scholarly journals Interaction of aerosol particles composed of protein and salts with water vapor: hygroscopic growth and microstructural rearrangement

2003 ◽  
Vol 3 (5) ◽  
pp. 4755-4832 ◽  
Author(s):  
E. Mikhailov ◽  
S. Vlasenko ◽  
R. Niessner ◽  
U. Pöschl
Keyword(s):  
Water Vapor ◽  
Mass Fraction ◽  
Osmotic Coefficient ◽  
Aerosol Particles ◽  
Dry Mass ◽  
Water Soluble ◽  
Equivalent Diameter ◽  
Hygroscopic Growth ◽  
Air Particulate ◽  
Kohler Theory

Abstract. The interaction of aerosol particles in the 100–200 nm size range composed of the protein bovine serum albumin (BSA) and the inorganic salts sodium chloride and ammonium nitrate with water vapor at ambient temperature and pressure (25°C, 1 atm) has been investigated by hygroscopicity tandem differential mobility analyzer (H-TDMA) experiments complemented by transmission electron microscopy (TEM) and Köhler theory calculations. BSA was chosen as a well-defined model substance for proteins and other macromolecular compounds, which constitute a large fraction of the water-soluble organic component of air particulate matter. Pure BSA particles exhibited deliquescence and efflorescence transitions at ~35% relative humidity (RH) and a hygroscopic diameter increase by up to ~10% at 95% RH in good agreement with model calculations based on a simple parameterisation of the osmotic coefficient. Pure NaCl particles were converted from near-cubic to near-spherical or polyhedral shape upon interaction with water vapor at relative humidities below the deliquescence threshold (partial surface dissolution and recrystallisation), and the diameters of pure NH4NO3 particles decreased by up to 10% due to chemical decomposition and evaporation. Mixed NaCl-BSA and NH4NO3-BSA particles interacting with water vapor exhibited mobility equivalent diameter reductions of up to 20%, depending on particle generation, conditioning, size, and chemical composition (BSA dry mass fraction 10–90%). These observations can be explained by formation of porous agglomerates (envelope void fractions up to 50%) due to ion-protein interactions and electric charge effects on the one hand, and by compaction of the agglomerate structure due to capillary condensation effects on the other. The size of NH4NO3-BSA particles was apparently also influenced by volatilisation of NH4NO3, but not as much as for pure salt particles, i.e. the protein inhibited the decomposition of NH4NO3 or the evaporation of the decomposition products NH3 and HNO3. The efflorescence threshold of NaCl-BSA particles decreased with increasing BSA dry mass fraction, i.e. the protein inhibited the formation of salt crystals and enhanced the stability of supersaturated solution droplets. The H-TDMA and TEM results indicate that the protein was enriched at the surface of the mixed particles and formed an envelope, which inhibits the access of water vapor to the particle core and leads to kinetic limitations of hygroscopic growth, phase transitions, and microstructural rearrangement processes. Besides these surface and kinetic effects, proteins and comparable organic macromolecules may also influence the thermodynamic properties of the aqueous bulk solution (solubilities, vapor pressures, and chemical equilibria, e.g. for the decomposition and evaporation of NH4NO3. The observed effects should be taken into account in the analysis of data from laboratory experiments and field measurements and in the modelling of aerosol processes involving water vapor and particles with complex composition. They can strongly influence experimental results, and depending on ambient conditions they may also play a significant role in the atmosphere (deliquescence, efflorescence, and CCN activation of particles). In fact, irregular hygroscopic growth curves similar to the ones observed in this study have recently been reported from H-TDMA experiments with water-soluble organics extracted from real air particulate matter and with humic-like substances. The Köhler theory calculations performed with different models demonstrate that the hygroscopic growth of particles composed of inorganic salts and proteins can be efficiently described with a simple volume additivity approach, provided that the correct dry solute mass equivalent diameter and composition are known. A simple parameterisation of the osmotic coefficient has been derived from an osmotic pressure virial equation and appears to be well-suited for proteins and comparable substances. It is fully compatible with traditional volume additivity models for salt mixtures, and for its application only the density and molar mass of the substance have to be known or estimated.

