Preprints
https://doi.org/10.5194/acp-2021-752
https://doi.org/10.5194/acp-2021-752

  24 Sep 2021

24 Sep 2021

Review status: this preprint is currently under review for the journal ACP.

Technical note: Entrainment-limited kinetics of bimolecular reactions in clouds

Christopher D. Holmes Christopher D. Holmes
  • Earth, Ocean, and Atmospheric Science, Florida State University, Tallahassee, FL 32306, USA

Abstract. The method of entrainment-limited kinetics enables atmospheric chemistry models that do not resolve clouds to simulate heterogeneous (surface and multiphase) cloud chemistry more accurately and efficiently than previous numerical methods. The method, which was previously described for reactions with first-order kinetics in clouds, incorporates cloud entrainment into the kinetic rate coefficient. This technical note shows how bimolecular reactions with second-order kinetics in clouds can also be treated with entrainment-limited kinetics, enabling efficient simulations of a wider range of cloud chemistry reactions. Accuracy is demonstrated using oxidation of SO2 to S(VI) – a key step in formation of acid rain – as an example. Over a large range of reaction rates, cloud fractions, and initial reactant concentrations, the numerical errors in the entrainment-limited bimolecular reaction rates are typically << 1 % and always < 4 %, which is far smaller than the errors found in several commonly used methods of simulating cloud chemistry with fractional cloud cover.

Christopher D. Holmes

Status: open (until 05 Nov 2021)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-752', Anonymous Referee #1, 13 Oct 2021 reply

Christopher D. Holmes

Christopher D. Holmes

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Short summary
Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
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