Geographical and diurnal features of amine‐enhanced boundary layer nucleation

Bergman, Tommi; Laaksonen, A.; Korhonen, Hannele; Malila, Jussi; Dunne, Eimear M.; Mielonen, Tero; Lehtinen, K. E. J.; Kühn, Thomas; Arola, Antti; Kokkola, Harri

doi:10.1002/2015jd023181

Cited by 44 publications

(51 citation statements)

References 144 publications

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“…To summarize, dimethylamine has hitherto been the most studied atmospheric amine. While other similar amine species have been assumed to have comparable average properties with respect to clustering [e.g., Loukonen et al, 2010;Bergman et al, 2015], both experimental [Jen et al, 2014;Glasoe et al, 2015] and theoretical [Kurtén et al, 2008;Paasonen et al, 2012] studies suggest that there may be differences between the stabilization potentials of different alkylamines at least for the smallest clusters. Systematic comparisons of different amine species are scarce, but they are needed to assess how to treat this complex array of species in atmospheric models.…”

Section: Introductionmentioning

confidence: 99%

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

et al. 2017

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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.

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Section: Introductionmentioning

confidence: 99%

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

et al. 2017

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“…It is further known that marine biota also release certain gasphase amines, such as trimethylamine (TMA), into the atmosphere (e.g., Ge et al, 2011a;Van Neste et al, 1987;Gibb et al, 1999;Facchini et al, 2008), which subsequently may contribute to aerosol chemistry. Numerous chamber, modeling and field studies at southern latitudes (e.g., Almeida et al, 2013;Kürten et al, 2017;You et al, 2014;Bergman et al, 2015;Müller et al, 2009) have focused on sources, emission rates and gas-to-particle partitioning processes of atmospheric amines. So far, this research has shown that amines may take part in aerosol chemistry in several ways.…”

Section: Introductionmentioning

confidence: 99%

Particulate trimethylamine in the summertime Canadian high Arctic lower troposphere

et al. 2017

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Abstract. Size-resolved and vertical profile measurements of single particle chemical composition (sampling altitude range 50-3000 m) were conducted in July 2014 in the Canadian high Arctic during an aircraft-based measurement campaign (NETCARE 2014). We deployed the single particle laser ablation aerosol mass spectrometer ALABAMA (vacuum aerodynamic diameter range approximately 200-1000 nm) to identify different particle types and their mixing states. On the basis of the single particle analysis, we found that a significant fraction (23 %) of all analyzed particles (in total: 7412) contained trimethylamine (TMA). Two main pieces of evidence suggest that these TMA-containing particles originated from emissions within the Arctic boundary layer. First, the maximum fraction of particulate TMA occurred in the Arctic boundary layer. Second, compared to particles observed aloft, TMA particles were smaller and less oxidized. Further, air mass history analysis, associated wind data and comparison with measurements of methanesulfonic acid give evidence of a marine-biogenic influence on particulate TMA. Moreover, the external mixture of TMAcontaining particles and sodium and chloride ("Na / Cl-") containing particles, together with low wind speeds, suggests particulate TMA results from secondary conversion of precursor gases released by the ocean. In contrast to TMAcontaining particles originating from inner-Arctic sources, particles with biomass burning markers (such as levoglucosan and potassium) showed a higher fraction at higher altitudes, indicating long-range transport as their source. Our measurements highlight the importance of natural, marine inner-Arctic sources for composition and growth of summertime Arctic aerosol.

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“…Only one study has so far reported sulfuric acid-amine nucleation (Zhao et al, 2011) despite amine mixing ratios of up to tens of parts per trillion volume at some sites (Yu and Lee, 2012;You et al, 2014;Freshour et al, 2014;Yao et al, 2016). A global modeling study of sulfuric acid-amine nucleation has been carried out so far (Bergman et al, 2015), applying a nucleation parametrization based on the measurements of Almeida et al (2013) and Glasoe et al (2015).…”

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confidence: 99%

New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

et al. 2018

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Abstract. A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios ( ∼ 100) relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1 × 10 6 and 3 × 10 7 cm −3 , and dimethylamine mixing ratio of ∼ 40 pptv, i.e., 1 × 10 9 cm −3 ).

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Geographical and diurnal features of amine‐enhanced boundary layer nucleation

Cited by 44 publications

References 144 publications

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

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

Particulate trimethylamine in the summertime Canadian high Arctic lower troposphere

New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

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