scholarly journals Interaction of aerosol particles composed of protein and saltswith water vapor: hygroscopic growth and microstructural rearrangement

2004 ◽  
Vol 4 (2) ◽  
pp. 323-350 ◽  
Author(s):  
E. Mikhailov ◽  
S. Vlasenko ◽  
R. Niessner ◽  
U. Pöschl
Keyword(s):  
Water Vapor ◽  
Mass Fraction ◽  
Osmotic Coefficient ◽  
Aerosol Particles ◽  
Dry Mass ◽  
Virial Equation ◽  
Inorganic Salts ◽  
Equivalent Diameter ◽  
Hygroscopic Growth ◽  
Kohler Theory

Abstract. The interaction of aerosol particles composed of the protein bovine serum albumin (BSA) and the inorganic salts sodium chloride and ammonium nitrate with water vapor has been investigated by hygroscopicity tandem differential mobility analyzer (H-TDMA) experiments complemented by transmission electron microscopy (TEM) and Köhler theory calculations (100-300nm particle size range, 298K, 960hPa). BSA was chosen as a well-defined model substance for proteins and other macromolecular compounds, which constitute a large fraction of the water-soluble organic component of air particulate matter. Pure BSA particles exhibited deliquescence and efflorescence transitions at 35% relative humidity () and a hygroscopic diameter increase by up to 10% at 95% in good agreement with model calculations based on a simple parameterisation of the osmotic coefficient. Pure NaCl particles were converted from near-cubic to near-spherical shape upon interaction with water vapor at relative humidities below the deliquescence threshold (partial surface dissolution and recrystallisation), and the diameters of pure NH4NO3 particles decreased by up to 10% due to chemical decomposition and evaporation. Mixed NaCl-BSA and NH4NO3-BSA particles interacting with water vapor exhibited mobility equivalent diameter reductions of up to 20%, depending on particle generation, conditioning, size, and chemical composition (BSA dry mass fraction 10-90%). These observations can be explained by formation of porous agglomerates (envelope void fractions up to 50%) due to ion-protein interactions and electric charge effects on the one hand, and by compaction of the agglomerate structure due to capillary condensation effects on the other. The size of NH4NO3-BSA particles was apparently also influenced by volatilisation of NH4NO3, but not as much as for pure salt particles, i.e. the protein inhibited the decomposition of NH4NO3 or the evaporation of the decomposition products NH3 and HNO3. The efflorescence threshold of NaCl-BSA particles decreased with increasing BSA dry mass fraction, i.e. the protein inhibited the formation of salt crystals and enhanced the stability of supersaturated solution droplets. The H-TDMA and TEM results indicate that the protein was enriched at the surface of the mixed particles and formed an envelope, which inhibits the access of water vapor to the particle core and leads to kinetic limitations of hygroscopic growth, phase transitions, and microstructural rearrangement processes. The Köhler theory calculations performed with different types of models demonstrate that the hygroscopic growth of particles composed of inorganic salts and proteins can be efficiently described with a simple volume additivity approach, provided that the correct dry solute mass equivalent diameter and composition are known. A parameterisation for the osmotic coefficient of macromolecular substances has been derived from an osmotic pressure virial equation. For its application only the density and molar mass of the substance have to be known or estimated, and it is fully compatible with traditional volume additivity models for salt mixtures.

scholarly journals Secondary aerosol formation promotes water uptake by organic-rich wildfire haze particles in Equatorial Asia

2017 ◽  
Author(s):  
Jing Chen ◽  
Sri Hapsari Budisulistiorini ◽  
Takuma Miyakawa ◽  
Yuichi Komazaki ◽  
Mikinori Kuwata
Keyword(s):  
Water Uptake ◽  
Mass Fraction ◽  
Water Soluble ◽  
Submicron Particles ◽  
Chemical Information ◽  
Hygroscopic Growth ◽  
Aerosol Formation ◽  
Secondary Formation ◽  
Soluble Organic Fraction ◽  
Haze Episode

