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Understanding ice development in cumulus congestus (CuCg) clouds, which are ubiquitous globally, is critical for improving our knowledge of cloud physics, precipitation and climate prediction models. Results presented here are representative of data collected in 1008 penetrations of moderate to strong updrafts in CuCg clouds by five research aircraft in six geographic locations. The results show that CuCg with warm (∼23°C) cloud-base temperatures, such as in tropical marine environments, experience a strong collision–coalescence process. Development of coalescence is also correlated with drop effective radius >∼12 to 14 μm in diameter. Increasing the cloud-base drop concentration with diameters from 15 to 35 μm and decreasing the drop concentration < 15 μm appears to enhance coalescence. While the boundary layer aerosol population is not a determinate factor in development of coalescence in most tropical marine environments, its impact on coalescence is not yet fully determined. Some supercooled large drops generated via coalescence fracture when freezing, producing a secondary ice process (SIP) with production of copious small ice particles that naturally seed the cloud. The SIP produces an avalanche effect, freezing the majority of supercooled liquid water before fresh updrafts reach the −16°C level. Conversely, CuCg with cloud-base temperatures ≤ ∼8°C develop significant concentrations of ice particles at colder temperatures, so that small supercooled water drops are lofted to higher elevations before freezing. Recirculation of ice in downdrafts at the edges of updrafts appears to be the primary mechanism for development of precipitation in CuCg with colder cloud-base temperatures. Significance Statement Cumulus congestus clouds occur globally and account for a significant amount of precipitation in the tropics. The physics underlying the warm rain process and development of ice in cumulus congestus clouds are fundamental to a better understanding of precipitation formation. The collected data show that the strength of collision–coalescence is strongly influenced by cloud-base temperature, and that millimeter-diameter supercooled cloud drops will form in convective clouds with base temperatures warmer than 20°C. When supercooled large drops form, there is a secondary ice process that rapidly freezes the large majority of supercooled cloud water before updrafts reach the −16°C level. Incorporating results from the observations will improve cloud-resolving and climate prediction models.

The Seeded and Natural Orographic Wintertime Clouds: The Idaho Experiment (SNOWIE) project aims to study the impacts of cloud seeding on winter orographic clouds. The field campaign took place in Idaho between 7 January and 17 March 2017 and employed a comprehensive suite of instrumentation, including ground-based radars and airborne sensors, to collect in situ and remotely sensed data in and around clouds containing supercooled liquid water before and after seeding with silver iodide aerosol particles. The seeding material was released primarily by an aircraft. It was hypothesized that the dispersal of the seeding material from aircraft would produce zigzag lines of silver iodide as it dispersed downwind. In several cases, unambiguous zigzag lines of reflectivity were detected by radar, and in situ measurements within these lines have been examined to determine the microphysical response of the cloud to seeding. The measurements from SNOWIE aim to address long-standing questions about the efficacy of cloud seeding, starting with documenting the physical chain of events following seeding. The data will also be used to evaluate and improve computer modeling parameterizations, including a new cloud-seeding parameterization designed to further evaluate and quantify the impacts of cloud seeding.

Aerosol and cloud microphysical measurements were collected by a research aircraft during August 2019 over the United Arab Emirates (UAE). The majority of scientific flights targeted summertime convection along the eastern Al Hajar Mountains bordering Oman, while one flight sampled non-orographic clouds over the western UAE near the Saudi Arabian border. In this work, we study the evolution of growing cloud turrets from cloud base (9 ∘C) up to the capping inversion level (−12 ∘C) using coincident cloud particle imagery and particle size distributions from cloud cores under different forcing. Results demonstrate the active role of background dust and pollution as cloud condensation nuclei (CCN) with the onset of their deliquescence in the subcloud region. Subcloud aerosol sizes are shown to extend from submicron to 100 µm sizes, with higher concentrations of ultra-giant CCN (d>10 µm) from local sources closer to the Saudi border, compared with the eastern orographic region where smaller CCN are observed. Despite the presence of ultra-giant CCN from dust and pollution in both regions, an active collision–coalescence (C–C) process is not observed within the limited depths of warm cloud ( m). The state-of-the-art observations presented in this paper can be used to initialize modeling case studies to examine the influence of aerosols on cloud and precipitation processes in the region and to better understand the impacts of hygroscopic cloud seeding on these clouds.

