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Search Results: 1 - 10 of 117917 matches for " T. Koop "
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The role of organic aerosols in homogeneous ice formation
B. K rcher,T. Koop
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2005,
Abstract: Recent field observations suggest that the fraction of organic-containing aerosol particles in ice cloud particles is diminished when compared to the background aerosol prior to freezing. In this work, we use model calculations to investigate possible causes for the observed behavior. In particular, homogeneous freezing processes in cooling air parcels containing aqueous inorganic particles and organic particles are studied with a detailed microphysical model. A disparate water uptake and resulting size differences that occur between organic and inorganic particles prior to freezing are identified as the most likely reason for the poor partitioning of organic aerosols into the ice phase. The differences in water uptake can be caused by changes in the relationship between solute mass fraction and water activity of the supercooled liquid phase, by modifications of the accommodation coefficient for water molecules, or by a combination thereof. The behavior of peak ice saturation ratios and total ice crystal number concentrations is examined, and the dependence of the results on cooling rate is investigated. Finally, processes are discussed that could possibly modify the homogeneous freezing behavior of organic particles.
The role of organic aerosols in homogeneous ice formation
B. K?rcher,T. Koop
Atmospheric Chemistry and Physics Discussions , 2004,
Abstract: Recent field observations suggest that the fraction of organics containing aerosol particles in ice cloud particles is diminished when compared to the background aerosol prior to freezing. In this work, we use model calculations to investigate possible causes for the observed behavior. In particular, homogeneous freezing processes in cooling air parcels containing aqueous inorganic particles (represented by sulfuric acid) and organic particles (represented by pure malonic acid and mixed malonic/sulfuric acid) are studied with a detailed microphysical model. A disparate water uptake and resulting size differences that occur between organic and inorganic particles prior to freezing are identified as the most likely reason for the poor partitioning of organic aerosols into the ice phase. The differences in water uptake can be caused by changes in the relationship between solute mass fraction and water activity of the supercooled liquid phase, by modifications of the accommodation coefficient for water molecules, or by a combination thereof. The behavior of peak ice saturation ratios and total ice crystal number concentrations is examined, and the dependence of the results on cooling rate is investigated. Finally, processes are discussed that could possibly modify the homogeneous freezing behavior of organic particles.
Enabling Reproducible Science with VisTrails
David Koop,Juliana Freire,Claudio T. Silva
Computer Science , 2013,
Abstract: With the increasing amount of data and use of computation in science, software has become an important component in many different domains. Computing is now being used more often and in more aspects of scientific work including data acquisition, simulation, analysis, and visualization. To ensure reproducibility, it is important to capture the different computational processes used as well as their executions. VisTrails is an open-source scientific workflow system for data analysis and visualization that seeks to address the problem of integrating varied tools as well as automatically documenting the methods and parameters employed. Growing from a specific project need to supporting a wide array of users required close collaborations in addition to new research ideas to design a usable and efficient system. The VisTrails project now includes standard software processes like unit testing and developer documentation while serving as a base for further research. In this paper, we describe how VisTrails has developed and how our efforts in structuring and advertising the system have contributed to its adoption in many domains.
