New particle formation from sulfuric acid and amines : Comparison of monomethylamine, dimethylamine, and trimethylamine

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Olenius , T , Halonen , R , Kurten , T , Henschel , H , Kupiainen-Määttä , O , Ortega , I K , Jen , C N , Vehkamäki , H & Riipinen , I 2017 , ' New particle formation from sulfuric acid and amines : Comparison of monomethylamine, dimethylamine, and trimethylamine ' , Journal of Geophysical Research : Atmospheres , vol. 122 , no. 13 , pp. 7103-7118 . https://doi.org/10.1002/2017JD026501

Title: New particle formation from sulfuric acid and amines : Comparison of monomethylamine, dimethylamine, and trimethylamine
Author: Olenius, Tinja; Halonen, Roope; Kurten, Theo; Henschel, Henning; Kupiainen-Määttä, Oona; Ortega, Ismael K.; Jen, Coty N.; Vehkamäki, Hanna; Riipinen, Ilona
Contributor organization: Department of Physics
Department of Chemistry
Date: 2017-07-16
Language: eng
Number of pages: 16
Belongs to series: Journal of Geophysical Research : Atmospheres
ISSN: 2169-897X
DOI: https://doi.org/10.1002/2017JD026501
URI: http://hdl.handle.net/10138/231077
Abstract: Amines are bases that originate from both anthropogenic and natural sources, and they are recognized as candidates to participate in atmospheric aerosol particle formation together with sulfuric acid. Monomethylamine, dimethylamine, and trimethylamine (MMA, DMA, and TMA, respectively) have been shown to enhance sulfuric acid-driven particle formation more efficiently than ammonia, but both theory and laboratory experiments suggest that there are differences in their enhancing potentials. However, as quantitative concentrations and thermochemical properties of different amines remain relatively uncertain, and also for computational reasons, the compounds have been treated as a single surrogate amine species in large-scale modeling studies. In this work, the differences and similarities of MMA, DMA, and TMA are studied by simulations of molecular cluster formation from sulfuric acid, water, and each of the three amines. Quantum chemistry-based cluster evaporation rate constants are applied in a cluster population dynamics model to yield cluster concentrations and formation rates at boundary layer conditions. While there are differences, for instance, in the clustering mechanisms and cluster hygroscopicity for the three amines, DMA and TMA can be approximated as a lumped species. Formation of nanometer-sized particles and its dependence on ambient conditions is roughly similar for these two: both efficiently form clusters with sulfuric acid, and cluster formation is rather insensitive to changes in temperature and relative humidity. Particle formation from sulfuric acid and MMA is weaker and significantly more sensitive to ambient conditions. Therefore, merging MMA together with DMA and TMA introduces inaccuracies in sulfuric acid-amine particle formation schemes.
Subject: OXIDIZED ORGANIC-MOLECULES
ATMOSPHERIC CONDITIONS
FREE-ENERGIES
CLUSTERS
NUCLEATION
AMMONIA
HYDRATION
WATER
THERMOCHEMISTRY
METHYLAMINE
114 Physical sciences
116 Chemical sciences
Peer reviewed: Yes
Rights: other
Usage restriction: openAccess
Self-archived version: publishedVersion


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