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Clusterome: A Comprehensive Data Set of Atmospheric Molecular Clusters for Machine Learning Applications

[Image: see text] Formation and growth of atmospheric molecular clusters into aerosol particles impact the global climate and contribute to the high uncertainty in modern climate models. Cluster formation is usually studied using quantum chemical methods, which quickly becomes computationally expens...

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Detalles Bibliográficos
Autores principales: Knattrup, Yosef, Kubečka, Jakub, Ayoubi, Daniel, Elm, Jonas
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10357536/
https://www.ncbi.nlm.nih.gov/pubmed/37483242
http://dx.doi.org/10.1021/acsomega.3c02203
Descripción
Sumario:[Image: see text] Formation and growth of atmospheric molecular clusters into aerosol particles impact the global climate and contribute to the high uncertainty in modern climate models. Cluster formation is usually studied using quantum chemical methods, which quickly becomes computationally expensive when system sizes grow. In this work, we present a large database of ∼250k atmospheric relevant cluster structures, which can be applied for developing machine learning (ML) models. The database is used to train the ML model kernel ridge regression (KRR) with the FCHL19 representation. We test the ability of the model to extrapolate from smaller clusters to larger clusters, between different molecules, between equilibrium structures and out-of-equilibrium structures, and the transferability onto systems with new interactions. We show that KRR models can extrapolate to larger sizes and transfer acid and base interactions with mean absolute errors below 1 kcal/mol. We suggest introducing an iterative ML step in configurational sampling processes, which can reduce the computational expense. Such an approach would allow us to study significantly more cluster systems at higher accuracy than previously possible and thereby allow us to cover a much larger part of relevant atmospheric compounds.