In situ data collected by three research aircraft in four geographical locations are analyzed to determine the relationship between cloud-base temperature, drop size distribution, and the development of supercooled water drops and ice in strong updraft cores of convective clouds. Data were collected in towering cumulus and feeder cells in the Caribbean, over the Gulf of Mexico, over land near the Gulf Coast, over land in the southeastern United States, and the high plains in Colorado and Wyoming. Convective clouds in the Caribbean, over the Gulf of Mexico and its coast, and over the southeastern United States all develop millimeter-diameter supercooled drops in updraft cores. Clouds over the high plains do not generate supercooled large drops, and rarely are drops >70 μm observed in updraft cores. Commensurate with the production of supercooled large drops, ice is generated and rapidly glaciates updraft cores through a hypothesized secondary ice process that is based on laboratory observations of large drops freezing and emitting tiny ice particles. Clouds over the high plains do not experience the secondary ice process and significant concentrations of supercooled liquid in the form of small drops are carried much higher (up to −35.5°C) in the updraft cores. An empirical relationship that estimates the maximum level to which supercooled liquid water will be transported, based on cloud-base drop size distribution and temperature, is developed. Implications have applications for modeling the transport of water vapor and particles into the upper troposphere and hygroscopic seeding of cumulus clouds.

This paper provides a summary of the assessment report of the World Meteorological Organization (WMO) Expert Team on Weather Modification that discusses recent progress on precipitation enhancement research. The progress has been underpinned by advances in our understanding of cloud processes and interactions between clouds and their environment, which, in turn, have been enabled by substantial developments in technical capabilities to both observe and simulate clouds from the microphysical to the mesoscale. We focus on the two cloud types most commonly seeded in the past: winter orographic cloud systems and convective cloud systems. A key issue for cloud seeding is the extension from cloud-scale research to water catchment–scale impacts on precipitation on the ground. Consequently, the requirements for the design, implementation, and evaluation of a catchment-scale precipitation enhancement campaign are discussed. The paper concludes by indicating the most important gaps in our knowledge. Some recommendations regarding the most urgent research topics are given to stimulate further research.

Cloud characteristics over the rain-shadow region of the north central peninsular India has been studied using C-band radar data for the period 21 September–30 October 2011. The period covers withdrawal and post-withdrawal periods of monsoon 2011. Though the study has been carried out for one season, it has been shown that it is representative of climatic feature over the region. The cloud characteristics have been discussed in the context of large scale dynamical and thermodynamical conditions over the region using NCEP wind data and radiosonde data, respectively. The large scale dynamic and thermodynamical conditions were found favorable for occurrence of widespread and deep convection. The cloud top heights show tri-modal distribution with peaks at 2–3, 4–6 and 8–12 km which are associated with cumulus, congestus and cumulonimbus clouds, respectively. The tops of these three types of the clouds are found to be associated with the stable layers in the atmosphere. The frequency of congestus clouds was the highest. The cloud characteristics over the region differ from other tropical land and oceanic regions in respect of maximum height, mean duration and cumulative frequency distribution. Distribution of cloud top height and duration show deviation from lognormality in the lower ends. It indicates that the cloud growth mechanism is different than that observed over other tropical land and oceanic regions and also due to the large wind shear prevailed over the region. During the period, a large number of suitable clouds were found available for hygroscopic and glaciogenic cloud seeding.