Abstract. Diameter growth factors (GF) of 100 nm haze particles at 85 % relative humidity and chemical characteristics were simultaneously monitored at Singapore in October 2015 during a pervasive wildfire haze episode, which was caused by peatland burning in Indonesia. Non-refractory submicron particles (NR-PM1) were dominated by organics (approximating 77.1 % in total mass), whereas sulfate was the most abundant inorganic constituent (11.7 % on average). A statistical analysis of the organic mass spectra showed that most of organics (36.0 % of NR-PM1 mass) were highly oxygenated. Diurnal variations of GF, number fraction of highly hygroscopic mode particles, mass fraction of sulfate, and mass fraction of oxygenated organics (OOA) synchronized well, peaking during daytime. The mean hygroscopicity parameter (κ) of haze particles was 0.189 ± 0.087, and mean κ values of organics were 0.157 ± 0.108 (κorg, bulk organics) and 0.287 ± 0.193 (κOOA, OOA), demonstrating the important roles of both sulfate and highly oxygenated organics in hygroscopic growth of wildfire haze particles. κorg was also affected by the water-soluble organic fraction to some extent. These results show the importance of secondary formation processes in promoting water uptake properties of wildfire haze particles, including both inorganic and organic species. Further detailed size-resolved as well as molecular level chemical information of organics will be necessary for more profound exploration of water uptake by wildfire haze particles in Equatorial Asia.

scholarly journals Synergistic effect of water-soluble species and relative humidity on morphological changes of aerosol particles in Beijing mega-city during severe pollution episodes

2018 ◽  
Author(s):  
Xiaole Pan ◽  
Baozhu Ge ◽  
Zhe Wang ◽  
Yu Tian ◽  
Hang Liu ◽  
...  
Keyword(s):  
Relative Humidity ◽  
Synergistic Effect ◽  
Mass Fraction ◽  
Mass Concentration ◽  
Morphological Changes ◽  
Aerosol Particles ◽  
Water Soluble ◽  
Coarse Mode ◽  
Heavy Pollution ◽  
Soluble Species

Abstract. Depolarization ratio (δ) of backscattered light from aerosol particle is an applicable parameter for real-time distinguishing spherical and non-spherical particles, which has been widely adopted by ground-based Lidar observation and satellite remote sensing. From November 2016 to February of 2017, it consecutively suffered from numbers of severe air pollution at Beijing with daily averaged mass concentration of PM2.5 (aerodynamic diameter less than 2.5 μm) larger than 150 μg/m3. We preformed concurrent measurements of water-soluble chemical species and depolarization properties of aerosol particles on the basis of a continuous dichotomous Aerosol Chemical Speciation Analyzer (ACSA-14) and a bench-top optical particle counter with a polarization detection module (POPC). We found that δ value of ambient particles generally decrease as mass concentration of PM2.5 increased at unfavorable meteorological condition. Ratio of mass concentration of nitrate (NO3−) to that of sulfate (SO42−) in PM2.5 was 1.5 ± 0.6, indicating of great importance of NOx in the formation of heavy pollution. Mass concentration of NO3− in PM2.5 (fNO3) was generally an order of magnitude higher than that in coarse mode (cNO3) with a mean fNO3 / cNO3 ratio of 14 ± 10. Relatively high allocation (fNO3/cNO3 = 5) of NO3− in coarse mode could be partially attributed to hygroscopic growth/coagulation of nitrate-rich fine mode particles under higher relative humidity condition. As a result, δ values of particles with Dp = 2 μm (δDp = 2) and 5 μm (δDp = 5) decreased evidently as the mass fraction of water-soluble species (NO3− and SO42−) increase in both PM2.5 and PM2.5–10, respectively. In particular, due to synergistic effect of RH, δDp = 5 value could decrease by 50 % as mass fraction of NO3− in PM2.5–10 increased from 8 % to 23 %. It suggested that alteration of non-sphericity of mineral dust particles was evident owing to coating with pollutants and heterogeneous reactions on the surface of the particle during heavy pollution period. This study brings the attention to great variability of morphological changes of aerosol particles along the transport, which have great complex effects in evaluating their climate and health effect.

