Understanding the Effect of Aerosol Properties on Cloud Droplet Formation During TCAP Field Campaign Report PDF Download

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Category :
Languages : en
Pages : 10

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The formation of clouds is an essential element in understanding the Earth's radiative budget. Liquid water clouds form when the relative humidity exceeds saturation and condensedphase water nucleates on atmospheric particulate matter. The effect of aerosol properties such as size, morphology, and composition on cloud droplet formation has been studied theoretically as well as in the laboratory and field. Almost without exception these studies have been limited to parallel measurements of aerosol properties and cloud formation or collection of material after the cloud has formed, at which point nucleation information has been lost. Studies of this sort are adequate when a large fraction of the aerosol activates, but correlations and resulting model parameterizations are much more uncertain at lower supersaturations and activated fractions.

Author: Beth Friedman
Publisher:
ISBN:
Category : Aerosols
Languages : en
Pages : 151

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Aerosol-cloud interactions represent a significant uncertainty with respect to radiative forcing and future climate change. Both particle composition and size play key, yet poorly understood, roles in determining the cloud nucleating capabilities of aerosols. The following describes ambient and laboratory measurements of cloud condensation nuclei (CCN) and ice nuclei (IN) measurements from a variety of sources, with the goal of understanding how composition and size interact in forming cloud droplets and ice crystals and the potential importance of aerosol composition and atmospheric aging processes on constraining uncertainties associated with the cloud nucleating properties of aerosols. Motivated by the anthropogenic emissions of soot particles as well as the potential properties of aged soot particles, ice formation and droplet activation of soot particles of various size and composition were studied. Generated soot particles were coated with a variety of atmospherically relevant acids of varying solubility properties. The particles were also exposed to ozone in order to simulate atmospheric oxidation and aging. A custom-built ice chamber was utilized to show that both uncoated and coated soot particles comparable to those generated in our studies are unlikely to significantly contribute to the global budget of heterogeneous IN at relevant atmospheric temperatures. This result is emphasized by comparison to an efficient ice nucleus, such as mineral dust. Coatings and oxidation by ozone also did not significantly alter the ice nucleation behavior of soot particles but aided in the uptake of water, suggesting the altered composition of a hydrophobic particle is important to take into account for cloud droplet activation. To assess the importance of particle composition in cloud droplet activation, measurements of CCN concentrations, single particle composition, and number size distributions were conducted at a high-elevation research site. The temporal evolution of detailed single particle chemical composition was compared with changes in CCN activation. A variety of particle types were observed; CCN activation largely followed the behavior of the sulfate-containing particle types; biomass burning particles also contained hygroscopic material that impacted CCN activation. The observed particles were largely aged; few local sources contributed to the particle composition due to the high elevation of the site. The results were also interpreted in terms of the assumed hygroscopicity of free tropospheric aerosol. As a further examination of the impacts of aging processes on aerosol hygroscopicity measurements of CCN concentrations, aerosol composition, and number size distributions were conducted during the winter season from of a variety of air masses, including aged marine, continental, and urban sources. Based on the measured chemistry and size properties of the ambient aerosol, CCN concentrations were predicted in order to assess the amount of composition detail necessary to explain droplet activation. Direct measurements of the composition of the activated droplets were also conducted with a novel technique to separate activated droplets from un-activated aerosol. Results suggest the importance of inorganic species in droplet activation, with non-oxidized organic species having negligible impacts on total aerosol hygroscopicity. Using the same novel separation technique, measurements of the single particle composition of activated droplet residual particles were determined at an urban site in the summertime, with similar air mass trajectories as the previous wintertime site, as well as influence from local urban aerosol sources. As a function of atmospheric supersaturation conditions the composition of activated droplet residual particles was compared to the ambient aerosol composition. The study was utilized to determine the level of composition and size detail required to describe droplet activation at a site with similar aged air mass trajectories to the previous study.

