerosol indirect effect.

Barahona, Donifan↗

Effects of Nonsphericity on the Behavior of Lorenz-Mie Resonances in Scattering Characteristics of Liquid-Cloud Droplets

By using the results of highly accurate T-matrix computations for randomly oriented oblate and prolate spheroids and Chebyshev particles with varying degrees of asphericity, we analyze the effects of a deviation of water-droplet shapes from that of a perfect sphere on the behavior of Lorenz-Mie morphology-dependent resonances of various widths. We demonstrate that the positions and profiles of the resonances can change significantly with increasing asphericity. The absolute degree of asphericity required to suppress a Lorenz-Mie resonance is approximately proportional to the resonance width. Our results imply that numerical averaging of scattering characteristics of real cloud droplets over sizes may rely on a significantly coarser size-parameter resolution than that required for ideal, perfectly spherical particles.

matrices (mathematics)↗

Chemical consequences of the initial diffusional growth of cloud droplets - A clean marine case

A simple microphysical cloud parcel model and a simple representation of the background marine aerosol are used to predict the concentrations and compositions of droplets of various sizes near cloud base. The aerosol consists of an externally-mixed ammonium bisulfate accumulation mode and a sea-salt coarse particle mode. The difference in diffusional growth rates between the small and large droplets as well as the differences in composition between the two aerosol modes result in substantial differences in solute concentration and composition with size of droplets in the parcel. The chemistry of individual droplets is not, in general, representative of the bulk (volume-weighted mean) cloud water sample. These differences, calculated to occur early in the parcel's lifetime, should have important consequences for chemical reactions such as aqueous phase sulfate production.

Twohy, C. H.↗

An Evaluation of the Liquid Cloud Droplet Effective Radius Derived from MODIS, Airborne Remote Sensing, and in Situ Measurements from CAMP2Ex

The cloud drop effective radius (Re) of the drop size distribution derived from passive satellite sensors is a key variable used in climate research. Validation of these satellite products has often taken place under stratiform cloud conditions that favor the assumption of cloud horizontal homogeneity used by the retrieval techniques. However, many studies have noted concerns with respect to significant biases in retrieved Re arising from cloud heterogeneity, for example, in cumulus cloud fields. Here, we examine data collected during the 2019 “Cloud, Aerosol and Monsoon Processes Philippines Experiment” (CAMP2Ex), which, in part, targeted the objective of providing the first detailed evaluation of Re retrieved across multiple platforms and techniques in a cumulus and congestus cloud region. Our evaluation consists of cross-comparisons of Re between the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard the Terra satellite, the Research Scanning Polarimeter (RSP) onboard the NASA P-3 aircraft, and in situ measurements from both the NASA P-3 and Learjet aircraft that are all taken in close spatiotemporal proximity to the same cloud fields. A particular advantage of our approach lies in the capability of the RSP to retrieve Re using a bi-spectral MODIS approach and a polarimetric approach, which allows for the evaluation of bi-spectral and polarimetric Re retrievals from an airborne perspective using the same samples. Averaged over all P-3 flight segments examined here for warm clouds, the RSP polarimetric method, the in situ method, and the bias-adjusted MODIS method of Fu et al. (2019) show a comparable median (mean ± standard deviation) for the Re samples of 9.6 (10.2 ± 4.0) µm, 11.0 (13.6 ± 11.3) µm, and 10.4 (10.8 ± 3.8) µm, respectively. These values are far lower than the values of 15.1 (16.2 ± 5.5) µm and 17.2 (17.7 ± 5.7) µm from the bi-spectral retrievals of RSP and MODIS, respectively. Similar results are observed when Re is segregated by cloud-top height and in detailed case studies. The clouds sampled during CAMP2Ex consist of mostly small (mean transect length ∼ 1.4 km) and low clouds (mean cloud-top height ∼ 1 km), which had more numerous small clouds than the trade wind cumuli sampled in past field campaigns such as Rain in Shallow Cumulus over the Ocean (RICO) and the Indian Ocean Experiment (INDOEX). The overestimates of Re from the RSP bi-spectral technique compared with the polarimetric technique increased as cloud size and cloud optical depth decreased. Drizzle, cloud-top bumpiness, and solar zenith angle, however, are not closely correlated with the overestimate of bi-spectral Re. For shallow clouds that dominated the liquid cloud cover for the CAMP2Ex region and period, we show that 3-D radiative transfer and cloud heterogeneity, particularly for the optically thin and small clouds, appear to be the leading cause of the large positive biases in bi-spectral retrievals. Because this bias varies with the underlying structure of the cloud field, caution continues to be warranted in studies that use bi-spectral Re retrievals in cumulus cloud fields.