Amorphous and crystalline aerosol particles interacting with water vapor – Part 1: Microstructure, phase transitions, hygroscopic growth and kinetic limitations
E. Mikhailov,S. Vlasenko,S. T. Martin,T. Koop
Atmospheric Chemistry and Physics Discussions , 2009,
Abstract: Interactions with water are crucial for the properties, transformation and climate effects of atmospheric aerosols. Here we outline characteristic features and differences in the interaction of amorphous and crystalline aerosol particles with water vapor. Using a hygroscopicity tandem differential mobility analyzer (H-TDMA), we performed hydration, dehydration and cyclic hydration&dehydration experiments with aerosol particles composed of levoglucosan, oxalic acid and ammonium sulfate (diameters ~100–200 nm, relative uncertainties <0.4%, relative humidities <5% to 95% at 298 K). The measurements and accompanying K hler model calculations provide new insights into particle microstructure, surface adsorption, bulk absorption, phase transitions and hygroscopic growth. The results of these and related investigations lead to the following main conclusions: 1. Many organic substances (including carboxylic acids, carbohydrates and proteins) tend to form amorphous rather than crystalline phases upon drying of aqueous solution droplets. Depending on viscosity and microstructure, the amorphous phases can be classified as glasses, rubbers, gels or viscous liquids. 2. Amorphous organic substances tend to absorb water vapor and undergo gradual deliquescence and hygroscopic growth at much lower relative humidity than their crystalline counterparts. 3. In the course of hydration and dehydration, certain organic substances can form rubber- or gel-like structures (supra-molecular networks) and undergo stepwise transitions between swollen and collapsed network structures. 4. Organic gels or (semi-)solid amorphous shells (glassy, rubbery, ultra-viscous) with low molecular diffusivity can kinetically limit the uptake and release of water by submicron aerosol particles on (multi-)second time scales, which may influence the hygroscopic growth and activation of aerosol particles as cloud condensation nuclei (CCN) and ice nuclei (IN). 5. The shape and porosity of amorphous and crystalline particles formed upon dehydration of aqueous solution droplets depend on chemical composition and drying conditions. The apparent volume void fractions of particles with highly porous structures can range up to ~50% or more (xerogels, aerogels). Void fractions as well as residual water in dried aerosol particles that are not water-free (due to kinetic limitations of drying or stable hydrate formation) should be taken into account in K hler model calculations of hygroscopic growth and CCN activation. 6. For efficient description of water uptake and phase transitions of amorphous and crystallin
Kinetic multi-layer model of gas-particle interactions in aerosols and clouds (KM-GAP): linking condensation, evaporation and chemical reactions of organics, oxidants and water
M. Shiraiwa, C. Pfrang, T. Koop,U. P schl
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2012,
Abstract: We present a novel kinetic multi-layer model for gas-particle interactions in aerosols and clouds (KM-GAP) that treats explicitly all steps of mass transport and chemical reaction of semi-volatile species partitioning between gas phase, particle surface and particle bulk. KM-GAP is based on the PRA model framework (P schl-Rudich-Ammann, 2007), and it includes gas phase diffusion, reversible adsorption, surface reactions, bulk diffusion and reaction, as well as condensation, evaporation and heat transfer. The size change of atmospheric particles and the temporal evolution and spatial profile of the concentration of individual chemical species can be modeled along with gas uptake and accommodation coefficients. Depending on the complexity of the investigated system and the computational constraints, unlimited numbers of semi-volatile species, chemical reactions, and physical processes can be treated, and the model shall help to bridge gaps in the understanding and quantification of multiphase chemistry and microphysics in atmospheric aerosols and clouds. In this study we demonstrate how KM-GAP can be used to analyze, interpret and design experimental investigations of changes in particle size and chemical composition in response to condensation, evaporation, and chemical reaction. For the condensational growth of water droplets, our kinetic model results provide a direct link between laboratory observations and molecular dynamic simulations, confirming that the accommodation coefficient of water at ~270 K is close to unity (Winkler et al., 2006). Literature data on the evaporation of dioctyl phthalate as a function of particle size and time can be reproduced, and the model results suggest that changes in the experimental conditions like aerosol particle concentration and chamber geometry may influence the evaporation kinetics and can be optimized for efficient probing of specific physical effects and parameters. With regard to oxidative aging of organic aerosol particles, we illustrate how the formation and evaporation of volatile reaction products like nonanal can cause a decrease in the size of oleic acid particles exposed to ozone.
Oxalic acid as a heterogeneous ice nucleus in the upper troposphere and its indirect aerosol effect
B. Zobrist,C. Marcolli,T. Koop,B. P. Luo
Atmospheric Chemistry and Physics Discussions , 2006,
Abstract: Heterogeneous ice freezing points of aqueous solutions containing various immersed solid dicarboxylic acids (oxalic, adipic, succinic, phthalic and fumaric) have been measured with a differential scanning calorimeter. The results show that only the dihydrate of oxalic acid (OAD) acts as a heterogeneous ice nucleus, with an increase in freezing temperature between 2-5 K depending on solution composition. In several field campaigns, oxalic acid enriched particles have been detected in the upper troposphere with single particle aerosol mass spectrometry. Simulations with a microphysical box model indicate that the presence of OAD may reduce the ice particle number density in cirrus clouds by up to ~50% when compared to exclusively homogeneous cirrus formation without OAD. Using the ECHAM4 climate model we estimate the global net radiative effect caused by this heterogeneous freezing to result in a cooling as high as -0.3 Wm-2.