Author:
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Category : Atmospheric ozone
Languages : en
Pages : 128

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Author: Sara Lance
Publisher:
ISBN:
Category : Aerosols
Languages : en
Pages :

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It has been historically assumed that most of the uncertainty associated with the aerosol indirect effect on climate can be attributed to the unpredictability of updrafts. We assess the sensitivity of cloud droplet number density to realistic variations in aerosol chemical properties and to variable updraft velocities using a 1-dimensional cloud parcel model. The results suggest that aerosol chemical variability may be as important to the aerosol indirect effect as the effect of unresolved cloud dynamics, especially in polluted environments. We next used a continuous flow streamwise thermal gradient Cloud Condesnation Nuclei counter (CCNc) to study the water-uptake properties of the ambient aerosol, by exposing an aerosol sample to a controlled water vapor supersaturation and counting the resulting number of droplets. The heat transfer properties and droplet growth within the CCNc were first modeled and experimentally characterized. We describe results from the MIRAGE field campaign at a ground-based site during March, 2006. Size-resolved CCN activation spectra and hygroscopic growth factor distributions of the ambient aerosol in Mexico City were obtained, and an analytical technique was developed to quantify a probability distribution of solute volume fractions for the CCN, as well as the aerosol mixing-state. The CCN were shown to be much less CCN active than ammonium sulfate, with water uptake properties more consistent with low molecular weight organic compounds. We also describe results from the GoMACCS field study, an airborne field campaign in Houston, Texas during August-September, 2006. GoMACCS tested our ability to predict CCN for highly polluted conditions with limited chemical information. Assuming the particles were composed purely of ammonium sulfate, CCN closure was obtained with a 10% overprediction bias on average for CCN concentrations ranging from less than 100 cm-3 to over 10,000 cm-3, but with on average 50% variability. Assuming measured concentrations of organics to be internally mixed and insoluble tended to reduce the overprediction bias for less polluted conditions, but led to underprediction bias in the most polluted conditions. Comparing the two campaigns, it is clear that the chemistry of the particles plays an important role in our ability to predict CCN concentrations.

Author: National Research Council
Publisher: National Academies Press
ISBN: 0309175917
Category : Science
Languages : en
Pages : 179

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This book recommends the initiation of an "integrated" research program to study the role of aerosols in the predicted global climate change. Current understanding suggest that, even now, aerosols, primarily from anthropogenic sources, may be reducing the rate of warming caused by greenhouse gas emissions. In addition to specific research recommendations, this book forcefully argues for two kinds of research program integration: integration of the individual laboratory, field, and theoretical research activities and an integrated management structure that involves all of the concerned federal agencies.

Author: Michael Steven Diamond
Publisher:
ISBN:
Category :
Languages : en
Pages : 209

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Book Description
Uncertainties in how airborne particles (aerosol) influence cloud reflectivity hinder our understanding of anthropogenic climate change. The study of aerosol-cloud interactions (ACI) is complicated by the difficulty of disentangling aerosol effects from other phenomena like meteorological variability. Natural laboratories (large-scale perturbations of known origin) and natural experiments (more abrupt and localized perturbations), in which a phenomenon of interest may be clearly separated from other sources of variability, offer promising means to better understand causality in ACI.Ship tracks--curvilinear cloud features following individual ships--are the quintessential example of natural experiments in ACI. Prior studies have not detected large-scale cloud changes from shipping, despite climate model predictions indicating sizable effects. In Chapter 2, we attribute increased cloud reflectivity within a major shipping corridor in the southeast Atlantic to enhanced cloud droplet numbers by estimating what cloud properties would have been without shipping. Increased cloud brightness from microphysical changes is partially offset by decreases in the total amount of cloud water. Extrapolating our results globally, we calculate an effective radiative forcing due to ACI of approximately -1 W/m2. Smoke from southern Africa blankets the southeast Atlantic Ocean from June-October, producing a natural laboratory with competing aerosol radiative effects. In Chapter 3, we investigate smoke effects on the transition between overcast stratocumulus and scattered cumulus clouds in regional climate and large eddy simulation models and compare the results with observations from recent field campaigns. Interactions between smoke and the large-scale circulation alter above-cloud temperature and moisture in ways that strongly affect cloud evolution. The COVID-19 outbreak and subsequent shutdown in China during February 2020 resulted in a sharp economic contraction. In Chapter 4, we show that nitrogen dioxide pollution declined by an unprecedented amount from its expected unperturbed value, but regional-scale column aerosol loadings and cloud microphysical properties were not detectably affected. The disparate impact is tied to differential economic impacts of the shutdown, in which transportation underwent much more drastic declines than industry and power generation. Anomalously warm and humid meteorological conditions and complex chemical interactions further decreased nitrogen dioxide but enhanced secondary aerosol formation.