Cloud microphysics↗

High Free-Tropospheric Aitken-Mode Aerosol Concentrations Buffer Cloud Droplet Concentrations in Large-Eddy Simulations of Precipitating Stratocumulus

A new Aitken mode aerosol microphysics scheme is developed for a large eddy simulation model in order to better investigate cloud-aerosol interactions in the marine boundary layer and to study the Aitken buffering hypothesis of McCoy et al. (2021), https://doi.org/10.1029/2020jd033529. This scheme extends the single-mode two-moment prognostic aerosol scheme of Berner et al. (2013), https://doi.org/10.5194/acp-13-12549-2013. Seven prognostic variables represent accumulation and Aitken log-normal aerosol modes in air and droplets as well as 3 gas species. Scavenging of interstitial and other unactivated aerosol by cloud and rain drops are treated using the scheme described in Berner et al. (2013), https://doi.org/10.5194/acp-13-12549-2013. The scheme includes coagulation of unactivated aerosol and a simple chemistry model with gas phase H 2 SO 4 , SO 2 , and DMS as prognostic variables to capture basic influences of sulfur chemistry on the model aerosols. Nucleation of H 2 SO 4 aerosol particles from gas-phase H 2 SO 4 is neglected. A deep, precipitating stratocumulus case (VAMOS Ocean Cloud Atmosphere Land Study RF06) is used to test the new scheme. The presence of the Aitken mode aerosol increases the cloud droplet concentration through activation of the larger Aitken particles and delays the creation of an ultraclean, strongly precipitating cumulus state. Scavenging of unactivated accumulation and Aitken particles by cloud and precipitation droplets accelerates the collapse. Increasing either the above-inversion Aitken concentration or the surface Aitken flux increases the Aitken population in the boundary layer and prevents the transition to an ultraclean state.

54 ENVIRONMENTAL SCIENCES↗

Impingement of Cloud Droplets on 36.5-Percent-Thick Joukowski Airfoil at Zero Angle of Attack and Discussion of Use as Cloud Measuring Instrument in Dye-Tracer Technique

The trajectories of droplets i n the air flowing past a 36.5-percent-thick Joukowski airfoil at zero angle of attack were determined. The amount of water i n droplet form impinging on the airfoil, the area of droplet impingement, and the rate of droplet impingement per unit area on the airfoil surface were calculated from the trajectories and cover a large range of flight and atmospheric conditions. With the detailed impingement information available, the 36.5-percent-thick Joukowski airfoil can serve the dual purpose of use as the principal element in instruments for making measurements in clouds and of a basic shape for estimating impingement on a thick streamlined body. Methods and examples are presented for illustrating some limitations when the airfoil is used as the principal element in the dye-tracer technique.

Brun, R. J.↗

Theoretical performance of a vortex generator type of cloud droplet sampler

One of the goals of the NASA global tropospheric research program is understanding the chemical processes which influence the chemistry of the natural troposphere. An important element of this program is the study of the role of heterogenous chemistry in global tropospheric chemical cycles. Any study of the part which clouds play in the chemistry of tropospheric trace constituents requires a determination of cloud water chemical composition. There exists, therefore, a need for highly efficient collector devices which can obtain unbiased samples of cloud water in sufficient quantities aboard an aircraft platform. A promising concept which could meet the dual requirements of accurate sampling and efficient collection of cloud water droplets in the vortex generator. This concept involves an inertial separator which uses the centrifugal force of a rotating airstream. The separator is built into a commercial device which has been used for many years as a dust separator for air breathing engines. Attention is given to the optimization of the sampler design.

