scholarly journals Cloud Activating Properties of Aerosol Observed during CELTIC

2007 ◽  
Vol 64 (2) ◽  
pp. 441-459 ◽  
Author(s):  
Craig A. Stroud ◽  
Athanasios Nenes ◽  
Jose L. Jimenez ◽  
Peter F. DeCarlo ◽  
J. Alex Huffman ◽  
...  
Keyword(s):  
Kinetic Model ◽  
Size Distribution ◽  
Organic Aerosol ◽  
Aerosol Size Distribution ◽  
Model Bias ◽  
Aerosol Composition ◽  
Ambient Aerosol ◽  
Aerosol Mass ◽  
Mass Fractions ◽  
Mass Size

Abstract 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.

scholarly journals The link between organic aerosol mass loading and degree of oxygenation: an α-pinene photooxidation study

2013 ◽  
Vol 13 (13) ◽  
pp. 6493-6506 ◽  
Author(s):  
L. Pfaffenberger ◽  
P. Barmet ◽  
J. G. Slowik ◽  
A. P. Praplan ◽  
J. Dommen ◽  
...  
Keyword(s):  
Mass Spectra ◽  
Organic Aerosol ◽  
Mass Loading ◽  
Smog Chamber ◽  
Organic Mass ◽  
Aerosol Composition ◽  
Ambient Aerosol ◽  
Aerosol Mass ◽  
Hygroscopic Properties ◽  
Mass Concentrations

Abstract. A series of smog chamber (SC) experiments was conducted to identify factors responsible for the discrepancy between ambient and SC aerosol degree of oxygenation. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer is used to compare mass spectra from α-pinene photooxidation with ambient aerosol. Composition is compared in terms of the fraction of particulate CO2+, a surrogate for carboxylic acids, vs. the fraction of C2H3O+, a surrogate for aldehydes, alcohols and ketones, as well as in the Van Krevelen space, where the evolution of the atomic hydrogen-to-carbon ratio (H : C) vs. the atomic oxygen-to-carbon ratio (O : C) is investigated. Low (near-ambient) organic mass concentrations were found to be necessary to obtain oxygenation levels similar to those of low-volatility oxygenated organic aerosol (LV-OOA) commonly identified in ambient measurements. The effects of organic mass loading and OH (hydroxyl radical) exposure were decoupled by inter-experiment comparisons at the same integrated OH concentration. An OH exposure between 3 and 25 × 107 cm−3 h is needed to increase O : C by 0.05 during aerosol aging. For the first time, LV-OOA-like aerosol from the abundant biogenic precursor α-pinene was produced in a smog chamber by oxidation at typical atmospheric OH concentrations. Significant correlation between measured secondary organic aerosol (SOA) and reference LV-OOA mass spectra is shown by Pearson's R2 values larger than 0.90 for experiments with low organic mass concentrations between 1.2 and 18 μg m−3 at an OH exposure of 4 × 107 cm−3 h, corresponding to about two days of oxidation time in the atmosphere, based on a global mean OH concentration of ~ 1 × 106 cm−3. α-Pinene SOA is more oxygenated at low organic mass loadings. Because the degree of oxygenation influences the chemical, volatility and hygroscopic properties of ambient aerosol, smog chamber studies must be performed at near-ambient concentrations to accurately simulate ambient aerosol properties.

scholarly journals The link between organic aerosol mass loading and degree of oxygenation: an α-pinene photooxidation study

2012 ◽  
Vol 12 (9) ◽  
pp. 24735-24764 ◽  
Author(s):  
L. Pfaffenberger ◽  
P. Barmet ◽  
J. G. Slowik ◽  
A. P. Praplan ◽  
J. Dommen ◽  
...  
Keyword(s):  
Mass Spectra ◽  
Organic Aerosol ◽  
Mass Loading ◽  
Smog Chamber ◽  
Organic Mass ◽  
Aerosol Composition ◽  
Ambient Aerosol ◽  
Aerosol Mass ◽  
Hygroscopic Properties ◽  
Mass Concentrations