The Habshan industrial site in the United Arab Emirates produces a regional-scale pollution plume associated with oil and gas processing, discharging high loadings of sulfates and chlorides into the atmosphere, which interact with the ambient aerosol population. Aerosol particles and trace gas chemistry at this site were studied on two flights in the summer of 2002. Measurements were collected along vertical plume profiles to show changes associated with atmospheric processing of particle and gas components. Close to the outlet stack, particle concentrations were over 10,000 cm−3, dropping to

Flight data measured in warm convective clouds near Istanbul in June 2008 were used to investigate the relative dispersion of cloud droplet size distribution. The relative dispersion (&varepsilon;), defined as the ratio between the standard deviation (σ) of the cloud droplet size distribution and cloud droplet average radius (⟨r⟩), is a key factor in regional and global models. The relationship between ε and the clouds' microphysical and thermodynamic characteristics is examined. The results show that ε is constrained with average values in the range of ~0.25–0.35. ε is shown not to be correlated with cloud droplet concentration or liquid water content (LWC). However, ε variance is shown to be sensitive to droplet concentration and LWC, suggesting smaller variability of &varepsilon; in the clouds' most adiabatic regions. A criterion for use of in situ airborne measurement data for calculations of statistical moments (used in bulk microphysical schemes), based on the evaluation of &varepsilon;, is suggested.

Aerosol particles from desert dust interact with clouds and influence climate on regional and global scales. The Riyadh (Saudi Arabia) aerosol campaign was initiated to study the effects of dust particles on cloud droplet nucleation and cloud properties. Here we report the results of individual-particle studies of samples that were collected from an aircraft in April 2007. We used analytical transmission electron microscopy, including energy-dispersive X-ray spectrometry, electron diffraction, and imaging techniques for the morphological, chemical, and structural characterization of the particles. Dust storms and regional background conditions were encountered during four days of sampling. Under dusty conditions, the coarse (supermicrometer) fraction resembles freshly crushed rock. The particles are almost exclusively mineral dust grains and include common rock-forming minerals, among which clay minerals, particularly smectites, are most abundant. Unaltered calcite grains also occur, indicating no significant atmospheric processing. The particles have no visible coatings but some contain traces of sulfur. The fine (submicrometer) fraction is dominated by particles of anthropogenic origin, primarily ammonium sulfate (with variable organic coating and some with soot inclusions) and combustion-derived particles (mostly soot). In addition, submicrometer, iron-bearing clay particles also occur, many of which are internally mixed with ammonium sulfate, soot, or both. We studied the relationships between the properties of the aerosol and the droplet microphysics of cumulus clouds that formed above the aerosol layer. Under dusty conditions, when a large concentration of coarse-fraction mineral particles was in the aerosol, cloud drop concentrations were lower and droplet diameters larger than under regional background conditions, when the aerosol was dominated by submicrometer sulfate particles.

As a response to extreme water shortages in southeast Queensland, Australia, brought about by reduced rainfall and increasing population, the Queensland government decided to explore the potential for cloud seeding to enhance rainfall. The Queensland Cloud Seeding Research Program (QCSRP) was conducted in the southeast Queensland region near Brisbane during the 2008/09 wet seasons. In addition to conducting an initial exploratory, randomized (statistical) cloud seeding study, multiparameter radar measurements and in situ aircraft microphysical data were collected. This comprehensive set of observational platforms was designed to improve the physical understanding of the effects of both ambient aerosols and seeding material on precipitation formation in southeast Queensland clouds. This focus on gaining physical understanding, along with the unique combination of modern observational platforms utilized in the program, set it apart from previous cloud seeding research programs. The overarching goals of the ...

Research and operational approaches to weather modification expressed in the National Research Council's 2003 report on “Critical Issues in Weather Modification Research” and in the Weather Modification Association's response to that report form the basis for this discussion. There is agreement that advances in the past few decades over a broad front of understanding physical processes and in technology have not been comprehensively applied to weather modification. Such advances need to be capitalized upon in the form of a concerted and sustained national effort to carry out basic and applied research in weather modification. The need for credible scientific evidence and the pressure for action should be resolved. Differences in the perception of current knowledge, the utility of numerical models, and the specific needs of research and operations in weather modification must be addressed. The increasing demand for water and the cost to society inflicted by severe weather require that the intellectual, tec...