A novel model to predict the physical state of atmospheric H2SO4/NH3/H2O aerosol particles
C. A. Colberg,B. P. Luo,H. Wernli,T. Koop
Atmospheric Chemistry and Physics Discussions , 2002,
Abstract: The physical state of tropospheric aerosol particles is largely unknown despite its importance for cloud formation and for the aerosols' radiative properties. Here we show the first systematic global modelling study of the physical state of the H2SO4/NH3/H2O aerosol, which constitutes an important class of aerosols in the free troposphere. The Aerosol Physical State Model (APSM) developed here is based on Lagrangian trajectories computed from ECMWF (European Centre for Medium Range Weather Forecasts) analyses, taking full account of the deliquescence/efflorescence hysteresis. As input APSM requires three data sets: (i) deliquescence and efflorescence relative humidities from laboratory measurements, (ii) ammonia-to-sulfate ratios (ASR) calculated by a global circulation model, and (iii) relative humidities determined from the ECMWF analyses. APSM results indicate that globally averaged a significant fraction (17-57%) of the ammoniated sulfate aerosol particles contain solids with the ratio of solid-containing to purely liquid particles increasing with altitude (between 2 and 10 km). In our calculations the most abundant solid is letovicite, (NH4)3H(SO4)2, while there is only little ammonium sulfate, (NH4)2SO4. Since ammonium bisulfate, NH4HSO4, does not nucleate homogeneously, it can only form via heterogeneous crystallization. As the ammonia-to-sulfate ratios of the atmospheric aerosol usually do not correspond to the stoichiometries of known crystalline substances, all solids are expected to occur in mixed-phase aerosol particles. This work highlights the global importance of letovicite, whose role as cloud condensation nucleus (CCN) and as scatterer of solar radiation remains to be scrutinized.
Do atmospheric aerosols form glasses?
B. Zobrist,C. Marcolli,D. A. Pedernera,T. Koop
Atmospheric Chemistry and Physics Discussions , 2008,
Abstract: A new process is presented by which water-soluble organics might influence ice nucleation, ice growth, chemical reactions and water uptake of aerosols in the upper troposphere: the formation of glassy aerosol particles. Glasses are disordered amorphous (non-crystalline) solids that form when a liquid is cooled without crystallization until the viscosity increases exponentially and molecular diffusion practically ceases. The glass transition temperatures, Tg, homogeneous ice nucleation temperatures, Thom, and ice melting temperatures, Tm, of various aqueous inorganic, organic and multi-component solutions are investigated with a differential scanning calorimeter. The investigated solutes are: various polyols, glucose, raffinose, levoglucosan, an aromatic compound, sulfuric acid, ammonium bisulphate and mixtures of dicarboxylic acids (M5), of dicarboxylic acids and ammonium sulphate (M5AS), of two polyols, of glucose and ammonium nitrate, and of raffinose and M5AS. The results indicate that aqueous solutions of the investigated inorganic solutes show Tg-values that are too low to be of atmospheric importance. In contrast, aqueous organic and multi-component solutions readily form glasses at low but atmospherically relevant temperatures (≤230 K). To apply the laboratory data to the atmospheric situation, the measured phase transition temperatures were transformed from a concentration to a water activity scale by extrapolating water activities determined between 252 K and 313 K to lower temperatures. The obtained state diagrams reveal that the higher the molar mass of the aqueous organic or multi-component solutes, the higher Tg of their respective solutions at a given water activity. To a lesser extent, Tg also depends on the hydrophilicity of the organic solutes. Therefore, aerosol particles containing larger and more hydrophobic organic molecules ( 150 g mol-1) are more likely to form glasses at intermediate to high relative humidities in the upper troposphere. Our results suggest that the water uptake of aerosols, heterogeneous chemical reactions in aerosol particles, as well as ice nucleation and ice crystal growth can be significantly impeded or even completely inhibited in organic-enriched aerosols at upper tropospheric temperatures with implications for cirrus cloud formation and upper tropospheric relative humidity.