Miller, I. M.↗

Surface Crystallization of Cloud Droplets: Implications for Climate Change and Ozone Depletion

The process of supercooled liquid water crystallization into ice is still not well understood. Current experimental data on homogeneous freezing rates of ice nucleation in supercooled water droplets show considerable scatter. For example, at -33 C, the reported freezing nucleation rates vary by as much as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Until now, experimental data on the freezing of supercooled water has been analyzed under the assumption that nucleation of ice took place in the interior volume of a water droplet. Here, the same data is reanalyzed assuming that the nucleation occurred "pseudoheterogeneously" at the air (or oil)-liquid water interface of the droplet. Our analysis suggest that the scatter in the nucleation data can be explained by two main factors. First, the current assumption that nucleation occurs solely inside the volume of a water droplet is incorrect. Second, because the nucleation process most likely occurs on the surface, the rates of nuclei formation could differ vastly when oil or air interfaces are involved. Our results suggest that ice freezing in clouds may initiate on droplet surfaces and such a process can allow for low amounts of liquid water (approx. 0.002 g per cubic meters) to remain supercooled down to -40 C as observed in the atmosphere.

Tabazadeh, A.↗

Effects of Cloud Horizontal Inhomogeneity and Drizzle on Remote Sensing of Cloud Droplet Effective Radius: Case Studies Based on Large-eddy Simulations

This study investigates effects of drizzle and cloud horizontal inhomogeneity on cloud effective radius (re) retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS). In order to identify the relative importance of various factors, we developed a MODIS cloud property retrieval simulator based on the combination of large-eddy simulations (LES) and radiative transfer computations. The case studies based on synthetic LES cloud fields indicate that at high spatial resolution (100 m) 3-D radiative transfer effects, such as illumination and shadowing, can induce significant differences between retrievals ofre based on reflectance at 2.1 m (re,2.1) and 3.7 m (re,3.7). It is also found that 3-D effects tend to have stronger impact onre,2.1 than re,3.7, leading to positive difference between the two (re,3.72.1) from illumination and negative re,3.72.1from shadowing. The cancellation of opposing 3-D effects leads to overall reasonable agreement betweenre,2.1 and re,3.7 at high spatial resolution as far as domain averages are concerned. At resolutions similar to MODIS, however, re,2.1 is systematically larger than re,3.7when averaged over the LES domain, with the difference exhibiting a threshold-like dependence on bothre,2.1and an index of the sub-pixel variability in reflectance (H), consistent with MODIS observations. In the LES cases studied, drizzle does not strongly impact reretrievals at either wavelength. It is also found that opposing 3-D radiative transfer effects partly cancel each other when cloud reflectance is aggregated from high spatial resolution to MODIS resolution, resulting in a weaker net impact of 3-D radiative effects onre retrievals. The large difference at MODIS resolution between re,3.7 and re,2.1 for highly inhomogeneous pixels with H 0.4 can be largely attributed to what we refer to as the plane-parallelrebias, which is attributable to the impact of sub-pixel level horizontal variability of cloud optical thickness onre retrievals and is greater for re,2.1 than re,3.7. These results suggest that there are substantial uncertainties attributable to 3-D radiative effects and plane-parallelre bias in the MODIS re,2.1retrievals for pixels with strong sub-pixel scale variability, and theH index can be used to identify these uncertainties.

Zhang, Zhibo↗

Parameterization of Cloud Droplet Formation in Global Climate Models

An aerosol activation parameterization has been developed based on a generalized representation of aerosol size and composition within the framework of an ascending adiabatic parcel; this allows for parameterizing the activation of chemically complex aerosol with an arbitrary size distribution and mixing state. The new parameterization introduces the concept of"population splitting", in which the cloud condensation nuclei (CCN) that form droplets are treated as two separate populations; those that have a size close to their critical diameter and those that do not.Explicit consideration of kinetic limitations of droplet growth is introduced. Our treatment of the activation process unravels much of its complexity. As a result of this, a substantial number of conditions of droplet formation can be treated completely free of empirical information or correlations; there are, however, some conditions of droplet activation for which an empirically derived correlation is utilized. Predictions of the parameterization are compared against extensive cloud parcel model simu;lations for a variety of aerosol activation conditions that cover a wide range of chemical variability and CCN concentrations. The parameterization tracks the parcel model simulations closely and robustly. The parameterization presented here is intended to allow for a comprehensive assessment of the aerosol indirect effect in general circulation models.

Nenes, A.↗

Development of a phase Doppler based probe for icing cloud droplet characterization

The development and evaluation of a compact optical fiber probe (OFP) for airborne and wind tunnel icing cloud characterizations is described. This probe was based upon the proven phase Doppler technique for measuring the size and velocity of spherical drops. Direct comparisons of the size distributions from the standard PDPA with the OFP were used to confirm the reliability of the probe. After some improvements in the fiber coupling efficiency, the number density and liquid water content data agreed to within 15 percent.

