Relationship between aerosol oxidation level and hygroscopic properties of laboratory generated secondary organic aerosol (SOA) particles

Massoli, P.; Lambe, Andrew T.; Ahern, Adam; Williams, Leah R.; Ehn, Mikael; Mikkilä, Jyri; Canagaratna, Manjula R.; Brune, William H.; Onasch, T. B.; Jayne, John T.; Petäj̈ä, Tuukka; Kulmala, Markku; Laaksonen, A.; Kolb, C. E.; Davidovits, P.; Worsnop, Douglas R.

doi:10.1029/2010gl045258

Cited by 299 publications

(422 citation statements)

References 74 publications

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“…To encompass the difficulty of representing the full molecular composition, the O : C of SOA has been included in global climate models to provide a description of the aerosol aging (Tost and Pringle, 2012). Furthermore, a number of recent studies have reported a positive correlation between hygroscopicity and bulk O : C for both laboratory and ambient SOA (Massoli et al, 2010;Jimenez et al, 2009;Chang et al, 2010;Duplissy et al, 2011).…”

Section: Methodsmentioning

confidence: 99%

Relating hygroscopicity and optical properties to chemical composition and structure of secondary organic aerosol particles generated from the ozonolysis of α-pinene

et al. 2015

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Abstract. Secondary organic aerosol (SOA) were generated from the ozonolysis of α-pinene in the CESAM (French acronym for Experimental Multiphasic Atmospheric Simulation Chamber) simulation chamber. The SOA formation and aging were studied by following their optical, hygroscopic and chemical properties. The optical properties were investigated by determining the particle complex refractive index (CRI). The hygroscopicity was quantified by measuring the effect of relative humidity (RH) on the particle size (size growth factor, GF) and on the scattering coefficient (scattering growth factor, f (RH)). The oxygen to carbon atomic ratios (O : C) of the particle surface and bulk were used as a sensitive parameter to correlate the changes in hygroscopic and optical properties of the SOA composition during their formation and aging in CESAM.The real CRI at 525 nm wavelength decreased from 1.43-1.60 (±0.02) to 1.32-1.38 (±0.02) during the SOA formation. The decrease in the real CRI correlated to the O : C decrease from 0.68 (±0.20) to 0.55 (±0.16). In contrast, the GF remained roughly constant over the reaction time, with values of 1.02-1.07 (±0.02) at 90 % (±4.2 %) RH. Simultaneous measurements of O : C of the particle surface revealed that the SOA was not composed of a homogeneous mixture, but contained less oxidised species at the surface which may limit water absorption. In addition, an apparent change in both mobility diameter and scattering coefficient with increasing RH from 0 to 30 % was observed for SOA after 14 h of reaction. We postulate that this change could be due to a change in the viscosity of the SOA from a predominantly glassy state to a predominantly liquid state.

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Section: Methodsmentioning

confidence: 99%

Relating hygroscopicity and optical properties to chemical composition and structure of secondary organic aerosol particles generated from the ozonolysis of α-pinene

et al. 2015

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“…however, that κ org has been observed to be higher in other studies, especially when the organic aerosol becomes more oxygenated that is when chemical aging has taken place(e.g., Chang et al, 2010;Massoli et al, 2010). At an O:C ratio of 0.2, i.e.…”

Section: Hygroscopicity Parameter Kappa (κ) and Ccn Closurementioning

confidence: 99%

“…CC BY 4.0 License. Duplissy et al, 2008;Frosch et al, 2011;Jimenez et al, 2009;Massoli et al, 2010;Wong et al, 2011). In addition, several studies have investigated the effect of organic surfactants.…”

Section: Introductionmentioning

confidence: 99%

What do we learn from long-term cloud condensation nuclei number concentration, particle number size distribution, and chemical composition measurements at regionally representative observatories?