Do atmospheric aerosols form glasses?
B. Zobrist,C. Marcolli,D. A. Pedernera,T. Koop
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2008,
Abstract: A new process is presented by which water soluble organics might influence ice nucleation, ice growth, chemical reactions and water uptake of aerosols in the upper troposphere: the formation of glassy aerosol particles. Glasses are disordered amorphous (non-crystalline) solids that form when a liquid is cooled without crystallization until the viscosity increases exponentially and molecular diffusion practically ceases. The glass transition temperatures, Tg, homogeneous ice nucleation temperatures, Thom, and ice melting temperatures, Tm, of various aqueous inorganic, organic and multi-component solutions are investigated with a differential scanning calorimeter. The investigated solutes are: various polyols, glucose, raffinose, levoglucosan, an aromatic compound, sulfuric acid, ammonium bisulfate and mixtures of dicarboxylic acids (M5), of dicarboxylic acids and ammonium sulfate (M5AS), of two polyols, of glucose and ammonium nitrate, and of raffinose and M5AS. The results indicate that aqueous solutions of the investigated inorganic solutes show Tg values that are too low to be of atmospheric importance. In contrast, aqueous organic and multi-component solutions readily form glasses at low but atmospherically relevant temperatures (≤230 K). To apply the laboratory data to the atmospheric situation, the measured phase transition temperatures were transformed from a concentration to a water activity scale by extrapolating water activities determined between 252 K and 313 K to lower temperatures. The obtained state diagrams reveal that the higher the molar mass of the aqueous organic or multi-component solutes, the higher Tg of their respective solutions at a given water activity. To a lesser extent, Tg also depends on the hydrophilicity of the organic solutes. Therefore, aerosol particles containing larger ( 150 g mol 1) and more hydrophobic organic molecules are more likely to form glasses at intermediate to high relative humidities in the upper troposphere. Our results suggest that the water uptake of aerosols, heterogeneous chemical reactions in aerosol particles, as well as ice nucleation and ice crystal growth can be significantly impeded or even completely inhibited in organic-enriched aerosols at upper tropospheric temperatures with implications for cirrus cloud formation and upper tropospheric relative humidity.
Kinetic multi-layer model of gas-particle interactions in aerosols and clouds (KM-GAP): linking condensation, evaporation and chemical reactions of organics, oxidants and water
M. Shiraiwa,C. Pfrang,T. Koop,U. P?schl
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2012, DOI: 10.5194/acp-12-2777-2012
Abstract: We present a novel kinetic multi-layer model for gas-particle interactions in aerosols and clouds (KM-GAP) that treats explicitly all steps of mass transport and chemical reaction of semi-volatile species partitioning between gas phase, particle surface and particle bulk. KM-GAP is based on the PRA model framework (P schl-Rudich-Ammann, 2007), and it includes gas phase diffusion, reversible adsorption, surface reactions, bulk diffusion and reaction, as well as condensation, evaporation and heat transfer. The size change of atmospheric particles and the temporal evolution and spatial profile of the concentration of individual chemical species can be modeled along with gas uptake and accommodation coefficients. Depending on the complexity of the investigated system and the computational constraints, unlimited numbers of semi-volatile species, chemical reactions, and physical processes can be treated, and the model shall help to bridge gaps in the understanding and quantification of multiphase chemistry and microphysics in atmospheric aerosols and clouds. In this study we demonstrate how KM-GAP can be used to analyze, interpret and design experimental investigations of changes in particle size and chemical composition in response to condensation, evaporation, and chemical reaction. For the condensational growth of water droplets, our kinetic model results provide a direct link between laboratory observations and molecular dynamic simulations, confirming that the accommodation coefficient of water at ~270 K is close to unity (Winkler et al., 2006). Literature data on the evaporation of dioctyl phthalate as a function of particle size and time can be reproduced, and the model results suggest that changes in the experimental conditions like aerosol particle concentration and chamber geometry may influence the evaporation kinetics and can be optimized for efficient probing of specific physical effects and parameters. With regard to oxidative aging of organic aerosol particles, we illustrate how the formation and evaporation of volatile reaction products like nonanal can cause a decrease in the size of oleic acid particles exposed to ozone.
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