Diamines Can Initiate New Particle Formation in the Atmosphere

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Elm , J , Passananti , M , Kurten , T & Vehkamäki , H 2017 , ' Diamines Can Initiate New Particle Formation in the Atmosphere ' , Journal of Physical Chemistry A , vol. 121 , no. 32 , pp. 6155-6164 . https://doi.org/10.1021/acs.jpca.7b05658

Title: Diamines Can Initiate New Particle Formation in the Atmosphere
Author: Elm, Jonas; Passananti, Monica; Kurten, Theo; Vehkamäki, Hanna
Contributor organization: Department of Physics
Department of Chemistry
Date: 2017-08-17
Language: eng
Number of pages: 10
Belongs to series: Journal of Physical Chemistry A
ISSN: 1089-5639
DOI: https://doi.org/10.1021/acs.jpca.7b05658
URI: http://hdl.handle.net/10138/299838
Abstract: Recent experimental evidence suggests that diamines can enhance atmospheric new particle formation more efficiently compared to monoamines such as dimethylamine Here we investigate the molecular interactions between sulfuric acid (sa) and the diamine putrescine (put) using computational methods. The molecular structure of up to four sulfuric acid molecules and up to four putrescine molecules were obtained, at the omega B97X-D/6-31++G(d,p) level of theory. We utilized a domain local pair natural orbital coupled cluster method (DLPNO-CCSD(T)/aug-cc-pVTZ) to obtain highly accurate binding energies of the clusters. We find that the (sa)(1-4)(put)(1-4) clusters show more ionic character than clusters consisting of sulfuric acid and dimethylamine (dma) by readily forming several sulfate ions in the cluster. To estimate the stability of the clusters, we calculate the evaporation rates and compare them to ESI-APi-TOF measurements. Using the atmospheric cluster dynamics code (ACDC), we simulate and compare the new particle formation rates between the (sa)(1-4)(put)(1-4) and (sa),(1-4)(dma)(1-4) cluster systems. We find that putrescine significantly enhances the formation of new particles compared to dimethylamine. Our findings suggest that a large range of amines with different basicity is capable of explaining various regions of the observed new particle formation events. These results indicate that diamines, or related compounds with high basicity, might be important species in forming the initial cluster with sulfuric acid and subsequently more abundant amines with lower basicity can assist in the new particle formation process by attaching to the sulfuric acid-diamine nucleus.
Subject: DENSITY-FUNCTIONAL THEORY
PRE-NUCLEATION CLUSTERS
SCOTS PINE FOREST
SULFURIC-ACID
EARTHS ATMOSPHERE
BOREAL FOREST
MASS-SPECTROMETER
AMINES
DIMETHYLAMINE
AMMONIA
114 Physical sciences
116 Chemical sciences
Peer reviewed: Yes
Rights: unspecified
Usage restriction: openAccess
Self-archived version: acceptedVersion


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