2020
DOI: 10.1021/acs.jpca.0c02932
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Hydration of Atmospheric Molecular Clusters III: Procedure for Efficient Free Energy Surface Exploration of Large Hydrated Clusters

Abstract: Sampling the shallow free energy surface of hydrated atmospheric molecular clusters is a significant challenge. Using computational methods we present an efficient approach to obtain minimum free energy structures for large hydrated clusters of atmospheric relevance. We study clusters consisting of two to four sulfuric acid (sa) molecules and hydrate them with up to five water (w) molecules. The structures of the "dry" clusters are obtained using the ABCluster program to yield a large pool of low-lying conform… Show more

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Cited by 20 publications
(28 citation statements)
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“…While these genetic algorithms show promising applications in cluster formation studies involving acids and bases, they rely on treating the molecules as rigid in the global optimization using a force field, which makes the methods difficult to apply to systems containing organic molecules with many rotamers. Recently, Rasmussen et al (Rasmussen et al, 2020)coupled the approach outlined by Kubečka et al (Kubečka et al, 2019) with the systematic hydrate sampling approach by Kildgaard et al (Kildgaard et al, 2018a,b) for studying the shallow potential free energy surface of sulfuric acid -water clusters. This approach appears to be a viable approach to study multicomponent atmospheric molecular clusters involving water.…”
Section: Potential Energymentioning
confidence: 99%
See 1 more Smart Citation
“…While these genetic algorithms show promising applications in cluster formation studies involving acids and bases, they rely on treating the molecules as rigid in the global optimization using a force field, which makes the methods difficult to apply to systems containing organic molecules with many rotamers. Recently, Rasmussen et al (Rasmussen et al, 2020)coupled the approach outlined by Kubečka et al (Kubečka et al, 2019) with the systematic hydrate sampling approach by Kildgaard et al (Kildgaard et al, 2018a,b) for studying the shallow potential free energy surface of sulfuric acid -water clusters. This approach appears to be a viable approach to study multicomponent atmospheric molecular clusters involving water.…”
Section: Potential Energymentioning
confidence: 99%
“…This will correctly lead to a lowering of the free energy as more conformers are taken into account. The effect of including higher free energy conformers has been shown to be relatively small on the order of -1 kcal/mol or lower for sulfuric acid -ammonia and sulfuric acid -pinic acid clusters (Partanen et al, 2016b), sulfuric acid -guanidine clusters (Kubečka et al, 2019) and sulfuric acid -water clusters (Rasmussen et al, 2020). It has also been illustrated that conformers 3 kcal/mol higher in energy compared to the lowest one will not contribute significantly to the free energy and can safely be neglected (Partanen et al, 2016b).…”
Section: The Effect Of Conformers On the Free Energiesmentioning
confidence: 99%
“…This has led to hydration being quite often neglected in cluster formation studies. Recently, an approach to systematically place water molecules around the exterior/interior of an existing cluster structure has provided an efficient tool to study the hydration of precursors of atmospheric relevance. , Rasmussen et al further coupled this systematic hydration approach with the configurational sampling methodology presented by Kubečka et al This allows for an efficient exploration of the free-energy surface of large hydrated clusters, and thus the incorporation of water molecules should receive more attention in the future.…”
Section: Chemical Complexitymentioning
confidence: 99%
“…In this paper we have studied the hydration of monomers and heterodimers up to 20 water molecules. Previous quantum chemical studies have often modeled up to 4 or 5 water molecules, [13][14][15]61 which limit the study of proton transfer reactions. Here we have discussed connections of aqueous-phase base strength and proton transfer reactions as well as sulfate formation from heterodimer bisulfate ion in water clusters.…”
Section: Discussionmentioning
confidence: 99%