Trace gas and aerosol data were collected through a series of flights over the arid Kalahari Makgadikgadi Pan system. These data show statistically significant spatial and temporal variations in ozone concentrations, while SO2 concentrations were found to be relatively constant. Transport and photochemical production processes are two possible mechanisms for the observed temporal variation in ozone concentration. The presence of certain types of vegetation that emit ozone-precursor gases may account for some of this spatial variation. Aerosols may also be formed as a result of the gases emitted. These species of vegetation alter atmospheric chemistry characteristics and influence the climate. In arid regions, the presence of trace gases and aerosols has an important effect on radiation budget and cloud formation processes, which are significant controlling factors of climate. This paper is a first attempt to synthesize the relationship between surface ecology and atmospheric chemistry of arid environments to better understand the regional climate.

Measurements were made of the emissions of particles and gases from two diesel-powered ships in the southern Atlantic Ocean off the coast of Namibia. The measurements are used to derive emission factors from ships of three species not reported previously, namely, black carbon, accumulation-mode particles, and cloud condensation nuclei (CCN), as well as for carbon dioxide, carbon monoxide (CO), methane (CH4), non-methane hydrocarbons, sulfur dioxide (SO2), nitrogen oxides (NOx), and condensation nuclei. The effects of fuel grade and engine power on ship emissions are discussed. The emission factors are combined with fuel usage data to obtain estimates of global annual emissions of various particles and gases from ocean-going ships. Global emissions of black carbon, accumulation- mode particles, and CCN from ocean-going ships are estimated to be 19-26 Gg yr(sup -1), (4.4-6.1) x 10(exp 26) particles yr(sup -1), and (1.0-1.5) x l0(exp 26) particles yr(sup -1), respectively. Black carbon emissions from ocean-going ships are approximately 0.2% of total anthropogenic emissions. Emissions of NOx and SO2 from ocean-going ships are approximately 10-14% and approximately 3-4%, respectively, of the total emissions of these species from the burning of fossil fuels, and approximately 40% and approximately 70%, respectively, of the total emissions of these species from the burning of biomass. Global annual emissions of CO and CH4 from ocean-going ships are approximately 2% and approximately 2-5%, respectively, of natural oceanic emissions of these species.

The May 1998 transport of smoke from fires in Mexico and Central America into the United States is examined. We combine data from ground-based Interagency Monitoring of Protected Visual Environments aerosol chemical sampling sites with in situ airborne and Sun photometer measurements to develop a consistent picture of the transported smoke-impacted aerosol optical and chemical properties. The aerosol observed in Mexico and the southern United States is found to have a higher sulfate mass fraction, higher single-scattering albedo, and larger accumulation mode radius than biomass burning aerosols observed by similar instrumentation in South America and Africa. We postulate that the smoke-impacted aerosol in the 1998 event was more hygroscopic than that observed in the other locations, because of the higher mass fractions of sulfate, and show that a simple model of corresponding changes in aerosol water content yields agreement with the observed variations in refractive index and radii. We further show that the single-scattering albedo cannot be fully explained by hygroscopic growth alone. Modifications to the model invoking variations in aerosol light-absorbing carbon content, which are consistent with differences in observed composition among the various smoke-impacted aerosols, bring the predictions of single-scattering albedo into alignment with our observations. The model demonstrates that the particle size, single-scattering albedo, and real refractive index of smoke-impacted aerosols are not independent but vary in tandem with variations in particle hygroscopicity and with variations in black carbon content. This relationship is an important consideration in the assessment of the effects of biomass burning aerosols, particularly those subject to long-range transport, on radiative forcing and climate.

