Anionic, Cationic, and Nonionic Surfactants in Atmospheric Aerosols from the Baltic Coast at Askö, Sweden: Implications for Cloud Droplet Activation

Gerard, V. B.; Nozière, Barbara; Baduel, Christine; Fine, L.; Frossard, A. A.; Cohen, R. C.

doi:10.1021/acs.est.5b05809

Cited by 74 publications

(128 citation statements)

References 39 publications

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“…Aerosol chemical composition measurements challenge the assumption that the surface tension of activating particles is equal to that of water. Organic aerosols contain surface active molecules in sufficient abundance to reduce the surface tension of macroscopic solutions (4,7,8), and these abundances could, in principle, be sufficient to maintain a reduced surface tension throughout activation (7)(8)(9)(10)(11). Such a reduction could increase CCN concentrations by an order of magnitude (12).…”

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confidence: 99%

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The surface tension of surfactant-containing, finite volume droplets

Bzdek

Reid

Malila

et al. 2020

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

119

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Surface tension influences the fraction of atmospheric particles that become cloud droplets. Although surfactants are an important component of aerosol mass, the surface tension of activating aerosol particles is still unresolved, with most climate models assuming activating particles have a surface tension equal to that of water. By studying picoliter droplet coalescence, we demonstrate that surfactants can significantly reduce the surface tension of finite-sized droplets below the value for water, consistent with recent field measurements. Significantly, this surface tension reduction is droplet size-dependent and does not correspond exactly to the macroscopic solution value. A fully independent monolayer partitioning model confirms the observed finite-size-dependent surface tension arises from the high surface-to-volume ratio in finite-sized droplets and enables predictions of aerosol hygroscopic growth. This model, constrained by the laboratory measurements, is consistent with a reduction in critical supersaturation for activation, potentially substantially increasing cloud droplet number concentration and modifying radiative cooling relative to current estimates assuming a water surface tension. The results highlight the need for improved constraints on the identities, properties, and concentrations of atmospheric aerosol surfactants in multiple environments and are broadly applicable to any discipline where finite volume effects are operative, such as studies of the competition between reaction rates within the bulk and at the surface of confined volumes and explorations of the influence of surfactants on dried particle morphology from spray driers.

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confidence: 99%

“…Most approaches infer surface tension from hygroscopic growth or critical supersaturation measurements (28). Moreover, many studies report only macroscopic solution surface tension measurements and do not consider surfacebulk partitioning effects (4,7,8,16,29). Consequently, predictions of surfactant partitioning in aerosol are not accompanied by direct…”

mentioning

confidence: 99%

The surface tension of surfactant-containing, finite volume droplets

Bzdek

Reid

Malila

et al. 2020

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

119

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“…For instance, a notable amount of organic matter (up to 60 % of the total mass) was detected with a compact time-of-flight aerosol mass spectrometer in the CCN measured at the PUY station . Paying more attention to the effect of surfactants on cloud droplet formation follows the global interest that emerged in the literature (McNeill et al, 2013), with a multiplicity of laboratory and field studies as well as global modeling studies (Prisle et al, 2012) dedicated to this research area (Gérard et al, 2016;Nozière et al, 2014).…”

Section: Activation Of Aerosol Particles Into Cloud Dropletsmentioning

confidence: 99%

Modeling the partitioning of organic chemical species in cloud phases with CLEPS (1.1)

Chaumerliac¹,

Deguillaume²,

Perroux³

et al. 2018

Atmos. Chem. Phys.

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Abstract. The new detailed aqueous-phase mechanism Cloud Explicit Physico-chemical Scheme (CLEPS 1.0), which describes the oxidation of isoprene-derived watersoluble organic compounds, is coupled with a warm microphysical module simulating the activation of aerosol particles into cloud droplets. CLEPS 1.0 was then extended to CLEPS 1.1 to include the chemistry of the newly added dicarboxylic acids dissolved from the particulate phase. The resulting coupled model allows the prediction of the aqueousphase concentrations of chemical compounds originating from particle scavenging, mass transfer from the gas-phase and in-cloud aqueous chemical reactivity. The aim of the present study was more particularly to investigate the effect of particle scavenging on cloud chemistry. Several simulations were performed to assess the influence of various parameters on model predictions and to interpret long-term measurements conducted at the top of Puy de Dôme (PUY, France) in marine air masses. Specific attention was paid to carboxylic acids, whose predicted concentrations are on average in the lower range of the observations, with the exception of formic acid, which is rather overestimated in the model. The different sensitivity runs highlight the fact that formic and acetic acids mainly originate from the gas phase and have highly variable aqueous-phase reactivity depending on the cloud acidity, whereas C 3 -C 4 carboxylic acids mainly originate from the particulate phase and are supersaturated in the cloud.

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“…The parameterizations provided in these studies differ by the aerosol size distribution they use and the way they treat the activation process. They have been discussed by Simpson et al (2014) to demonstrate the effect of activating large particles described by a single lognormal mode simulation and by Ghan et al (2011), who concluded that all parameterizations performed well under the most common conditions, i.e., when CCN are mainly in the accumulation mode.…”

Section: Activation Of Aerosol Particles Into Cloud Dropletsmentioning

confidence: 99%

Modeling the partitioning of organic chemical species in cloud phases with CLEPS (1.1)

Chaumerliac¹,

Deguillaume²,

Perroux³

et al. 2017

Preprint

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The new detailed aqueous-phase mechanism Cloud Explicit Physico-chemical Scheme (CLEPS 1.0), which describes the oxidation of isoprene-derived watersoluble organic compounds, is coupled with a warm microphysical module simulating the activation of aerosol particles into cloud droplets. CLEPS 1.0 was then extended to CLEPS 1.1 to include the chemistry of the newly added dicarboxylic acids dissolved from the particulate phase. The resulting coupled model allows the prediction of the aqueousphase concentrations of chemical compounds originating from particle scavenging, mass transfer from the gas-phase and in-cloud aqueous chemical reactivity. The aim of the present study was more particularly to investigate the effect of particle scavenging on cloud chemistry. Several simulations were performed to assess the influence of various parameters on model predictions and to interpret long-term measurements conducted at the top of Puy de Dôme (PUY, France) in marine air masses. Specific attention was paid to carboxylic acids, whose predicted concentrations are on average in the lower range of the observations, with the exception of formic acid, which is rather overestimated in the model. The different sensitivity runs highlight the fact that formic and acetic acids mainly originate from the gas phase and have highly variable aqueous-phase reactivity depending on the cloud acidity, whereas C 3 -C 4 carboxylic acids mainly originate from the particulate phase and are supersaturated in the cloud.Published by Copernicus Publications on behalf of the European Geosciences Union.

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Anionic, Cationic, and Nonionic Surfactants in Atmospheric Aerosols from the Baltic Coast at Askö, Sweden: Implications for Cloud Droplet Activation

Cited by 74 publications

References 39 publications

The surface tension of surfactant-containing, finite volume droplets

The surface tension of surfactant-containing, finite volume droplets

Modeling the partitioning of organic chemical species in cloud phases with CLEPS (1.1)

Modeling the partitioning of organic chemical species in cloud phases with CLEPS (1.1)

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