Comment on ‘‘Self-nucleation in the sulfuric acid–water system’’

Renninger, R.G.; Hiller, F. Charles; Bone, Roger C.

doi:10.1063/1.442201

Cited by 56 publications

(24 citation statements)

References 6 publications

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“…However, it has been found that the composition of cluster surface layer may differ significantly from the bulk due to surface enrichment or adsorption [ Wilemski , 1987; Mirabel and Reiss , 1987; Laaksonen et al , 1999]. In the case, when the surface and bulk (or interior) molecules in the cluster are distinguished, the surface derivative term in is eliminated by using the Gibbs adsorption isotherm that leads to the following revised Kevin equations for the binary mixture [ Renninger et al , 1981] …”

Section: A Kinetic Model Of H2so4‐h2o Quasi‐unary Nucleationmentioning

confidence: 99%

Binary H₂SO₄‐H₂O homogeneous nucleation based on kinetic quasi‐unary nucleation model: Look‐up tables

2006

J. Geophys. Res.

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[1] Recently, we have shown that the binary homogeneous nucleation (BHN) of H 2 SO 4 and H 2 O can be treated as a quasi-unary nucleation (QUN) of H 2 SO 4 in the equilibrium with H 2 O vapor and have developed a kinetic H 2 SO 4 -H 2 O nucleation model, which simulates the dynamic evolutions of cluster distributions explicitly. In this paper we present improved and updated version of the QUN model, which has been modified through the incorporation of more rigorous thermodynamics of the cluster formation and the effect of the surface area of preexisting particles on nucleation rates. The difference in the model predictions of the improved and original QUN models is not dramatic; however, the improved QUN model is more consistent thermodynamically. The predicted BHN rates based on the QUN model are in good agreement with existing observations within the range of uncertainties. We also study the dependence of kinetic BHN rates on key input parameters and discuss the conditions in which the H 2 SO 4 -H 2 O homogeneous nucleation in the atmosphere may become significant. The nucleation rates look-up tables derived from the QUN model, which can be readily used to find the nucleation rates at given conditions, are presented. The look-up tables cover a wide range of key parameters that can be found in the ambient atmosphere, in the laboratory studies, and in the exhaust plumes. These look-up tables can be easily incorporated in multidimensional models to predict BHN rates, and they can be utilized directly for the analysis and interpretation of the observed nucleation events.

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Section: A Kinetic Model Of H2so4‐h2o Quasi‐unary Nucleationmentioning

confidence: 99%

Binary H₂SO₄‐H₂O homogeneous nucleation based on kinetic quasi‐unary nucleation model: Look‐up tables

2006

J. Geophys. Res.

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“…Furthermore, the classical binary nucleation rate depends exponentially on σ 3 , where σ is the composition dependent binary liquid surface tension for the critical cluster. 2,4,[26][27][28][29][30][31][32][33][34][35] A 10% error in σ can affect the nucleation rate by as much as 8 orders of magnitude. In many systems of interest, the critical cluster size is of the order of 10-100 molecules, making the use of bulk surface tension suspect.…”

Section: Introductionmentioning

confidence: 99%

Monte Carlo Simulations of Small Sulfuric Acid−Water Clusters

Kathmann

Hale

2001

J. Phys. Chem. B

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Effective atom-atom potentials are developed for binary sulfuric acid-water clusters and applied in a Bennett Metropolis Monte Carlo calculation to determine free energy differences for small neighboring sized clusters of fixed composition at 298 K. The atom-atom pair potentials consist of Lennard-Jones short-range and Coulombic long-range terms and assume rigid SO 4 2δ-with two unconstrained H δ+ and rigid H 2 O molecules interacting via revised central force (RSL2) potentials. The potential parameters are determined from both ab initio studies and tests of the potential using the statistical mechanical formalism for binary cluster size distributions. In the potential tests, fixed composition free energy differences, δf km,m , for [H 2 O] km [H 2 SO 4 ] m clusters are plotted versus (km + m) -1/3 , and the resulting slope and intercept (in the large cluster regime) are used to extract model dependent binary liquid surface tension and partial vapor pressures at 298 K. The potential parameters are adjusted to obtain approximate agreement with experimental surface tension and partial vapor pressures for k ) 1 and 4 (84% and 57% weight percent H 2 SO 4 , respectively). The free energy differences for m e 15 are presented, together with internal cluster energy contributions, snapshots of cluster structure, and evidence for onset of the large cluster regime near m ) 5. The long-range goals have been to test the free energy difference procedure for studying binary cluster properties and to develop model potentials appropriate for the simulation of small binary clusters at low temperatures characteristic of stratospheric sulfuric acid-water aerosols.

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“…For instance, Reiss assumed the surface tension to be independent of composition [14], while Doyle extended CNT by taking into account a surface tension that depends on the cluster composition [17]. However, more than 20 years later, it was shown by Renninger [18], Wilemski [19,20], and Reiss [21] that Doyle's derivation leads to thermodynamic inconsistencies. A revised thermodynamically consistent classical binary nucleation theory was developed by Wilemski in which the composition of the surface layer and the interior of the cluster could vary independently [19,20].…”

Section: Pacs Numbersmentioning

confidence: 99%

Crystal nucleation in binary hard-sphere mixtures: the effect of order parameter on the cluster composition

Smallenburg

Filion

et al. 2011

Molecular Physics

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Comment on ‘‘Self-nucleation in the sulfuric acid–water system’’

Cited by 56 publications

References 6 publications

Binary H₂SO₄‐H₂O homogeneous nucleation based on kinetic quasi‐unary nucleation model: Look‐up tables

Binary H₂SO₄‐H₂O homogeneous nucleation based on kinetic quasi‐unary nucleation model: Look‐up tables

Monte Carlo Simulations of Small Sulfuric Acid−Water Clusters

Crystal nucleation in binary hard-sphere mixtures: the effect of order parameter on the cluster composition

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Comment on ‘‘Self-nucleation in the sulfuric acid–water system’’

Cited by 56 publications

References 6 publications

Binary H2SO4‐H2O homogeneous nucleation based on kinetic quasi‐unary nucleation model: Look‐up tables

Binary H2SO4‐H2O homogeneous nucleation based on kinetic quasi‐unary nucleation model: Look‐up tables

Monte Carlo Simulations of Small Sulfuric Acid−Water Clusters

Crystal nucleation in binary hard-sphere mixtures: the effect of order parameter on the cluster composition

Contact Info

Product

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Binary H₂SO₄‐H₂O homogeneous nucleation based on kinetic quasi‐unary nucleation model: Look‐up tables

Binary H₂SO₄‐H₂O homogeneous nucleation based on kinetic quasi‐unary nucleation model: Look‐up tables