Preprints
https://doi.org/10.5194/egusphere-2023-2587
https://doi.org/10.5194/egusphere-2023-2587
15 Nov 2023
 | 15 Nov 2023

How non-equilibrium aerosol chemistry impacts particle acidity: the GMXe AERosol CHEMistry (GMXe–AERCHEM, v1.0) sub-submodel of MESSy

Simon Rosanka, Holger Tost, Rolf Sander, Patrick Jöckel, Astrid Kerkweg, and Domenico Taraborrelli

Abstract. Aqueous-phase chemical processes in clouds, fog, and deliquescent aerosols are known to alter atmospheric composition and acidity significantly. Traditionally, global and regional models predict aerosol composition by relying on thermodynamic equilibrium models and neglect non-equilibrium processes. Here, we present the AERosol CHEMistry (GMXe–AERCHEM, v1.0) sub-submodel developed for the Modular Earth Submodel System (MESSy) as an add-on to the thermodynamic equilibrium model (i.e., ISORROPIA-II) used by MESSy’s Global Modal-aerosol eXtension (GMXe) submodel. AERCHEM allows the representation of non-equilibrium aqueous-phase chemistry of varying complexity in deliquescent fine aerosols. We perform a global simulation for the year 2010 by using the available detailed kinetic model for the chemistry of inorganic and small oxygenated organics. We evaluate AERCHEM’s performance by comparing the simulated concentrations of sulfate, nitrate, ammonium, and chloride to in situ measurements of three monitoring networks. Overall, AERCHEM reproduces observed concentrations reasonably well. We find that especially in the USA, the consideration of non-equilibrium chemistry in deliquescent aerosols reduces the model bias for sulfate, nitrate, and ammonium, when compared to simulated concentrations by ISORROPIA-II. Over most continental regions, fine aerosol acidity simulated by AERCHEM is similar to the predictions by ISORROPIA-II but tends to simulate slightly lower aerosol acidity in most regions. The consideration of non-equilibrium chemistry in deliquescent aerosols leads to a significant higher aerosol acidity in the marine boundary layer, which is in line with observations and recent literature. AERCHEM allows investigating the global-scale impact of aerosol non-equilibrium chemistry on atmospheric composition. This will aid the exploration of key multiphase processes and improve the model predictions for oxidation capacity and aerosols in the troposphere.

Journal article(s) based on this preprint

10 Apr 2024
How non-equilibrium aerosol chemistry impacts particle acidity: the GMXe AERosol CHEMistry (GMXe–AERCHEM, v1.0) sub-submodel of MESSy
Simon Rosanka, Holger Tost, Rolf Sander, Patrick Jöckel, Astrid Kerkweg, and Domenico Taraborrelli
Geosci. Model Dev., 17, 2597–2615, https://doi.org/10.5194/gmd-17-2597-2024,https://doi.org/10.5194/gmd-17-2597-2024, 2024
Short summary
Simon Rosanka, Holger Tost, Rolf Sander, Patrick Jöckel, Astrid Kerkweg, and Domenico Taraborrelli

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on "How non-equilibrium aerosol chemistry impacts particle acidity...."', Anonymous Referee #1, 04 Dec 2023
  • RC2: 'Comment on egusphere-2023-2587', Anonymous Referee #2, 11 Dec 2023

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on "How non-equilibrium aerosol chemistry impacts particle acidity...."', Anonymous Referee #1, 04 Dec 2023
  • RC2: 'Comment on egusphere-2023-2587', Anonymous Referee #2, 11 Dec 2023

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload
AR by Simon Rosanka on behalf of the Authors (08 Feb 2024)  Author's response   Author's tracked changes   Manuscript 
ED: Publish as is (12 Feb 2024) by Jason Williams
AR by Simon Rosanka on behalf of the Authors (16 Feb 2024)

Journal article(s) based on this preprint

10 Apr 2024
How non-equilibrium aerosol chemistry impacts particle acidity: the GMXe AERosol CHEMistry (GMXe–AERCHEM, v1.0) sub-submodel of MESSy
Simon Rosanka, Holger Tost, Rolf Sander, Patrick Jöckel, Astrid Kerkweg, and Domenico Taraborrelli
Geosci. Model Dev., 17, 2597–2615, https://doi.org/10.5194/gmd-17-2597-2024,https://doi.org/10.5194/gmd-17-2597-2024, 2024
Short summary
Simon Rosanka, Holger Tost, Rolf Sander, Patrick Jöckel, Astrid Kerkweg, and Domenico Taraborrelli

Data sets

Model simulation data used in "How non-equilibrium aerosol chemistry impacts particle acidity: the GMXe AERosol CHEMistry (GMXe-AERCHEM, v1.0) sub-submodel of MESSy" Simon Rosanka, Holger Tost, Rolf Sander, Patrick Jöckel, Astrid Kerkweg, and Domenico Taraborrelli https://doi.org/10.5281/zenodo.10059700

Simon Rosanka, Holger Tost, Rolf Sander, Patrick Jöckel, Astrid Kerkweg, and Domenico Taraborrelli

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Short summary
The capabilities of the Modular Earth Submodel System (MESSy) are extended to account for non-equilibrium aqueous-phase chemistry in the representation of deliquescent aerosols. When applying the new development in a global simulation we find that MESSy’s bias in modelling routinely observed inorganic aerosol mass concentrations is reduced. Furthermore, the representation of fine aerosol pH is particularly improved in the marine boundary layer.