Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies

Ervens, B.; Turpin, Barbara J.; Weber, R. J.

doi:10.5194/acp-11-11069-2011

Cited by 1,187 publications

(1,359 citation statements)

References 268 publications

(335 reference statements)

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“…[13,21] (SOA gas is not as oxidised as measured atmospheric aerosol.) SOA aq and SOA gas form from different precursors under different atmospheric conditions and have different properties and behaviour.…”

Section: Introductionmentioning

confidence: 99%

“…[1][2][3][4][5][6][7][8][9][10][11] As a result, gas-phase followed by aqueous-phase chemistry contributes to secondary organic aerosol (SOA). [12,13] SOA is also formed when semiand low-volatility products of gas-phase chemistry sorb to particulate organic matter [14,15] (here SOA gas is used to denote SOA formed by this latter pathway and SOA aq to denote SOA formed with a contribution from aqueous-phase chemistry).…”

Section: Introductionmentioning

confidence: 99%

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Glyoxal secondary organic aerosol chemistry: effects of dilute nitrate and ammonium and support for organic radical–radical oligomer formation

Kirkland¹,

Lim²,

Tan³

et al. 2013

Environ. Chem.

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Environmental context. Atmospheric waters (clouds, fogs and wet aerosols) are media in which gases can be converted into particulate matter. This work explores aqueous transformations of glyoxal, a water-soluble gas with anthropogenic and biogenic sources. Results provide new evidence in support of previously proposed chemical mechanisms. These mechanisms are beginning to be incorporated into transport models that link emissions to air pollution concentrations and behaviour.Abstract. Glyoxal (GLY) is ubiquitous in the atmosphere and an important aqueous secondary organic aerosol (SOA) precursor. At dilute (cloud-relevant) organic concentrations, OH radical oxidation of GLY has been shown to produce oxalate. GLY has also been used as a surrogate species to gain insight into radical and non-radical reactions in wet aerosols, where organic and inorganic concentrations are very high (in the molar region). The work herein demonstrates, for the first time, that tartarate forms from GLY þ OH . Tartarate is a key product in a previously proposed organic radical-radical reaction mechanism for oligomer formation from GLY oxidation. Previously published model predictions that include this GLY oxidation pathway suggest that oligomers are major products of OH radical oxidation at the high organic concentrations found in wet aerosols. The tartarate measurements herein provide support for this proposed oligomer formation mechanism. This paper also demonstrates, for the first time, that dilute (cloud or fog-relevant) concentrations of inorganic nitrogen (i.e. ammonium and nitrate) have little effect on the GLY þ OH chemistry leading to oxalate formation in clouds. This, and results from previous experiments conducted with acidic sulfate, increase confidence that the currently understood dilute GLY þ OH chemistry can be used to predict GLY SOA formation in clouds and fogs. It should be recognised that organic-inorganic interactions can play an important role in droplet evaporation chemistry and in wet aerosols. The chemistry leading to SOA formation in these environments is complex and remains poorly understood.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Glyoxal secondary organic aerosol chemistry: effects of dilute nitrate and ammonium and support for organic radical–radical oligomer formation

Kirkland¹,

Lim²,

Tan³

et al. 2013

Environ. Chem.

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“…There is an intrinsic complexity of the atmospheric aerosols with regard to hygroscopicity, given the large differences in particle sizes, varying from nanometer to micrometer, and the varying chemical components in different size modes. Water content is found to be a key factor in determining total ambient particulate matter (PM) mass concentration, causing an impact on light scattering and extinction coefficient (Day and Malm, 2001;Garland et al, 2007;Jung et al, 2009), and has profound implications for atmospheric chemistry as it can enhance chemical reaction rates on the aerosol (Ervens et al, 2011;Lee et al, 2011;Wang et al, 2012).…”

Section: Introductionmentioning

confidence: 99%

Continuous Measurement of Ambient Aerosol Liquid Water Content in Beijing

Fajardo

Jiang

Hao

2016

Aerosol Air Qual. Res.