Author: Luz Teresa Padro Martinez
Publisher:
ISBN:
Category : Atmospheric aerosols
Languages : en
Pages :

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It is well known that atmospheric aerosols provide the sites for forming cloud droplets, and can affect the Earth's radiation budget through their interactions with clouds. The ability of aerosols to act as cloud condensation nuclei is a strong function of their chemical composition and size. The compositional complexity of aerosol prohibits their explicit treatment in atmospheric models of aerosol-cloud interactions. Nevertheless, the cumulative impact of organics on CCN activity is still required, as carbonaceous material can constitute up to 90% of the total aerosol, 10-70% of which is water soluble. Therefore it is necessary to characterize the water soluble organic carbon fraction by CCN activation, droplet growth kinetics, and surface tension measurements. In this thesis, we investigate the water soluble properties, such as surface tension, solubility, and molecular weight, of laboratory and ambient aerosols and their effect on CCN formation. A mechanism called Curvature Enhanced Solubility is proposed and shown to explain the apparent increased solubility of organics. A new method, called Köhler Theory Analysis, which is completely new, fast, and uses minimal amount of sample was developed to infer the molar volume (or molar mass) of organics. Due to the success of the technique in predicting the molar volume of laboratory samples, it was applied to aerosols collected in Mexico City. Additionally the surface tension, CCN activity, and droplet growth kinetics of these urban polluted aerosols were investigated. Studies performed for the water soluble components showed that the aerosols in Mexico City have surfactants present, can readily become CCN, and have growth similar to ammonium sulfate. Finally, aerosols from three different polluted sources, urban, bovine, and ship emissions, were collected and characterized. The data assembled was used to predict CCN concentrations and access our understanding of the system. From these analyses, it was evident that knowledge of the chemical composition and mixing state of the aerosol is necessary to achieve agreement between observations and predictions. The data obtained in this thesis can be introduced and used as constraints in aerosol-cloud interaction parameterizations developed for global climate models, which could lead to improvements in the indirect effect of aerosols.

Author: Hsiang-He Lee
Publisher:
ISBN: 9781321363142
Category :
Languages : en
Pages :

