22 Feb 2024
 | 22 Feb 2024
Status: a revised version of this preprint is currently under review for the journal AR.

A cluster-of-functional-groups approach for studying organic enhanced atmospheric cluster formation

Astrid Nørskov Pedersen, Yosef Knattrup, and Jonas Elm

Abstract. The role of organic compounds in atmospheric new particle formation is difficult to disentangle due to the myriad of potentially important oxygenated organic molecules (OOMs) present in the atmosphere. Using state-of-the-art quantum chemical methods, we here employ a novel approach, denoted the “cluster-of-functional-groups" approach, for studying the involvement of OOMs in atmospheric cluster formation. Instead of the usual “trial-and-error" approach of testing the ability of experimentally identified OOMs to form stable clusters with other nucleation precursors, we here study which, and how many, intermolecular interactions that are required in a given OOM to form stable clusters. In this manner we can reverse engineer the elusive structure of OOM candidates that might be involved in organic enhanced atmospheric cluster formation.

We calculated the binding free energies of all combinations of donor/acceptor organic functional groups to investigate which functional groups that most preferentially bind with each other and with other nucleation precursors such as sulfuric acid and bases (ammonia, methyl-, dimethyl-, and trimethylamine). We find that multiple carboxyl groups leads to substantially more stable clusters compared to all other combinations of functional groups. Employing cluster dynamics simulations, we investigate how a hypothetically OOM composed of multiple carboxyl groups can stablize sulfuric acid – base clusters and provide recommendations for potential atmospheric multi-carboxylic acid tracer compounds that should be explicitly studied in the future.

The presented “cluster-of-functional-groups" approach is generally applicable and can be employed in many other applications, such as ion-induced nucleation and potentially in elucidating the structural patterns in molecules that facilitate ice nucleation.

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Astrid Nørskov Pedersen, Yosef Knattrup, and Jonas Elm

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'a small suggested improvement to the model', Theo Kurtén, 04 Mar 2024
  • RC2: 'Comment on ar-2024-6', Anonymous Referee #2, 10 Mar 2024
  • AC1: 'Comment on ar-2024-6', Jonas Elm, 06 Apr 2024
Astrid Nørskov Pedersen, Yosef Knattrup, and Jonas Elm
Astrid Nørskov Pedersen, Yosef Knattrup, and Jonas Elm


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Short summary
Aerosol formation is an important process for our global climate. While inorganic spiecies have been shown to be important for aerosol formation, there remains a large gap in our knowledge about the exact involvement of organics. We present a new quantum chemical procedure for screening relevant organics that for the first time allow us to obtain direct molecular level insight into the organics involved in aerosol formation.