Water is one of the most basic commodities on earth sustaining human life. In many regions of the world, traditional sources and supplies of ground water, rivers and reservoirs, are either inadequate or under threat from ever-increasing demands on water from changes in land use and growing populations. This has prompted scientists and engineers to explore the possibility of augmenting water supplies by means of cloud seeding. This paper provides an overview of the current scientific status of weather modification activities to enhance pre- cipitation for both glaciogenic and hygroscopic seeding experiments. It is important to emphasize that although funding for scientific studies has decreased substantially during the past decade, operational programs have actually increased. During the last 10 years there has been a thorough scrutiny of past experiments involving experiments using glaciogenic seeding. Although there still exist indications that seeding can increase precipitation, a number of recent studies have questioned many of the positive results, weakening the scientific credibility. As a result, considerable skep- ticism exists as to whether these methods provides a cost-effective means for increasing precipitation for water resources. Recent results from hygroscopic seeding experiments provided for some renewed optimism in the field of precipita- tion enhancement. Although promising results have been obtained to date, some fundamental questions remain that need to be answered in order to provide a sound scientific basis for this technology.

The purpose of this study is to assess the relative importance of collision and coalescence efficiencies as reported in the literature in different drop size regimes for the development of precipitation via the condensation–coalescence process. The stochastic growth of cloud droplet distributions due to collection processes is studied using a detailed microphysical parcel model. The evolution of rainwater content (LR) and the radar reflectivity factor (Z) are plotted in order to trace the progress of transfer of cloud water into rainwater and determine the importance of droplet collection in different size ranges. The results indicate that the van der Waals forces are effective in enhancing droplet collision when the droplets are small and the distributions are narrow. Wake capture is negligible for clouds forming in a continental air mass with low liquid water contents. However, it is effective when coalescence becomes the dominant growth process and rainwater content has reached high values. Wh...

The 1995 Arizona Program was a field experiment aimed at advancing the understanding of winter storm development in a mountainous region of central Arizona. From 15 January through 15 March 1995, a wide variety of instrumentation was operated in and around the Verde Valley southwest of Flagstaff, Arizona. These instruments included two Doppler dual-polarization radars, an instrumented airplane, a lidar, microwave and infrared radiometers, an acoustic sounder, and other surface-based facilities. Twenty-nine scientists from eight institutions took part in the program. Of special interest was the interaction of topographically induced, storm-embedded gravity waves with ambient upslope flow. It is hypothesized that these waves serve to augment the upslope-forced precipitation that falls on the mountain ridges. A major thrust of the program was to compare the observations of these winter storms to those predicted with the Clark-NCAR 3D, nonhydrostatic numerical model.

An explicit microphysical parametrization including ice physics was developed for use in the NCAR/Penn State Mesoscale Model Version 5 (MM5). This scheme includes three options of increasing complexity to represent the hydrometeor species. The scheme is evaluated by comparing model simulations with two well observed winter storms that occurred during the Winter Icing and Storms Project. The evaluation focused on the prediction of supercooled liquid water (SLW), which is of particular importance to aircraft icing. The intercomparisons showed that: 1 The double-moment microphysical scheme, in which both ice mixing ratios and number concentrations were predicted, performed best, with close agreement to the observed fields. 2 The single-moment schemes, in which the mixing ratio of ice species are predicted and number concentration specified, performed reasonably well if a diagnostic equation for No, s, the Y-intercept of the assumed exponential snow distribution, is allowed to vary with snow mixing ratio. 3 Accurate microphysical simulations of SLW in shallow upslope clouds and cyclonic storms required accurate simulations of the kinematic and thermodynamic structure and evolution of the storms. Though the two storms were dynamically different, the SLW formed through a balance of the condensational growth of cloud water and the depletion of cloud water by deposition and riming of snow and/or graupel for both storms. The results of this study suggest that accurate prediction of SLW over limited areas of the country may be possible using the current microphysical parametrization and high-resolution grids (δχ

Recent research to improve forecasts of in-flight icing conditions has involved the development of algorithms to apply to the output of numerical weather prediction models. The abilities of several of these algorithms to predict icing conditions, as verified by pilot reports (PIREPs), are compared for two numerical weather prediction models (Eta and the Mesoscale Analysis and Prediction System) for the Winter Icing and Storms Program 1994 (WISP94) time period (25 January–25 March 1994). Algorithms included in the comparison were developed by the National Aviation Weather Advisory Unit [NAWAU, now the Aviation Weather Center (AWC)], the National Center for Atmospheric Research’s Research Applications Program (RAP), and the U.S. Air Force. Operational icing forecasts (AIRMETs) issued by NAWAU for the same time period are evaluated to provide a standard of comparison. The capabilities of the Eta Model’s explicit cloud liquid water estimates for identifying icing regions are also evaluated and compar...

