Molecular-Level Understanding of Synergistic Effects in Sulfuric Acid-Amine-Ammonia Mixed Clusters. Myllys, N., Chee, S., Olenius, T., Lawler, M., & Smith, J. Journal of Physical Chemistry A, 123(12):2420-2425, 2019.
abstract   bibtex   
The abundance and basicity of a stabilizing base have shown to be key factors in sulfuric acid driven atmospheric new-particle formation. However, since experiments indicate that a low concentration of ammonia enhances particle formation from sulfuric acid and dimethylamine, which is a stronger base, there must be additional factors affecting the particle formation efficiency. Using quantum chemistry, we provide a molecular-level explanation for the synergistic effects in sulfuric acid-dimethylamine-ammonia cluster formation. Because of the capability of ammonia to form more intermolecular interactions than dimethylamine, it can act as a bridge-former in sulfuric acid-dimethylamine clusters. In many cluster compositions, ammonia is more likely to be protonated than dimethylamine, although it is a weaker base. By nanoparticle formation rate simulations, we show that due to the synergistic effects, ammonia can increase the particle formation rate by up to 5 orders of magnitude compared to the two-component sulfuric acid-amine system.
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 title = {Molecular-Level Understanding of Synergistic Effects in Sulfuric Acid-Amine-Ammonia Mixed Clusters},
 type = {article},
 year = {2019},
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 pages = {2420-2425},
 volume = {123},
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 created = {2019-07-11T17:26:48.110Z},
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 abstract = {The abundance and basicity of a stabilizing base have shown to be key factors in sulfuric acid driven atmospheric new-particle formation. However, since experiments indicate that a low concentration of ammonia enhances particle formation from sulfuric acid and dimethylamine, which is a stronger base, there must be additional factors affecting the particle formation efficiency. Using quantum chemistry, we provide a molecular-level explanation for the synergistic effects in sulfuric acid-dimethylamine-ammonia cluster formation. Because of the capability of ammonia to form more intermolecular interactions than dimethylamine, it can act as a bridge-former in sulfuric acid-dimethylamine clusters. In many cluster compositions, ammonia is more likely to be protonated than dimethylamine, although it is a weaker base. By nanoparticle formation rate simulations, we show that due to the synergistic effects, ammonia can increase the particle formation rate by up to 5 orders of magnitude compared to the two-component sulfuric acid-amine system.},
 bibtype = {article},
 author = {Myllys, Nanna and Chee, Sabrina and Olenius, Tinja and Lawler, Michael and Smith, James},
 journal = {Journal of Physical Chemistry A},
 number = {12}
}

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