Abstract. A series of smog chamber (SC) experiments was conducted to identify driving factors responsible for the discrepancy between ambient and SC aerosol degree of oxygenation. An Aerodyne high resolution time-of-flight aerosol mass spectrometer is used to compare mass spectra from α-pinene photooxidation with ambient aerosol. Composition is compared in terms of the fraction of organic mass measured at m/z 44 (f44), a surrogate for carboxylic/organic acids as well as the atomic oxygen-to-carbon ratio (O : C), vs. f43, a surrogate for aldehydes, alcohols and ketones. Low (near-ambient) organic mass concentrations were found to be necessary to obtain oxygenation levels similar to those of low-volatility oxygenated organic aerosol (LV-OOA) commonly identified in ambient measurements. The effects of organic mass loading and OH (hydroxyl radical) exposure were decoupled by inter-experiment comparisons at the same integrated OH concentration. On average, an OH exposure of 2.9 ± 1.3 × 107 cm−3 h is needed to increase f44 by 1% during aerosol aging. For the first time, LV-OOA-like aerosol from the abundant biogenic precursor α-pinene was produced in a smog chamber by oxidation at typical atmospheric OH concentrations. Significant correlation between measured secondary organic aerosol (SOA) and reference LV-OOA mass spectra is shown by Pearson's R2 values larger than 0.90 for experiments with low organic mass concentrations between 1.5 and 15 μg m−3 at an OH exposure of 4 × 107 cm−3 h, corresponding to about two days oxidation time in the atmosphere, based on a global mean OH concentration of ∼1 × 106 cm−3. Not only is the α-pinene SOA more oxygenated at low organic mass loadings, but the functional dependence of oxygenation on mass loading is enhanced at atmospherically-relevant precursor concentrations. Since the degree of oxygenation influences the chemical, volatility and hygroscopic properties of ambient aerosol, smog chamber studies must be performed at near-ambient concentrations to accurately simulate ambient aerosol properties.

scholarly journals Physical properties of secondary photochemical aerosol from OH oxidation of a cyclic siloxane

2019 ◽  
Vol 19 (3) ◽  
pp. 1649-1664 ◽  
Author(s):  
Nathan J. Janechek ◽  
Rachel F. Marek ◽  
Nathan Bryngelson ◽  
Ashish Singh ◽  
Robert L. Bullard ◽  
...  
Keyword(s):  
Size Distribution ◽  
Flow Reactor ◽  
Oxidation Products ◽  
Aerosol Size Distribution ◽  
Atmospheric Models ◽  
Aerosol Mass ◽  
Differential Mobility Analysis ◽  
Mass Fractions ◽  
High Production ◽  
Seed Aerosol

Abstract. Cyclic volatile methyl siloxanes (cVMS) are high-production chemicals present in many personal care products. They are volatile, hydrophobic, and relatively long-lived due to slow oxidation kinetics. Evidence from chamber and ambient studies indicates that oxidation products may be found in the condensed aerosol phase. In this work, we use an oxidation flow reactor to produce ∼100 µg m−3 of organosilicon aerosol from OH oxidation of decamethylcyclopentasiloxane (D5) with aerosol mass fractions (i.e., yields) of 0.2–0.5. The aerosols were assessed for concentration, size distribution, morphology, sensitivity to seed aerosol, hygroscopicity, volatility and chemical composition through a combination of aerosol size distribution measurement, tandem differential mobility analysis, and electron microscopy. Similar aerosols were produced when vapor from solid antiperspirant was used as the reaction precursor. Aerosol yield was sensitive to chamber OH and to seed aerosol, suggesting sensitivity of lower-volatility species and recovered yields to oxidation conditions and chamber operation. The D5 oxidation aerosol products were relatively non-hygroscopic, with an average hygroscopicity kappa of ∼0.01, and nearly non-volatile up to 190 ∘C temperature. Parameters for exploratory treatment as a semi-volatile organic aerosol in atmospheric models are provided.

scholarly journals Physical Properties of Secondary Photochemical Aerosol from OH Oxidation of a Cyclic Siloxane

2018 ◽  
Author(s):  
Nathan J. Janechek ◽  
Rachel F. Marek ◽  
Nathan Bryngelson ◽  
Ashish Singh ◽  
Robert L. Bullard ◽  
...  
Keyword(s):  
Size Distribution ◽  
Flow Reactor ◽  
Oxidation Products ◽  
Aerosol Size Distribution ◽  
Atmospheric Models ◽  
Aerosol Mass ◽  
Differential Mobility Analysis ◽  
Mass Fractions ◽  
High Production ◽  
Seed Aerosol

Abstract. Cyclic volatile methyl siloxanes (cVMS) are high production chemicals present in many personal care products. They are volatile, hydrophobic, and relatively long-lived due to slow oxidation kinetics. Evidence from chamber and ambient studies indicates that oxidation products may be found in the condensed aerosol phase. In this work, we use an oxidation flow reactor to produce ~ 100 µg m−3 of organosilicon aerosol from OH oxidation of decamethylcyclopentasiloxane (D5) with aerosol mass fractions (i.e. yields) of 0.2–0.5. The aerosols were assessed for concentration, size distribution, morphology, sensitivity to seed aerosol, hygroscopicity, volatility and chemical composition through a combination of aerosol size distribution measurement, tandem differential mobility analysis, and electron microscopy. Similar aerosols were produced when vapor from solid antiperspirant or from hair conditioner was used as the reaction precursor. Aerosol yield was sensitive to chamber OH, indicating an interplay between oxidation conditions and the concentration of lower volatility species. The D5 oxidation aerosol products were relatively non-hygroscopic, with average hygroscopicity kappa of ~ 0.01, and nearly non-volatile up to 190 °C temperature. Recommended parameters for treatment as a semi-volatile organic aerosol in atmospheric models are provided.