The purpose of the Federal Aviation Administration’s Icing Forecasting Improvement Program is to conduct research on icing conditions both in flight and on the ground. This paper describes a portion of the in-flight aircraft icing prediction effort through a comprehensive icing prediction and evaluation project conducted by the Research Applications Program at the National Center for Atmospheric Research. During this project, in- flight icing potential was forecast using algorithms developed by RAP, the National Weather Service’s National Aviation Weather Advisory Unit, and the Air Force Global Weather Center in conjunction with numerical model data from the Eta, MAPS, and MM5 models. Furthermore, explicit predictions of cloud liquid water were available from the Eta and MM5 models and were also used to forecast icing potential. To compare subjectively the different algorithms, predicted icing regions and observed pilot reports were viewed simultaneously on an interactive, real-time display. To m...

Some possible effects of hygroscopic seeding with flares are explored by calculating how such seeding would modify the initial size distribution of cloud droplets and the subsequent evolution of that size distribution by coalescence. To be representative of recent experiments in South Africa, the calculations emphasize the effects of hygroscopic particles that can be produced by flares, instead of the larger particles used in most past hygroscopic-seeding experiments. Parcel calculations representing simultaneous condensation and coalescence suggest that the formation of rain through the warm-rain process can be accelerated significantly by the addition of such hygroscopic particles. Some observations of the effects of hygroscopic material near cloud base support at least the early stages of the calculations. The results suggest that the positive effects being obtained in the South African experiment may occur through such acceleration of the warm-rain process. Possible cloud-seeding applications and climate implications are discussed.

Polarimetric radar can be used to identify various types of hydrometeors. Ice crystals of the varied growth habits depolarize and backscatter millimeter-wavelength radiation according to crystal aspect ratio, bulk density, and orientation, and the polarization state of the incident radiation. In this paper model calculations of the depolarization caused by various crystal types are extended from previous work, and Ka-band (8.66 mm) radar measurements of linear and elliptical depolarization ratios (LDR and EDR) from various ice hydrometeors are presented. The measurements for regular crystals are related to the models. Drizzle drops, which are quasi-spherical, serve as a reference. Signature discrimination in cloud systems with more than one type of hydrometeor is addressed. The model calculations illustrate the interplay of the parameters that control depolarization. They predict that in the depolarization signatures, crystals of the various basic planar and columnar habits should generally be mo...

A three-dimensional, time-dependent, nested-grid model is used to calculate the targeting of tracer or Seeding material over complex terrain in northern Arizona. Good agreement with measurements of SF6 tracer is reported in three case studies. Released in upwind valleys, the tracer movement and dispersion are strongly influenced by both valley flow and gravity waves excited by the mountains, as well as by changes in the synoptic flow, which can change substantially even during a single storm. The interaction between the airflow and the topography seem to be the dominant factor determining the dispersion and transport of tracer material.

A case study showing comparisons between observations and numerical simulations of the passage of a winter storm over complex terrain is presented. The interactions between the mesoscale and cloud environments and the microphysical and dynamical processes are addressed using both observations and numerical simulations. A three-dimensional, time-dependent nested grid model was used to conduct numerical simulations of the three-dimensional airflow and cloud evolution over the Mogollon Rim and adjacent terrain in Arizona. The modeling results indicated that the flow patterns and cloud liquid water (CLW) were closely linked to the topography. To a large extent, gravity waves excited by the flow over the mountains determine the distribution of clouds and precipitation. The waves extend through deep layers of the atmosphere with substantial updrafts and downdrafts, at times exceeding 5 m s−1. The simulated vertical velocities and horizontal wavelengths of about 20 km were in good agreement with the air...

