Soluble-Insoluble Transition in Binary Heterogeneous Nucleation

Petersen, D.; Ortner, Rosemarie; Vrtala, Aron; Pe, Wagner; Kulmala, Markku; Laaksonen, A.

doi:10.1103/physrevlett.87.225703

Cited by 19 publications

(24 citation statements)

References 10 publications

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“…This heterogeneous nucleation process is energetically more probable than homogeneous nucleation but less probable than activation (Petersen et al, 2001;Kulmala et al, 2000b). If the particles would be "activated" with the heterogeneous nucleation process, followed by condensational growth, the observed growth rates as a function of size would lie between those corresponding to condensation of nucleating vapours and those following nano-Köhler theory.…”

Section: Growth By Other Vapoursmentioning

confidence: 99%

Initial steps of aerosol growth

et al. 2004

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Abstract. The formation and growth of atmospheric aerosols depend on several steps, namely nucleation, initial steps of growth and subsequent -mainly condensational -growth. This work focuses on the initial steps of growth, meaning the growth right after nucleation, where the interplay of curvature effects and thermodynamics has a significant role on the growth kinetics. More specifically, we investigate how ion clusters and aerosol particles grow from 1.5 nm to 20 nm (diameter) in atmospheric conditions using experimental data obtained by air ion and aerosol spectrometers. The measurements have been performed at a boreal forest site in Finland. The observed trend that the growth rate seems to increase as a function of size can be used to investigate possible growth mechanisms. Such a growth rate is consistent with a recently suggested nano-Köhler mechanism, in which growth is activated at a certain size with respect to condensation of organic vapors. The results also imply that charge-enhanced growth associated with ion-mediated nucleation plays only a minor role in the initial steps of growth, since it would imply a clear decrease of the growth rate with size. Finally, further evidence was obtained on the earlier suggestion that atmospheric nucleation and the subsequent growth of fresh nuclei are likely to be uncoupled phenomena via different participating vapors.

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Section: Growth By Other Vapoursmentioning

confidence: 99%

Initial steps of aerosol growth

et al. 2004

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“…Simultaneous solution of the above-presented equilibrium equations requires that the values of the activity coefficients γ os and γ wat as well as the surface tension are estimated. To this end, we have applied a thermodynamic model that makes possible to treat a multi-component system as a pseudobinary one (Petersen et al, 2001). In this case the ionic salt and associated water form together one component and the organic compound forms the second component.…”

Section: Approachmentioning

confidence: 99%

Modelling the formation of organic particles in the atmosphere

Anttila¹,

Kerminen²,

Kulmala³

et al. 2003

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Abstract. A modelling study investigating the formation of organic particles from inorganic, thermodynamically stable clusters was carried out. A recently-developed theory, the so-called nano-Köhler theory, which describes a thermodynamic equilibrium between a nanometer-size cluster, water and water-soluble organic compound, was implemented in a dynamical model along with a treatment of the appropriate aerosol and gas-phase processes. The obtained results suggest that both gaseous sulphuric acid and organic vapours contribute to organic particle formation. The initial growth of freshly-nucleated clusters having a diameter around 1 nm is driven by condensation of gaseous sulphuric acid and by a lesser extent cluster self-coagulation. After the clusters have reached sizes of around 2 nm in diameter, low-volatile organic vapours start to condense spontaneously into the clusters, thereby accelerating their growth to detectable sizes. A shortage of gaseous sulphuric acid or organic vapours limit, or suppress altogether, the particle formation, since freshly-nucleated clusters are rapidly coagulated away by pre-existing particles. The obtained modelling results were applied to explaining the observed seasonal cycle in the number of aerosol formation events in a continental forest site.

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“…Here we apply a simplified, yet non-ideal thermodynamic model which can be readily implemented into aerosol dynamical models. We assume that that the multicomponent system behaves as a pseudobinary [Petersen et al, 2001], which permits us to treat solution as if it were consisting of two components only: the first one is the organic compound and the second one ammonium bisulphate in ionic form together with associated water. The pseudobinary activity coefficients are determined using Van Laar equations, and the activity coefficient of water is obtained by multiplying the pseudobinary activity coefficient, g pb , by that of water in a pure water-ammonium bisulphate solution [Tang and Munkelwitz, 1994].…”

Section: D04205mentioning

confidence: 99%

Organic aerosol formation via sulphate cluster activation

et al. 2004

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[1] The formation of aerosols, and subsequent cloud condensation nuclei, remains one of the least understood atmospheric processes upon which global climate change critically depends. Under atmospheric conditions, the process of homogeneous nucleation (formation of stable clusters $ 1 nm in size), and their subsequent growth into new particles (>3 nm), determines the aerosol and cloud nuclei population, yet, hitherto, no theory has elucidated the new particle formation phenomenon in detail. In this study, we present a new theory which provides a mechanistic explanation for new particle formation via activation of stable inorganic clusters by organic vapors. The new nano-particle activation theory is analogous to Köhler theory which describes cloud formation in a supersaturated water vapor field but differs in that it describes the activation of inorganic stable nano-clusters into aerosol particles in a supersaturated organic vapor which initiates spontaneous and rapid growth of clusters. Inclusion of the new theory into aerosol formation models predicts that increases in organic vapor densities lead to even greater increases in particle production, which, in turn, will influence the global radiative cooling effect of atmospheric aerosols.

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Soluble-Insoluble Transition in Binary Heterogeneous Nucleation

Cited by 19 publications

References 10 publications

Initial steps of aerosol growth

Initial steps of aerosol growth

Modelling the formation of organic particles in the atmosphere

Organic aerosol formation via sulphate cluster activation

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