Enthalpy and entropy changes in formation of gas phase sulfnric acid monohydrates and dihydrates as a result of fitting to experimental pressure data

Noppel, Madis

doi:10.1029/2000jd900192

Cited by 12 publications

(9 citation statements)

References 26 publications

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“…[10] Here we will give only a brief overview of the classical nucleation theory. For a more detailed description the reader is referred to our earlier work Noppel et al, 2002] and references therein.…”

Section: Theory and Modelmentioning

confidence: 99%

“…where K i are the equilibrium constants for the successive additions of water molecules to an acid molecule. Their temperature dependent values are given by Noppel et al [2002]. The equilibrium constants are calculated at a reference vapor concentration r 0 = p 0 /(kT ) where the reference pressure p 0 is set to 1 atm, T is the temperature and k is the Boltzmann constant.…”

Section: Theory and Modelmentioning

confidence: 99%

“…We have recently investigated the homogeneous nucleation of sulfuric acid and water under atmospheric conditions using the most rigorous nucleation kinetics, the thermodynamically consistent version of the classical nucleation model and an improved model for the formation of sulfuric acid water hydrates [ Noppel et al , 2002]. This improved model for hydrate formation in sulfuric acid–water nucleation is based on ab initio calculations of small sulfuric acid clusters and on experimental data for vapor pressures and equilibrium constants [ Noppel et al , 2002; Noppel , 2000]. It was shown [ Noppel et al , 2002] that the nucleation rates derived with the revised theory are in most cases within the observational error.…”

Section: Introductionmentioning

confidence: 99%

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An improved parameterization for sulfuric acid–water nucleation rates for tropospheric and stratospheric conditions

et al. 2002

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[1] In this paper we present parameterized equations for calculation of sulfuric acidwater critical nucleus compositions, critical cluster radii and homogeneous nucleation rates for tropospheric and stratospheric conditions. The parameterizations are based on a classical nucleation model. We used an improved model for the hydrate formation relying on ab initio calculations of small sulfuric acid clusters and on experimental data for vapor pressures and equilibrium constants for hydrate formation. The most rigorous nucleation kinetics and the thermodynamically consistent version of the classical binary homogeneous nucleation theory were used. The parameterized nucleation rates are compared with experimental ones, and at room temperature and relative humidities above 30% they are within experimental error. At lower temperatures and lower humidities the agreement is somewhat poorer. Overall, the values of nucleation rates are increased compared to a previous parameterization and are within an order of magnitude compared with theoretical values for all conditions studied. The parameterized equations will reduce the computing time by a factor 1/500 compared to nonparameterized nucleation rate calculations and therefore are in particular useful for large-scale models. The parameterized formulas are valid at temperatures between 230.15 K and 305.15 K, relative humidities between 0.01% and 100%, and sulfuric acid concentrations from 10 4 to 10 11 cm À3 . They can be used to extrapolate the classical results down to 190 K. The parametrization is limited to cases where nucleation rates are between 10 À7 and 10 10 cm À3 s À1, and the critical cluster contains at least four molecules.INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 1610 Global Change: Atmosphere (0315, 0325); 0365 Atmospheric Composition and Structure: Troposphere-composition and chemistry; KEYWORDS: nucleation, sulfuric acid, water, aerosol formation Citation: Vehkamäki, H., M. Kulmala, I. Napari, K. E. J. Lehtinen, C. Timmreck, M. Noppel, and A. Laaksonen, An improved parameterization for sulfuric acid -water nucleation rates for tropospheric and stratospheric conditions,

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Section: Theory and Modelmentioning

confidence: 99%

Section: Theory and Modelmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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An improved parameterization for sulfuric acid–water nucleation rates for tropospheric and stratospheric conditions

et al. 2002

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“…For more details regarding CBHN and hydrate theory, the reader is referred to Heist and Reiss [], Jaecker‐Voirol et al . [], Jaecker‐Voirol and Mirabel [, ], Noppel [, ], Noppel et al . [], and Seinfeld and Pandis [, Chapter 11].…”

Section: Cn Layer Formationmentioning

confidence: 99%

“…Thus, ΔG * refers to ΔG Ã unhyd , the uncorrected free energy. For more details regarding CBHN and hydrate theory, the reader is referred to Heist and Reiss [1974], Jaecker-Voirol et al [1987], Jaecker-Voirol and Mirabel [1988,1989], Noppel [1998Noppel [ , 2000, Noppel et al [2002], and Seinfeld and Pandis [2006, Chapter 11].…”

Section: Nucleation Modelingmentioning

confidence: 99%

Condensation nuclei measurements in the midlatitude (1982–2012) and Antarctic (1986–2010) stratosphere between 20 and 35 km

Campbell

Deshler

2014

JGR Atmospheres

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[1] Balloon-borne stratospheric condensation nuclei (CN) measurements have been made from McMurdo Station, Antarctica (78°S), 1986-2010, and from Laramie, Wyoming (41°N), 1982 to the present. In the Antarctic region, the measurements show the formation of a layer of enhanced concentrations of stratospheric CN, between 21 and 27 km, around mid August, reaching its maximum extent between September and early October. CN concentrations increase from backgrounds of 10-20 cm À3 to over 100 cm À3 in the layer. In the northern midlatitudes, the measurements show a quasi-annual and smaller layer of enhanced CN concentrations between 25 and 31 km in late winter and early spring. In the quasi-annual layers, CN concentrations increase from backgrounds of 1-10 cm À3 to over 20 cm À3. Volcanic eruptions appear to enhance the CN layers observed over Laramie and McMurdo. The Arctic Oscillation generally correlates with the magnitude of the Laramie CN layer, suggesting the importance of meridional transport. Volatility measurements and nucleation modeling support a sulfuric acid and water composition and binary homogeneous nucleation as the likely CN formation mechanism in both locations. Bimonthly measurements above Laramie support coagulation as the main reason for the dissipation of the CN layer. Air parcel trajectory modeling confirms that the CN layer forms locally to McMurdo and that it is related to solar exposure, while above Laramie trajectory analysis indicates that Arctic conditions and ambient temperature changes during northerly transport impact the magnitude of the CN layer above Laramie.

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Thermodynamics of Nafion™–vapor interactions. I. Water vapor

Reucroft

Rivin

Schneider

2002

Polymer

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Enthalpy and entropy changes in formation of gas phase sulfnric acid monohydrates and dihydrates as a result of fitting to experimental pressure data

Cited by 12 publications

References 26 publications

An improved parameterization for sulfuric acid–water nucleation rates for tropospheric and stratospheric conditions

An improved parameterization for sulfuric acid–water nucleation rates for tropospheric and stratospheric conditions

Condensation nuclei measurements in the midlatitude (1982–2012) and Antarctic (1986–2010) stratosphere between 20 and 35 km

Thermodynamics of Nafion™–vapor interactions. I. Water vapor

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