[1] In August through September 2004 the United Arab Emirates Unified Aerosol Experiment (UAE2) was conducted in the southern Arabian Gulf region. We present atmospheric thermodynamic and aerosol data collected on 18 flights by the South African Aerocommander aircraft. In the first few kilometers, we observed high concentrations of both regional dust (from 100 to 300 μg m−3 in background, to over 1.5 mg m−3 in events) and ubiquitous sulfate based pollution from the Gulf's prevalent petroleum industry (10–100 μg m−3). Smoke and pollution from Europe and possibly Africa were found at levels between 1.5 and 5 km. Inland, classic deep over desert boundary layer characteristics were found. Over the Arabian Gulf, dust and pollution were most often either trapped below or sequestered above a strong stable boundary. However, there were cases where a well-distributed aerosol layer crossed the inversion uniformly. Data suggest that the observed vertical profiles can be explained by the rapid formation of stable marine boundary layers as air moves offshore. This can decouple aerosol layers from within the boundary layer to those aloft in regions of vertical wind shear. In the case of pollution, the ability of flaring plumes to penetrate the inversion may also in part determine layering. In coastal regions without vertical wind shear, uniform concentrations with height across the inversion are a result of internal boundary layer development. We conclude that the bulk of the observed variability in particle vertical distribution appear to be controlled by mesoscale and microscale processes, such as the sea/land breeze.

[1] We used conventional and environmental transmission electron microscopes to determine morphology, composition, and water uptake of individual natural inorganic aerosol particles collected from industrial pollution plumes and from clean and polluted marine environments. Five particle types are described in detail. They range from relatively insoluble mineral grains to internally mixed particles containing NaCl with other soluble or relatively insoluble material. We studied the hygroscopic behavior of these particles from 0 to 100% relative humidity (RH). Relatively insoluble materials do not take up water over the experimental RH range. Single crystals of NaCl from both natural and laboratory sources have a well-defined deliquescence point of approximately 76% RH at 291 K. NaCl-bearing aggregate particles appear to deliquesce between 74 and 76% RH (same RH within error) when NaCl is internally mixed with relatively insoluble phases, but the particles deliquesce at lower RH when aggregated with other soluble phases such as NaNO3. For all NaCl-bearing particles studied, hygroscopic growth is pronounced above 76% RH, and water uptake by the particles is dominated by the soluble phase. Furthermore, the soluble phase initiating deliquescence controls the locus of further hygroscopic growth of the aggregate particle. Our results demonstrate that composition and mixing state affect water uptake of natural aerosol particles. Furthermore, internally mixed particles are confirmed to deliquesce at lower RH values than predicted from the individual components.

[1] Episodes of regionally extensive haze were observed over southern African during the dry season intensive of the Southern African Regional Science Initiative (SAFARI 2000). Several case studies of southern African haze layers were examined and characterized in terms of physical structure as they exited off of the eastern coastal region of southern Africa. In situ observations of aerosols and trace gases and their physical and chemical characteristics were collected on board South African Weather Service Aerocommander research aircraft. Haze structure, based on these measurements, is examined as it varies with synoptic type. Despite strong differences in the observed ENSO regime between SAFARI 2000 and that observed during the Southern African Fire-Atmosphere Research Initiative (SAFARI-92) and their respective aerosol accumulation mechanisms (col Rrgions/weak anticyclones versus strong anticyclones), a surprising degree of consistency in the observed vertical structure of the lower troposphere was found in southern Africa. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0368 Atmospheric Composition and Structure: Troposphere—constituent transport and chemistry; KEYWORDS: haze layers, synoptic circulations, ENSO

