Preprints
https://doi.org/10.5194/egusphere-2022-1449
https://doi.org/10.5194/egusphere-2022-1449
25 Jan 2023
 | 25 Jan 2023

Collision-sticking rates of acid–base clusters in the gas phase determined from atomistic simulation and a novel analytical interacting hard-sphere model

Huan Yang, Ivo Neefjes, Valtteri Tikkanen, Jakub Kubečka, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl

Abstract. Kinetics of collision-sticking processes between vapor molecules and clusters of low volatile compounds govern the initial steps of atmospheric new particle formation. Conventional non-interacting hard-sphere models underestimate the collision rate by neglecting long-range attractive forces, and the commonly adopted assumption that every collision leads to the formation of a stable cluster (unit mass accommodation coefficient) is questionable for small clusters, especially at elevated temperatures. Here, we present a generally applicable analytical interacting hard-sphere model for evaluating collision rates between molecules and clusters, accounting for long-range attractive forces. In the model, the collision cross section is calculated based on an effective molecule-cluster potential, derived using Hamaker's approach. Applied to collisions of sulfuric acid or dimethylamine with neutral bisulphate-dimethylammonium clusters composed of 1–32 dimers, our new model predicts collision rates 2–3 times higher than the non-interacting model for small clusters, while decaying asymptotically to the non-interacting limit as cluster size increases, in excellent agreement with a collision rate theory-atomistic molecular dynamics simulation approach. Additionally, we calculated sticking rates and mass accommodation coefficients (MAC) using atomistic molecular dynamics collision simulations. For sulfuric acid, unit MAC is observed for collisions with all cluster sizes at temperatures between 200 K and 400 K. For dimethylamine, we find that MACs decrease with increasing temperature and decreasing cluster size. At low temperatures, the unit MAC assumption is generally valid, but at elevated temperatures MACs can drop below 0.2 for small clusters.

Journal article(s) based on this preprint

01 Jun 2023
Collision-sticking rates of acid–base clusters in the gas phase determined from atomistic simulation and a novel analytical interacting hard-sphere model
Huan Yang, Ivo Neefjes, Valtteri Tikkanen, Jakub Kubečka, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 23, 5993–6009, https://doi.org/10.5194/acp-23-5993-2023,https://doi.org/10.5194/acp-23-5993-2023, 2023
Short summary

Huan Yang et al.

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2022-1449', Anonymous Referee #1, 15 Feb 2023
  • RC2: 'Comment on egusphere-2022-1449', Anonymous Referee #2, 26 Feb 2023

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2022-1449', Anonymous Referee #1, 15 Feb 2023
  • RC2: 'Comment on egusphere-2022-1449', Anonymous Referee #2, 26 Feb 2023

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload
AR by huan yang on behalf of the Authors (18 Apr 2023)  Author's response   Author's tracked changes   Manuscript 
ED: Referee Nomination & Report Request started (19 Apr 2023) by Hinrich Grothe
RR by Anonymous Referee #1 (02 May 2023)
ED: Publish as is (02 May 2023) by Hinrich Grothe
AR by huan yang on behalf of the Authors (02 May 2023)

Journal article(s) based on this preprint

01 Jun 2023
Collision-sticking rates of acid–base clusters in the gas phase determined from atomistic simulation and a novel analytical interacting hard-sphere model
Huan Yang, Ivo Neefjes, Valtteri Tikkanen, Jakub Kubečka, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 23, 5993–6009, https://doi.org/10.5194/acp-23-5993-2023,https://doi.org/10.5194/acp-23-5993-2023, 2023
Short summary

Huan Yang et al.

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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.

Short summary
We present a new analytical model for collision rates between molecules and clusters of arbitrary sizes, that accounts for long-range interactions. The model is verified against atomistic simulations of typical acid-base clusters participating in atmospheric new particle formation. Results show that accounting for long-range interactions leads to 2–3 times higher collision rates for small clusters, indicating the necessity of including such forces in atmospheric new particle formation modelling.