Neutral Sulfuric Acid-Water Clustering Rates: Bridging the Gap between Molecular Simulation and Experiment

Philip T.M. Carlsson; Steven Celik; Daniel Becker; Tinja Olenius; Jonas Elm; Thomas Zeuch

doi:10.1021/acs.jpclett.0c01045

Neutral Sulfuric Acid-Water Clustering Rates: Bridging the Gap between Molecular Simulation and Experiment

Philip T.M. Carlsson, Steven Celik, Daniel Becker, Tinja Olenius, Jonas Elm, Thomas Zeuch

iCLIMATE Aarhus University Interdisciplinary Centre for Climate Change - iCLIMATE Aarhus University Interdisciplinary Centre for Climate Change, Langelandsgade
Department of Chemistry

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Abstract

The role of sulfuric acid during atmospheric new particle formation is an ongoing topic of discussion. In this work, we provide quantitative experimental constraints for quantum chemically calculated evaporation rates for the smallest H2SO4-H2O clusters, characterizing the mechanism governing nucleation on a kinetic, single-molecule level. We compare experimental particle size distributions resulting from a highly supersaturated homogeneous H2SO4 gas phase with the results from kinetic simulations employing quantum chemically derived decomposition rates of electrically neutral H2SO4 molecular clusters up to the pentamer at a large range of relative humidities. By using high H2SO4 concentrations, we circumvent the uncertainties concerning contaminants and competing reactions present in studies at atmospheric conditions. We show good agreement between molecular simulation and experimental measurements and provide the first evaluation of theoretical predictions of the stabilization provided by water molecules.

Original language	English
Journal	The Journal of Physical Chemistry Letters
Volume	11
Issue	10
Pages (from-to)	4239-4244
Number of pages	6
ISSN	1948-7185
DOIs	https://doi.org/10.1021/acs.jpclett.0c01045
Publication status	Published - May 2020

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title = "Neutral Sulfuric Acid-Water Clustering Rates: Bridging the Gap between Molecular Simulation and Experiment",

abstract = "The role of sulfuric acid during atmospheric new particle formation is an ongoing topic of discussion. In this work, we provide quantitative experimental constraints for quantum chemically calculated evaporation rates for the smallest H2SO4-H2O clusters, characterizing the mechanism governing nucleation on a kinetic, single-molecule level. We compare experimental particle size distributions resulting from a highly supersaturated homogeneous H2SO4 gas phase with the results from kinetic simulations employing quantum chemically derived decomposition rates of electrically neutral H2SO4 molecular clusters up to the pentamer at a large range of relative humidities. By using high H2SO4 concentrations, we circumvent the uncertainties concerning contaminants and competing reactions present in studies at atmospheric conditions. We show good agreement between molecular simulation and experimental measurements and provide the first evaluation of theoretical predictions of the stabilization provided by water molecules.",

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Neutral Sulfuric Acid-Water Clustering Rates: Bridging the Gap between Molecular Simulation and Experiment. / Carlsson, Philip T.M.; Celik, Steven; Becker, Daniel et al.
In: The Journal of Physical Chemistry Letters, Vol. 11, No. 10, 05.2020, p. 4239-4244.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

TY - JOUR

T1 - Neutral Sulfuric Acid-Water Clustering Rates

T2 - Bridging the Gap between Molecular Simulation and Experiment

AU - Carlsson, Philip T.M.

AU - Celik, Steven

AU - Becker, Daniel

AU - Olenius, Tinja

AU - Elm, Jonas

AU - Zeuch, Thomas

PY - 2020/5

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AB - The role of sulfuric acid during atmospheric new particle formation is an ongoing topic of discussion. In this work, we provide quantitative experimental constraints for quantum chemically calculated evaporation rates for the smallest H2SO4-H2O clusters, characterizing the mechanism governing nucleation on a kinetic, single-molecule level. We compare experimental particle size distributions resulting from a highly supersaturated homogeneous H2SO4 gas phase with the results from kinetic simulations employing quantum chemically derived decomposition rates of electrically neutral H2SO4 molecular clusters up to the pentamer at a large range of relative humidities. By using high H2SO4 concentrations, we circumvent the uncertainties concerning contaminants and competing reactions present in studies at atmospheric conditions. We show good agreement between molecular simulation and experimental measurements and provide the first evaluation of theoretical predictions of the stabilization provided by water molecules.

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Neutral Sulfuric Acid-Water Clustering Rates: Bridging the Gap between Molecular Simulation and Experiment

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