scholarly journals Technical note: Analytical formulae for the critical supersaturations and droplet diameters of CCN containing insoluble material

2008 ◽  
Vol 8 (7) ◽  
pp. 1985-1988 ◽  
Author(s):  
H. Kokkola ◽  
M. Vesterinen ◽  
T. Anttila ◽  
A. Laaksonen ◽  
K. E. J. Lehtinen
Keyword(s):  
Aerosol Particles ◽  
Technical Note ◽  
Water Soluble ◽  
Cloud Drop ◽  
Insoluble Material ◽  
Kohler Theory ◽  
Analytical Formulae ◽  
Molecular Sizes ◽  
Organic Particles ◽  
Soluble Material

Abstract. In this paper, we consider the cloud drop activation of aerosol particles consisting of water soluble material and an insoluble core. Based on the Köhler theory, we derive analytical equations for the critical diameters and supersaturations of such particles. We demonstrate the use of the equations by comparing the critical supersaturations of particles composed of ammonium sulfate and insoluble substances with those of model organic particles with varying molecular sizes.

scholarly journals Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

2015 ◽  
Vol 15 (15) ◽  
pp. 8847-8869 ◽  
Author(s):  
E. F. Mikhailov ◽  
G. N. Mironov ◽  
C. Pöhlker ◽  
X. Chi ◽  
M. L. Krüger ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Water Uptake ◽  
Aerosol Particles ◽  
Organic Coating ◽  
Water Soluble ◽  
Submicron Particles ◽  
Hygroscopic Growth ◽  
Accumulation Mode ◽  
Hygroscopic Properties ◽  
Coarse Mode

Abstract. In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in central Siberia (61° N, 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical compositions of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38 % of particulate matter (PM) in the accumulation mode and coarse mode, respectively. The water-soluble fraction of organic matter was estimated to be 52 and 8 % of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34 % in the accumulation mode vs. ~ 47 % in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4 % RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same relative humidity (RH), starting at ~ 70 %, while efflorescence occurred at different humidities, i.e., at ~ 35 % RH for submicron particles vs. ~ 50 % RH for supermicron particles. This ~ 15 % RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4 % RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv,ws value related to the water-soluble (ws) fraction was estimated to be ~ 0.15 for the accumulation mode and ~ 0.36 for the coarse mode, respectively. The obtained κv,ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (κv ≈ 0.15) and a Colorado mountain forest (κv ≈ 0.16 ). We used the Zdanovskii–Stokes–Robinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, κv,p. The obtained κv,p values overestimate the experimental FDHA-KIM-derived κv,ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (> 300 nm) and supermicron aerosol particles possess core–shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ~ 10−12 cm2 s−1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall, the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second timescales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.

scholarly journals The rate of equilibration of viscous aerosol particles

2016 ◽  
Vol 16 (8) ◽  
pp. 5299-5313 ◽  
Author(s):  
Simon O'Meara ◽  
David O. Topping ◽  
Gordon McFiggans
Keyword(s):  
Diffusion Coefficient ◽  
Diffusion Coefficients ◽  
Aerosol Particles ◽  
Volatile Component ◽  
Water Soluble ◽  
Ambient Atmosphere ◽  
Equilibration Time ◽  
Hygroscopic Growth ◽  
Research Activity ◽  
Model Framework

Abstract. The proximity of atmospheric aerosol particles to equilibrium with their surrounding condensable vapours can substantially impact their transformations, fate and impacts and is the subject of vibrant research activity. In this study we first compare equilibration timescales estimated by three different models for diffusion through aerosol particles to assess any sensitivity to choice of model framework. Equilibration times for diffusion coefficients with varying dependencies on composition are compared for the first time. We show that even under large changes in the saturation ratio of a semi-volatile component (es) of 1–90 % predicted equilibration timescales are in agreement, including when diffusion coefficients vary with composition. For condensing water and a diffusion coefficient dependent on composition, a plasticising effect is observed, leading to a decreased estimated equilibration time with increasing final es. Above 60 % final es maximum equilibration times of around 1 s are estimated for comparatively large particles (10 µm) containing a relatively low diffusivity component (1  ×  10−25 m2 s−1 in pure form). This, as well as other results here, questions whether particle-phase diffusion through water-soluble particles can limit hygroscopic growth in the ambient atmosphere. In the second part of this study, we explore sensitivities associated with the use of particle radius measurements to infer diffusion coefficient dependencies on composition using a diffusion model. Given quantified similarities between models used in this study, our results confirm considerations that must be taken into account when designing such experiments. Although quantitative agreement of equilibration timescales between models is found, further work is necessary to determine their suitability for assessing atmospheric impacts, such as their inclusion in polydisperse aerosol simulations.