[1] The sources and transport of cloud condensation nuclei (CCN) over southern Africa have been investigated using in situ measurements collected during the Aerosol Recirculation and Rainfall Experiment (ARREX) wet season projects and during the Southern African Regional Science Initiative (SAFARI-2000) intensive dry season campaign. CCN concentrations over the subcontinent are generally higher in the dry season than in the wet season and exceed 2000 cm−3 in highly polluted air masses. In the late dry season, CCN concentrations are highest in the northern regions of the subcontinent due to the burning of savanna biomass. Emissions from industries and power plants on the South African Highveld are a prolific year-round source of CCN and are sufficient to account for CCN levels south of 20°S throughout the year. Most CCN are contained within the mixing layer, which extends to an altitude of 3000–4000 m over the plateau and is capped by a temperature inversion. Multiple inversions and absolutely stable layers control the stratification of aerosols and CCN. Biomass burning particles are efficient CCN, and the median diameter of the accumulation mode is large (up to 0.19 μm). Recently emitted industrial aerosols are less soluble and have a smaller median diameter (0.11 μm). Twice as many aerosols act as CCN in the dry season (68%) than in the wet season (34%). The fraction is highest in the dry season over the tropical regions (>80%), where smoke aerosol predominates. Elevated aerosol and CCN concentrations are expected to have implications for direct radiative forcing, especially in the dry season, and for indirect forcing in the wet season.

Measurements within continental convective clouds in the Highveld region of South Africa indicate that the first appreciable nucleation of ice occurs between the −9° to −12°C levels as the cloud top rises through these levels. Moreover, these crystals usually take the form of double plates. Frozen drop centers were observed in 30% of the double crystals, with the diameter of the frozen drop between 10 and 20 μm. The growth of these ice crystals is investigated using ice crystal measurements collected in situ as well as a modeling study. New information regarding axial dimensions, bulk densities, and riming characteristics of double-plate crystals is presented. Numerical simulations were performed to compare the growth characteristics of ice crystals nucleated at different temperature levels between −6° and −16°C in updrafts of 1 and 3 m s−1. Crystals nucleated at temperatures ≥−12°C are shown to start riming at smaller sizes than previously thought and these crystals are potentially important as ...

Measurements of aerosol size distribution, chemical composition, and cloud condensation nuclei (CCN) concentration were performed during the Chemical Emission, Loss, Transformation, and Interactions with Canopies (CELTIC) field program at Duke Forest in North Carolina. A kinetic model of the cloud activation of ambient aerosol in the chamber of the CCN instrument was used to perform an aerosol–CCN closure study. This study advances prior investigations by employing a novel fitting algorithm that was used to integrate scanning mobility particle sizer (SMPS) measurements of aerosol number size distribution and aerosol mass spectrometer (AMS) measurements of the mass size distribution for sulfate, nitrate, ammonium, and organics into a single, coherent description of the ambient aerosol in the size range critical to aerosol activation (around 100-nm diameter). Three lognormal aerosol size modes, each with a unique internally mixed composition, were used as input into the kinetic model. For the two smaller size modes, which control CCN number concentration, organic aerosol mass fractions for the defined cases were between 58% and 77%. This study is also unique in that the water vapor accommodation coefficient was estimated based on comparing the initial timing for CCN activation in the instrument chamber with the activation predicted by the kinetic model. The kinetic model overestimated measured CCN concentrations, especially under polluted conditions. Prior studies have attributed a positive model bias to an incomplete understanding of the aerosol composition, especially the role of organics in the activation process. This study shows that including measured organic mass fractions with an assumed organic aerosol speciation profile (pinic acid, fulvic acid, and levoglucosan) and an assumed organic aerosol solubility of 0.02 kg kg−1 still resulted in a significant model positive bias for polluted case study periods. The slope and y intercept for the CCN predicted versus CCN observed regression was found to be 1.9 and −180 cm−3, respectively. The overprediction generally does not exceed uncertainty limits but is indicative that a bias exists in the measurements or application of model. From this study, uncertainties in the particle number and mass size distributions as the cause for the model bias can be ruled out. The authors are also confident that the model is including the effects of growth kinetics on predicted activated number. However, one cannot rule out uncertainties associated with poorly characterized CCN measurement biases, uncertainties in assumed organic solubility, and uncertainties in aerosol mixing state. Sensitivity simulations suggest that assuming either an insoluble organic fraction or external aerosol mixing were both sufficient to reconcile the model bias.