scholarly journals Aerosol chemical and optical properties over the Paris area within ESQUIF project

2006 ◽  
Vol 6 (11) ◽  
pp. 3257-3280 ◽  
Author(s):  
A. Hodzic ◽  
R. Vautard ◽  
P. Chazette ◽  
L. Menut ◽  
B. Bessagnet
Keyword(s):  
Optical Properties ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Dust Particles ◽  
Aerosol Size Distribution ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Coarse Mode ◽  
Paris Area ◽  
Flight Trajectories

Abstract. Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environments against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce the plume structure and location fairly well both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirm the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicates that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated by about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%), and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrates the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However, for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

scholarly journals On the competition among aerosol number, size and composition in predicting CCN variability: a multi-annual field study in an urbanized desert

2015 ◽  
Vol 15 (12) ◽  
pp. 6943-6958 ◽  
Author(s):  
E. Crosbie ◽  
J.-S. Youn ◽  
B. Balch ◽  
A. Wonaschütz ◽  
T. Shingler ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Size Distribution ◽  
North American ◽  
Monsoon Season ◽  
Aerosol Size Distribution ◽  
North American Monsoon ◽  
Aerosol Composition ◽  
Data Set ◽  
The North ◽  
Concentration Changes

Abstract. A 2-year data set of measured CCN (cloud condensation nuclei) concentrations at 0.2 % supersaturation is combined with aerosol size distribution and aerosol composition data to probe the effects of aerosol number concentrations, size distribution and composition on CCN patterns. Data were collected over a period of 2 years (2012–2014) in central Tucson, Arizona: a significant urban area surrounded by a sparsely populated desert. Average CCN concentrations are typically lowest in spring (233 cm−3), highest in winter (430 cm−3) and have a secondary peak during the North American monsoon season (July to September; 372 cm−3). There is significant variability outside of seasonal patterns, with extreme concentrations (1 and 99 % levels) ranging from 56 to 1945 cm−3 as measured during the winter, the season with highest variability. Modeled CCN concentrations based on fixed chemical composition achieve better closure in winter, with size and number alone able to predict 82 % of the variance in CCN concentration. Changes in aerosol chemical composition are typically aligned with changes in size and aerosol number, such that hygroscopicity can be parameterized even though it is still variable. In summer, models based on fixed chemical composition explain at best only 41 % (pre-monsoon) and 36 % (monsoon) of the variance. This is attributed to the effects of secondary organic aerosol (SOA) production, the competition between new particle formation and condensational growth, the complex interaction of meteorology, regional and local emissions and multi-phase chemistry during the North American monsoon. Chemical composition is found to be an important factor for improving predictability in spring and on longer timescales in winter. Parameterized models typically exhibit improved predictive skill when there are strong relationships between CCN concentrations and the prevailing meteorology and dominant aerosol physicochemical processes, suggesting that similar findings could be possible in other locations with comparable climates and geography.

scholarly journals Aerosol chemical and optical properties over the Paris area within ESQUIF project

2006 ◽  
Vol 6 (1) ◽  
pp. 401-454 ◽  
Author(s):  
A. Hodzic ◽  
R. Vautard ◽  
P. Chazette ◽  
L. Menut ◽  
B. Bessagnet
Keyword(s):  
Optical Properties ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Dust Particles ◽  
Aerosol Size Distribution ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Coarse Mode ◽  
Paris Area ◽  
Flight Trajectories

Abstract. Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environment against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce fairly well the plume structure and location both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirmed the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicated that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated of about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%) and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrated the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

scholarly journals Constructing a data-driven receptor model for organic and inorganic aerosol – a synthesis analysis of eight mass spectrometric data sets from a boreal forest site

2019 ◽  
Vol 19 (6) ◽  
pp. 3645-3672 ◽  
Author(s):  
Mikko Äijälä ◽  
Kaspar R. Daellenbach ◽  
Francesco Canonaco ◽  
Liine Heikkinen ◽  
Heikki Junninen ◽  
...  
Keyword(s):  
Boreal Forest ◽  
Organic Aerosol ◽  
Mass Spectrometric ◽  
Chemical Components ◽  
Forest Site ◽  
Aerosol Composition ◽  
Mass Spectrometric Data ◽  
Spectrometric Data ◽  
Aerosol Mass ◽  
Inorganic Aerosol