scholarly journals Hygroscopic properties of smoke-generated organic aerosol particles emitted in the marine atmosphere

2013 ◽  
Vol 13 (19) ◽  
pp. 9819-9835 ◽  
Author(s):  
A. Wonaschütz ◽  
M. Coggon ◽  
A. Sorooshian ◽  
R. Modini ◽  
A. A. Frossard ◽  
...  
Keyword(s):  
Mass Fraction ◽  
Cloud Condensation Nuclei ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Marine Atmosphere ◽  
Hygroscopic Growth ◽  
Organic Mass ◽  
Aerosol Mass ◽  
Hygroscopic Properties ◽  
Mass Fractions

Abstract. During the Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE), a plume of organic aerosol was produced by a smoke generator and emitted into the marine atmosphere from aboard the R/V Point Sur. In this study, the hygroscopic properties and the chemical composition of the plume were studied at plume ages between 0 and 4 h in different meteorological conditions. In sunny conditions, the plume particles had very low hygroscopic growth factors (GFs): between 1.05 and 1.09 for 30 nm and between 1.02 and 1.1 for 150 nm dry size at a relative humidity (RH) of 92%, contrasted by an average marine background GF of 1.6. New particles were produced in large quantities (several 10 000 cm−3), which lead to substantially increased cloud condensation nuclei (CCN) concentrations at supersaturations between 0.07 and 0.88%. Ratios of oxygen to carbon (O : C) and water-soluble organic mass (WSOM) increased with plume age: from < 0.001 to 0.2, and from 2.42 to 4.96 μg m−3, respectively, while organic mass fractions decreased slightly (~ 0.97 to ~ 0.94). High-resolution aerosol mass spectrometer (AMS) spectra show that the organic fragment m/z 43 was dominated by C2H3O+ in the small, new particle mode and by C3H7+ in the large particle mode. In the marine background aerosol, GFs for 150 nm particles at 40% RH were found to be enhanced at higher organic mass fractions: an average GF of 1.06 was observed for aerosols with an organic mass fraction of 0.53, and a GF of 1.04 for an organic mass fraction of 0.35.

scholarly journals Importance of aerosol composition and mixing state for cloud droplet activation in the high Arctic

2014 ◽  
Vol 14 (15) ◽  
pp. 21223-21283 ◽  
Author(s):  
C. Leck ◽  
E. Svensson
Keyword(s):  
Water Vapor ◽  
Cloud Droplet ◽  
Polymer Gels ◽  
High Arctic ◽  
Water Soluble ◽  
Local Source ◽  
Aerosol Composition ◽  
Pack Ice ◽  
Kohler Theory ◽  
Droplet Activation

