A model for particle formation and growth in the atmosphere with molecular resolution in size

Lehtinen, K. E. J.; Kulmala, M.

doi:10.5194/acpd-2-1791-2002

Cited by 46 publications

(54 citation statements)

References 18 publications

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“…Particle formation events have been observed in 22% of the BEWA field experiment days indicating that nucleation and subsequent growth of particles may be considered a frequent phenomenon in the atmospheric boundary layer. Also, the particle growth dynamics are consistent with earlier studies supporting the assumption of a general nucleation mechanism which may be modeled to gain deeper insight into particle nucleation and growth dynamics [e.g., Lehtinen and Kulmala , 2003].…”

Section: Discussionmentioning

confidence: 99%

Observations of particle formation and growth in a mountainous forest region in central Europe

et al. 2004

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In the summers of 2001 and 2002, particle formation and growth were observed at a forest ecosystem research site in the “Fichtelgebirge” mountain range in NE Bavaria, Germany. Atmospheric nucleation events, identified through detailed analysis of the time evolution of submicron particle size distributions, differed considerably from nonevent days with respect to ultrafine particle concentrations and meteorological parameters. Particle diameter growth rates, as quantified through the geometric mean diameter development of the 3–60 nm particle fraction, ranged from 2.2 to 5.7 nm h−1. While H2SO4 concentrations typically explained less than 10% of the observed growth rates, a significant fraction of particle growth may be explained through condensation of organic vapors from α‐pinene oxidation. On several days, cocondensation of H2SO4 and α‐pinene oxidation products was sufficient to fully explain the observed growth dynamics. While BVOC emissions from the tree vegetation may contribute to particle formation, the forest also acts as an effective sink for particles. This is reflected in the dominance of particle deposition to the forest over emission, with the strongest deposition fluxes occurring during particle formation events.

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Section: Discussionmentioning

confidence: 99%

Observations of particle formation and growth in a mountainous forest region in central Europe

et al. 2004

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“…Thus, we assume any collision to result in a reactive attachment of sulfuric acid. The collision rate coefficient k coll , i , j itself can be formulated as [ Friedlander , 2000; Lehtinen and Kulmala , 2003] where D p , i / j are the diameters and = the thermal speeds of the colliding molecules i and j , and M i / j corresponds to the molecular mass. In the formulas above, the subscript j refers to sulfuric acid.…”

Section: Nucleation Rate At Molecular Levelmentioning

confidence: 99%

How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation

et al. 2008

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[1] New particle formation has been observed to take place all around the world. However, because of the inability to determine the chemical composition of the smallest clusters or particles, indirect tools such as the correlation between nucleation rate and measured sulfuric acid concentrations have been used to infer the nucleation mechanism. In this study we describe the observed correlation with gaseous sulfuric acid concentrations by interactions of sesquiterpene oxidation products with sulfuric acid. Two formation pathways of nucleation initiating molecules are considered. The interaction of sulfuric acid with organic sulfates, which are formed from stabilized Criegee intermediates (sCIs, formed from sesquiterpenes), can be used to explain the observed squared relationship between particle formation rate and ambient sulfuric acid concentrations. The corresponding linear dependence is explained with the participation of secondary ozonides, which are formed from sCIs and aldehydes. Both pathways are negatively affected by increasing water vapor concentration as observed in recent studies. In order to check the assumptions made we apply the derived nucleation coefficients to measurements of the BACCI/QUEST IV campaign made during spring 2005 in Hyytiälä, Finland. A reasonable agreement between the measurement data and the predicted nucleation rates is found, giving support for the presented nucleation description.Citation: Bonn, B., M. Kulmala, I. Riipinen, S.-L. Sihto, and T. M. Ruuskanen (2008), How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation,

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“…The formation and growth of nucleation mode particles being our main focus, we chose as our reference such an approximation: a model that describes particles smaller than 10 nm in diameter molecule by molecule [ Lehtinen and Kulmala , 2002]. In this region, the approach is free of discretization errors and mimics the dynamics of newly formed particles in great detail.…”

Section: Representation Of Particle Size Distributionmentioning

confidence: 99%

Simulation of atmospheric nucleation mode: A comparison of nucleation models and size distribution representations

Korhonen¹

2003

J. Geophys. Res.

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[1] Atmospheric particle formation and growth were investigated using different nucleation models and size distribution representations. Nucleation was modeled using recently developed parameterizations for binary nucleation of water and sulphuric acid and ternary nucleation of water, sulphuric acid, and ammonia. A comparison with older nucleation parameterizations, combined with full aerosol dynamics, demonstrated that the difference in nucleation rate (1-2 orders of magnitude) is clearly reflected in the resulting total particle concentration. A comparison of binary and ternary nucleation schemes showed that above 240 K the ternary nucleation rate exceeds the binary by over 10 orders of magnitude, indicating that in most cases, at lower tropospheric conditions, only ternary nucleation can be relevant. In addition, the performance of aerosol dynamics models applying either a multimodal monodisperse or a fixed sectional size distribution representation was evaluated against a molecular resolution model, which follows the changes in the nucleation mode particle size distribution molecule by molecule. Regarding total number concentration, the sectional method converged to the molecular resolution approach when increasing the number of size sections. With strong condensational growth, however, numerical diffusion problems were evident. Overall, the performance of the sectional method with low number of sections was not satisfactory. The monodisperse method gave very good results, at least in terms of total number, when the background modes were set to match the condensation sinks of respective lognormal modes. On the basis of our study the multimodal monodisperse method seems to be a possible candidate when selecting the size distribution approach for large-scale atmospheric models.

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A model for particle formation and growth in the atmosphere with molecular resolution in size

Cited by 46 publications

References 18 publications

Observations of particle formation and growth in a mountainous forest region in central Europe

Observations of particle formation and growth in a mountainous forest region in central Europe

How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation

Simulation of atmospheric nucleation mode: A comparison of nucleation models and size distribution representations

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