Schmale

Henning

Decesari

et al. 2017

Preprint

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Abstract.Aerosol-cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Numerous observations of CCN number concentration exist, and many closure studies have been performed to predict CCN number concentrations based on particle number size 5 distributions, chemical composition, and the κ-Köhler theory. Most of these studies provide details for short time periods or focus on special environmental conditions. These observations, however, cannot address questions of large-scale temporal and spatial CCN variability. Here we analyze long-term observations of CCN number concentrations, particle number size distributions and chemical composition from twelve sites on three continents. Eight of these stations are part of the European Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS). 10We group the observatories into categories according to their official classification: coastal background (Barrow, Alaska; Mace Head, Ireland; Finokalia, Crete; Noto Peninsula, Japan), rural background (Melpitz, Germany; Cabauw, the Netherlands; Vavihill, Sweden), alpine sites (Puy de Dôme, France; Jungfraujoch, Switzerland), remote forest sites (ATTO, Brazil; SMEAR, Finland) and the urban environment (Seoul, South Korea). Expectedly, CCN characteristics are highly variable across regions. However, they also vary within categories, most strongly in the coastal background group, where 15 CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behavior, most continental stations exhibit very similar relative activation ratios across the range of 0.1 to 1.0 % supersaturation. At the coastal sites the activation ratios spread more widely across the SS spectrum.Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g., atBarrow (Arctic Haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), 20 the rain forest (wet and dry season), or Finokalia (forest fire influence in fall). The rural background and urban sites exhibit relatively little variability throughout the year while short-term variability can be high especially at the urban site.The average hygroscopicity parameter, κ, calculated from the chemical composition of submicron particles, was highest at the coastal site of Mace Head (0.6) and the lowest at the rain forest station ATTO (0.2 -0.3). We performed closure studies to predict CCN number concentrations from the particle number size distribution and chemical composition measurements. 25The prediction accuracy for the average concentrations is high. The ratio between predicted and measured CCN concentrations is between 0.87 and 1.4. The temporal variability is also well represented, as reflected by Pearson c...

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“…Understanding the gas-particle partitioning of atmospheric aerosol is necessary for effective OA modeling and prediction of the aerosol budget ). Furthermore, understanding the contribution of SOA to aerosol number and hygroscopicity is important for prediction of cloud condensation nuclei (CCN) (Kanakidou et al 2005;Roelofs 2008;Asa-Awuku et al 2009;Chang et al 2010;Massoli et al 2010;Engelhart et al 2011;Lambe et al 2011;Riipinen et al 2011;Gantt et al 2012).…”

Section: Introductionmentioning

confidence: 99%

Toward the Determination of Joint Volatility-Hygroscopicity Distributions: Development and Response Characterization for Single-Component Aerosol

Cerully

Hite

McLaughlin

et al. 2014

Aerosol Science and Technology

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This work presents the development and characterization of a thermodenuder for the study and interpretation of aerosol volatility. Thermodenuder measurements are further combined with a continuous-flow streamwise thermal gradient CCN counter to obtain the corresponding aerosol hygroscopicity. The thermodenuder response function is characterized with monodisperse aerosol of variable volatility and hygroscopicity. The measurements are then interpreted with a comprehensive instrument model embedded within an optimization framework to retrieve aerosol properties with constrained uncertainty. Special attention is given to the interpretation of the size distribution of the thermodenuded aerosol, deconvoluting the effects of impurities and multiple charging, and to simplifications on the treatment of thermodenuder geometry, temperature, the cooling section, and the effects of curvature and accommodation coefficient on inferred particle volatility. Retrieved vapor pressures are consistent with published literature and shown to be most sensitive to uncertainty in the accommodation coefficient.

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Relationship between aerosol oxidation level and hygroscopic properties of laboratory generated secondary organic aerosol (SOA) particles

Cited by 299 publications

References 74 publications

Relating hygroscopicity and optical properties to chemical composition and structure of secondary organic aerosol particles generated from the ozonolysis of α-pinene

Relating hygroscopicity and optical properties to chemical composition and structure of secondary organic aerosol particles generated from the ozonolysis of α-pinene

What do we learn from long-term cloud condensation nuclei number concentration, particle number size distribution, and chemical composition measurements at regionally representative observatories?

Toward the Determination of Joint Volatility-Hygroscopicity Distributions: Development and Response Characterization for Single-Component Aerosol

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