Abstract. The interactions between organic and inorganic aerosol chemical components are integral to understanding and modelling climate and health-relevant aerosol physicochemical properties, such as volatility, hygroscopicity, light scattering and toxicity. This study presents a synthesis analysis for eight data sets, of non-refractory aerosol composition, measured at a boreal forest site. The measurements, performed with an aerosol mass spectrometer, cover in total around 9 months over the course of 3 years. In our statistical analysis, we use the complete organic and inorganic unit-resolution mass spectra, as opposed to the more common approach of only including the organic fraction. The analysis is based on iterative, combined use of (1) data reduction, (2) classification and (3) scaling tools, producing a data-driven chemical mass balance type of model capable of describing site-specific aerosol composition. The receptor model we constructed was able to explain 83±8 % of variation in data, which increased to 96±3 % when signals from low signal-to-noise variables were not considered. The resulting interpretation of an extensive set of aerosol mass spectrometric data infers seven distinct aerosol chemical components for a rural boreal forest site: ammonium sulfate (35±7 % of mass), low and semi-volatile oxidised organic aerosols (27±8 % and 12±7 %), biomass burning organic aerosol (11±7 %), a nitrate-containing organic aerosol type (7±2 %), ammonium nitrate (5±2 %), and hydrocarbon-like organic aerosol (3±1 %). Some of the additionally observed, rare outlier aerosol types likely emerge due to surface ionisation effects and likely represent amine compounds from an unknown source and alkaline metals from emissions of a nearby district heating plant. Compared to traditional, ion-balance-based inorganics apportionment schemes for aerosol mass spectrometer data, our statistics-based method provides an improved, more robust approach, yielding readily useful information for the modelling of submicron atmospheric aerosols physical and chemical properties. The results also shed light on the division between organic and inorganic aerosol types and dynamics of salt formation in aerosol. Equally importantly, the combined methodology exemplifies an iterative analysis, using consequent analysis steps by a combination of statistical methods. Such an approach offers new ways to home in on physicochemically sensible solutions with minimal need for a priori information or analyst interference. We therefore suggest that similar statistics-based approaches offer significant potential for un- or semi-supervised machine-learning applications in future analyses of aerosol mass spectrometric data.

A detailed investigation of ambient aerosol composition and size distribution in an urban atmosphere

2012 ◽  
Vol 20 (4) ◽  
pp. 2556-2568 ◽  
Author(s):  
S. Levent Kuzu ◽  
Arslan Saral ◽  
Selami Demir ◽  
Gülsüm Summak ◽  
Göksel Demir
Keyword(s):  
Size Distribution ◽  
Urban Atmosphere ◽  
Aerosol Composition ◽  
Ambient Aerosol

scholarly journals Modeling kinetic partitioning of secondary organic aerosol and size distribution dynamics: representing effects of volatility, phase state, and particle-phase reaction

2014 ◽  
Vol 14 (10) ◽  
pp. 5153-5181 ◽  
Author(s):  
R. A. Zaveri ◽  
R. C. Easter ◽  
J. E. Shilling ◽  
J. H. Seinfeld
Keyword(s):  
Size Distribution ◽  
Rate Constant ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Diffusion Reaction ◽  
Aerosol Size Distribution ◽  
Particle Phase ◽  
Distribution Dynamics ◽  
Bulk Diffusivity ◽  
New Framework

Abstract. This paper describes and evaluates a new framework for modeling kinetic gas-particle partitioning of secondary organic aerosol (SOA) that takes into account diffusion and chemical reaction within the particle phase. The framework uses a combination of (a) an analytical quasi-steady-state treatment for the diffusion–reaction process within the particle phase for fast-reacting organic solutes, and (b) a two-film theory approach for slow- and nonreacting solutes. The framework is amenable for use in regional and global atmospheric models, although it currently awaits specification of the various gas- and particle-phase chemistries and the related physicochemical properties that are important for SOA formation. Here, the new framework is implemented in the computationally efficient Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) to investigate the competitive growth dynamics of the Aitken and accumulation mode particles. Results show that the timescale of SOA partitioning and the associated size distribution dynamics depend on the complex interplay between organic solute volatility, particle-phase bulk diffusivity, and particle-phase reactivity (as exemplified by a pseudo-first-order reaction rate constant), each of which can vary over several orders of magnitude. In general, the timescale of SOA partitioning increases with increase in volatility and decrease in bulk diffusivity and rate constant. At the same time, the shape of the aerosol size distribution displays appreciable narrowing with decrease in volatility and bulk diffusivity and increase in rate constant. A proper representation of these physicochemical processes and parameters is needed in the next generation models to reliably predict not only the total SOA mass, but also its composition- and number-diameter distributions, all of which together determine the overall optical and cloud-nucleating properties.

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