Journal
JOURNAL OF PHYSICAL CHEMISTRY A
Volume 123, Issue 12, Pages 2420-2425Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.9b00909
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Funding
- Jenny and Antti Wihuri Foundation
- U.S. National Science Foundation [CHE-1710580]
- Swedish Research Council Formas [2015-749]
- Knut and Alice Wallenberg Foundation (Academy Fellowship AtmoRemove)
- AForsk Foundation [18-334]
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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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