Abstract. Concentrations of cloud condensation nuclei (CCN) were measured throughout an expedition by icebreaker around the central Arctic Ocean, including a 3 week ice drift operation at 87° N, from 3 August to 9 September 2008. In agreement with previous observations in the area and season median daily CCN concentrations at 0.2% water vapor supersaturation were typically in the range of 15 to 30 cm−3, but concentrations varied by two to three orders of magnitude over the expedition and were occasionally below 1 cm−3. The CCN concentrations were highest near the ice edge and fell by a factor of three in the first 48 h of transport from the open sea into the pack ice region. For longer transport times they increased again indicating a local source over the pack ice, suggested to be polymer gels, via drops injected into the air by bubbles bursting on open leads. By assuming Köhler theory and simulating the cloud nucleation process using a Lagrangian adiabatic air parcel model that solves the kinetic formulation for condensation of water on size resolved aerosol particles we inferred the properties of the unexplained non-water soluble aerosol fraction that is necessary for reproducing the observed concentrations of CCN. We propose that the portion of the internally/externally mixed water insoluble particles was larger in the corresponding smaller aerosol sizes ranges. These particles were physically and chemically behaving as polymer gels: the interaction of the hydrophilic and hydrophobic entities on the structures of polymer gels during cloud droplet activation would at first only show a partial wetting character and only weak hygroscopic growth. Given time, a high CCN activation efficiency is achieved, which is promoted by the hydrophilicity or surface-active properties of the gels. Thus the result in this study argues for that the behavior of the high Arctic aerosol in CCN-counters operating at water vapor supersaturations > 0.4% (high relative humidities) may not be properly explained by conventional Köhler theory.

scholarly journals Technical Note: Analytical formulae for the critical supersaturations and droplet diameters of CCN containing insoluble material

2007 ◽  
Vol 7 (6) ◽  
pp. 17967-17974
Author(s):  
H. Kokkola ◽  
M. Vesterinen ◽  
T. Anttila ◽  
A. Laaksonen ◽  
K. E. J. Lehtinen
Keyword(s):  
Aerosol Particles ◽  
Technical Note ◽  
Water Soluble ◽  
Cloud Drop ◽  
Insoluble Material ◽  
Kohler Theory ◽  
Analytical Formulae ◽  
Molecular Sizes ◽  
Organic Particles ◽  
Soluble Material

Abstract. In this paper, we consider the cloud drop activation of aerosol particles consisting of water soluble material and an insoluble core. Based on the Köhler theory, we derive analytical equations for the critical diameters and supersaturations of such particles. We demonstrate the use of the equations by comparing the critical supersaturations of particles composed of ammonium sulfate and insoluble substances with those of model organic particles with varying molecular sizes.

scholarly journals Hygroscopic growth and critical supersaturations for mixed aerosol particles of inorganic and organic compounds of atmospheric relevance

2005 ◽  
Vol 5 (3) ◽  
pp. 2833-2877 ◽  
Author(s):  
B. Svenningsson ◽  
J. Rissler ◽  
E. Swietlicki ◽  
M. Mircea ◽  
M. Bilde ◽  
...  
Keyword(s):  
Sodium Chloride ◽  
Succinic Acid ◽  
Organic Compounds ◽  
Water Activity ◽  
Aerosol Particles ◽  
Water Soluble ◽  
Mixing Rule ◽  
Hygroscopic Growth ◽  
Organic Fraction ◽  
Surface Tensions

Abstract. The organic fraction of atmospheric aerosols contains a multitude of compounds and usually only a small fraction can be identified and quantified. However, a limited number of representative organic compounds can be used to describe the water-soluble organic fraction. In this work, initiated within the EU 5FP project SMOCC, four mixtures containing various amounts of inorganic salts (ammonium sulfate, ammonium nitrate, and sodium chloride) and three model organic compounds (levoglucosan, succinic acid and fulvic acid) were studied. The interaction between water vapor and aerosol particles was studied at different relative humidities: at subsaturation using a hygroscopic tandem differential mobility analyzer (H-TDMA) and at supersaturation using a cloud condensation nuclei spectrometer (CCN spectrometer). Surface tensions as a function of carbon concentrations were measured using a bubble tensiometer. Parameterizations of water activity as a function of molality, based on hygroscopic growth, are given for the pure organic compounds and for the mixtures, indicating van't Hoff factors around 1 for the organics. The Zdanovskii-Stokes-Robinson (ZSR) mixing rule was tested on the hygroscopic growth of the mixtures and it was found to adequately explain the hygroscopic growth for 3 out of 4 mixtures, when the limited solubility of succinic acid is taken into account. One mixture containing sodium chloride was studied and showed a pronounced deviation from the ZSR mixing rule. Critical supersaturations calculated using the parameterizations of water activity and the measured surface tensions were compared with those determined experimentally.

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