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The source-oriented Weather Research and Forecasting chemistry model (SOWC) was modified to include warm/cold cloud processes and applied to investigate 1) how source-oriented aerosols influence fog formation and optical properties in the atmosphere, 2) how aerosol mixing state influences cloud and ice formation and atmospheric optical properties during a winter storm, and 3) the direct, semi-direct, and indirect effects of long-range transport dust on severe weather over California and the Eastern Pacific. SOWC tracks 6-dimensional chemical variables (X, Z, Y, Size Bins, Source Types, Species) through an explicit simulation of atmospheric chemistry and physics. In this study, all aerosol source types can activate to form cloud condensation nuclei (CCN) based on the Köhler theory, but the dust is the only source of ice nuclei (IN). Furthermore, a new source-oriented cloud module in the two-moment Purdue Lin microphysics scheme, and a new module with all source-oriented hydrometeors (cloud, ice, rain, snow and graupel) in the Morrison two-moment microphysics scheme were implemented into the SOWC model to study fog events and winter storm cases, respectively. In Chapter 2, the enhanced SOWC model was used to study a fog event that occurred on January 17th, 2011, in the Central Valley of California. The SOWC reasonably portrays the spatial distribution and duration of the fog event consistent with observations. The source-oriented mixture representation of particles reduced cloud droplet number relative to the internal mixture approach that artificially coats hydrophobic particles with hygroscopic components. The fraction of aerosols activating into CCN at a supersaturation of 0.5% in the Central Valley decreased from 86% in the internal mixture model to 68% in the source-oriented model. This increased the surface energy flux by 3-5 W m-2 and surface temperature by as much as 0.15 K. In Chapter 3, the enhanced SOWC model was used to study a winter storm that occurred on March 6th, 2011, in California. Compared to ground based observations, SOWC with the modified Morrison microphysics scheme and modified Goddard radiation schemes predicted reasonable precipitation, but the onset of precipitation is delayed by 5 hours. Immersion freezing was the main mechanism for ice nuclei formation. Secondary coatings on dust particles increased IN from immersion freezing but decreased IN from contact freezing. Increasing CCN and IN in the internal mixing experiment produced more ice crystals and cloud droplets but did not significantly alter total perception under the conditions studied. However, because of the reducing riming efficiency from snow to graupel in the source-oriented mixing experiment, it resulted more snowfall (less rainfall) on the ground, especially over the mountain area. In Chapter 4, the SOWC model was used to understand the direct, semi-direct, and indirect effects of long-range transport dust on severe weather over Eastern Pacific Ocean. The maximum averaged IN nucleation rate increased 36% after adding long-range transport dust. Because clouds in mid-latitude originate precipitately via the ice phase, an increase in IN can enhance ice formation from supercooled water by heterogenetic freezing (mainly contact freezing) and then to alter hydrometer water amount. Adding long-range transport dust increased the mixing ratio and number concentration for almost all hydrometers. However, the changes of adding local dust in local+LR_dust from LR_dust is more complicated due to the importance of hydrometers in the cumulus scheme. The change in the strength of convection after adding long-range transport dust (or local dust) also produces a noticeable distinction in the precipitation pattern, but the total precipitation did not have major difference after adding long-range transport dust (or local dust).

Author: Kerry J. Knox
Publisher: Springer Science & Business Media
ISBN: 3642163483
Category : Science
Languages : en
Pages : 209

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Book Description
Aerosols play a critical role in a broad range of scientific disciplines, such as atmospheric chemistry and physics, combustion science, drug delivery and human health. This thesis explores the fundamentals of a new technique for capturing single or multiple particles using light, and for characterising these particles by Raman or fluorescence spectroscopy. The outcome of this research represents a significant development in optical manipulation techniques, specifically in optical tweezing. These findings can be applied to studies of the mass accommodation of gas-phase water molecules adsorbing onto a water surface. Not only is this a fundamental process of interest to physical chemists, but it is important for understanding the role of aerosol particles in the atmosphere, including their ability to become cloud droplets. This new strategy for investigating aerosol dynamics is fundamental in helping us understand the indirect effect of aerosols on the climate.

Author: Yuan Wang
Publisher: Springer
ISBN: 9783662515945
Category : Science
Languages : en
Pages : 0

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The studies in this dissertation aim at advancing our scientific understandings about physical processes involved in the aerosol-cloud-precipitation interaction and quantitatively assessing the impacts of aerosols on the cloud systems with diverse scales over the globe on the basis of the observational data analysis and various modeling studies. As recognized in the Fifth Assessment Report by the Inter-government Panel on Climate Change, the magnitude of radiative forcing by atmospheric aerosols is highly uncertain, representing the largest uncertainty in projections of future climate by anthropogenic activities. By using a newly implemented cloud microphysical scheme in the cloud-resolving model, the thesis assesses aerosol-cloud interaction for distinct weather systems, ranging from individual cumulus to mesoscale convective systems. This thesis also introduces a novel hierarchical modeling approach that solves a long outstanding mismatch between simulations by regional weather models and global climate models in the climate modeling community. More importantly, the thesis provides key scientific solutions to several challenging questions in climate science, including the global impacts of the Asian pollution. As scientists wrestle with the complexities of climate change in response to varied anthropogenic forcing, perhaps no problem is more challenging than the understanding of the impacts of atmospheric aerosols from air pollution on clouds and the global circulation.