Rudoff, R. C.↗

Cloud Water Chemistry and Aerosol Processing: Assessing the Hydroxyl Radical Burst in Newly Formed Cloud Droplets (Field Campaign Report)

Aerosol particles are tiny liquid or solid particles in the atmosphere, ranging in size from a few nanometers to several micrometers in diameter. Aerosol-cloud interactions are the most uncertain aspect of the climate system, and models routinely underpredict aerosol particle formation. Clouds are well known to alter aerosol size, chemical composition, and radiative properties, but the processes are poorly characterized. Organics and sulfates are the most abundant materials in particles, and for each of these there are significant gaps in the understanding of the role of clouds in their formation and/or aging. Many of the cloud processes are driven by aqueous chemistry that depends on hydroxyl (OH) radicals, the subject of this project.

54 ENVIRONMENTAL SCIENCES↗

Drop clustering and drop size correlations from holographic imagery suggest cloud droplet spectral broadening via entrainment-mixing

The question of how droplets rapidly grow large enough to initiate collision-coalescence has persisted for decades. Many theories explaining the production of sufficiently large drops (i.e., those in the “bottleneck” size range; ∼ 25–50 µm diameters) involve drop clustering on millimeter scales. A novel method is introduced to evaluate drop clustering trends particle-by-particle (i.e., the number/proximity of neighboring drops for given droplets; defined as drop clustering fields) which are diagnosed relative to drops within their shared drop environments – in contrast to previous studies which diagnose drop clustering of defined sample volumes, or in terms of absolute length scales. Specifically, this study evaluates the statistical likelihood that drops of a given size are associated with either a significant number of neighboring drops, or are significantly isolated from neighboring drops. Observations are acquired from the HOLODEC during the Cloud System Evolution in the Trades campaign, which sampled subtropical marine clouds. The HOLODEC measures drop size distributions and the 3D spatial coordinates of droplets. Results show drops within the bottleneck size range (diameters of ∼ 25–50 µm) are most likely to be significantly isolated from neighboring drops. This “isolated large drop trend” is primarily observed at subsaturated conditions, suggesting entrainment is the contributing factor. Holograms associated with this trend are more likely to have broader drop size distributions, larger maximum drop sizes and overly regions where precipitation reaches the lowest altitudes from the sampled cloud, suggesting entrainment-mixing drop size distribution broadening is a relevant precipitation-initiation mechanism.

D'Alessandro, John J. [Univ. of Washington, Seattl↗

Removal of trace gases can both increase and decrease cloud droplet formation

Aerosols consist of liquid or solid particles dispersed in a gas. Aerosol measurements generally rely on drying the particles before quantifying their physicochemical properties. This drying can potentially remove semivolatile compounds from the particles. Here, we show size-resolved cloud condensation nuclei (CCN) measurements quantifying the hygroscopicity parameter in the presence and absence of a denuder. The denuder efficiently removed alkanes and weakly functionalized acids, aldehydes, and alcohols with fewer than 10 carbon atoms from the gas phase. Denuding organic compounds perturbed the CCN-derived hygroscopicity parameter by up to 50%. Denuding either rendered the particles more or less CCN active, and the direction of the effect depended on sample relative humidity and trace gas concentration. The effect was weakest in early spring and strongest in late spring and summer. The measurements demonstrate an unexpectedly strong coupling between the particle and gas phase, influencing CCN activity through either volatilization or surface adsorption, or both.

54 ENVIRONMENTAL SCIENCES↗

Optics of Water Cloud Droplets Mixed with Black-Carbon Aerosols

We use the recently extended superposition T-matrix method to calculate scattering and absorption properties of micrometer-sized water droplets contaminated by black carbon. Our numerically exact results reveal that, depending on the mode of soot-water mixing, the soot specific absorption can vary by a factor exceeding 6.5. The specific absorption is maximized when the soot material is quasi-uniformly distributed throughout the droplet interior in the form of numerous small monomers. The range of mixing scenarios captured by our computations implies a wide range of remote sensing and radiation budget implications of the presence of black carbon in liquid-water clouds. We show that the popular Maxwell-Garnett effective-medium approximation can be used to calculate the optical cross sections, single-scattering albedo, and asymmetry parameter for the quasi-uniform mixing scenario, but is likely to fail in application to other mixing scenarios and in computations of the elements of the scattering matrix.

soot↗