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The amount of liquid water present on ambient aerosol particles influences its radiative properties, the partitioning of gas-phase organic and inorganic compounds to the condensed phase, and the assessment of particle health effects upon inhalation. An improved home-made Dry-Ambient Aerosol Size Spectrometer (DAASS) was implemented and deployed at a sampling site in Beijing to measure water content and volumetric growth factor of fine ambient aerosol during clean and polluted days. Aerosol chemical composition was characterized by an aerosol chemical speciation monitor (ACSM). Meteorological conditions were also assessed to trace origin of the air masses arriving at the site. A thermodynamic model, ISORROPIA II, was used to predict aerosol water content based on inorganic compositions measured by ACSM. It was then compared with the aerosol water content measured by DAASS. During the two-week sampling period, an aerosol efflorescence behavior was observed around 50% relative humidity (RH). Aerosol at the sample location was predominantly alkaline, with an average acidity ratio of 1.3 during the polluted days but very variable during the clean days. This fact coupled with generally low ambient RH resulted in low amounts of liquid water detected during the campaign. When RH reached its maximum of 87% and aerosol appeared to be more acidic, the maximum amount of aerosol water content measured was 1.3 µg m -3 (44.9% wt of DAASS measured ambient aerosol). Measured aerosol water content and model predictions seem to show a better agreement during the more polluted days, but during the clean days aerosol organic fraction appears to have an important contribution in the water content. We argue that the organicassociated water is comparable with that associated with inorganic compositions during the clean periods at low ambient RH conditions.

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“…A number of studies indicate that ambient SOA concentrations are underpredicted within models, often substantially so, when these traditional parameterizations are used (e.g., 5,6). Some of this bias has been attributed to missing SOA precursors in emissions inventories, such as so-called intermediate volatility organic compounds, to ambient photochemical aging of semivolatile compounds occurring beyond that in chamber experiments (7) or to aerosol water/cloud processing (8). The addition of a more complete spectrum of SOA precursors into models has not, however, closed the measurement/prediction gap robustly.…”

mentioning

confidence: 99%

Influence of vapor wall loss in laboratory chambers on yields of secondary organic aerosol

Zhang

Cappa

Jathar

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

454

619

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Secondary organic aerosol (SOA) constitutes a major fraction of submicrometer atmospheric particulate matter. Quantitative simulation of SOA within air-quality and climate models-and its resulting impacts-depends on the translation of SOA formation observed in laboratory chambers into robust parameterizations. Worldwide data have been accumulating indicating that model predictions of SOA are substantially lower than ambient observations. Although possible explanations for this mismatch have been advanced, none has addressed the laboratory chamber data themselves. Losses of particles to the walls of chambers are routinely accounted for, but there has been little evaluation of the effects on SOA formation of losses of semivolatile vapors to chamber walls. Here, we experimentally demonstrate that such vapor losses can lead to substantially underestimated SOA formation, by factors as much as 4. Accounting for such losses has the clear potential to bring model predictions and observations of organic aerosol levels into much closer agreement.M ost of the understanding concerning the formation of secondary organic aerosol (SOA) from atmospheric oxidation of volatile organic compounds (VOCs) over the past 30 y has been developed from data obtained in laboratory chambers (1). SOA is a major component of particulate matter smaller than 1 μm (2) and consequently has important impacts on regional and global climate and human health and welfare. Accurate simulation of SOA formation and abundance within 3D models is critical to quantifying its atmospheric impacts. Measurements of SOA formation in laboratory chambers provide the basis for the parameterizations of SOA formation (3) in regional air-quality models and global climate models (4). A number of studies indicate that ambient SOA concentrations are underpredicted within models, often substantially so, when these traditional parameterizations are used (e.g., 5, 6). Some of this bias has been attributed to missing SOA precursors in emissions inventories, such as so-called intermediate volatility organic compounds, to ambient photochemical aging of semivolatile compounds occurring beyond that in chamber experiments (7) or to aerosol water/cloud processing (8). The addition of a more complete spectrum of SOA precursors into models has not, however, closed the measurement/prediction gap robustly. For example, recent analysis of organic aerosol (OA) concentrations in Los Angeles revealed that observed OA levels, which are dominated by SOA, exceed substantially those predicted by current atmospheric models (9), in accord with earlier findings in Mexico City (10).Here, we demonstrate that losses of SOA-forming vapors to chamber walls during photooxidation experiments can lead to substantial and systematic underestimation of SOA. Recent experiments have demonstrated that losses of organic vapors to the typically Teflon walls of a laboratory chamber can be substantial (11), but the effects on SOA formation have not yet been quantitatively established. In essence, the walls serve ...

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Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies

Cited by 1,187 publications

References 268 publications

Glyoxal secondary organic aerosol chemistry: effects of dilute nitrate and ammonium and support for organic radical–radical oligomer formation

Glyoxal secondary organic aerosol chemistry: effects of dilute nitrate and ammonium and support for organic radical–radical oligomer formation

Continuous Measurement of Ambient Aerosol Liquid Water Content in Beijing

Influence of vapor wall loss in laboratory chambers on yields of secondary organic aerosol

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