Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms

Sihto, S.-L.; Kulmala, Markku; Kerminen, Veli‐Matti; Maso, Miikka Dal; Petäj̈ä, Tuukka; Riipinen, Ilona; Korhonen, Hannele; Arnold, Frank; Janson, Robert W; Boy, Michael; Laaksonen, A.; Lehtinen, K. E. J.

doi:10.5194/acp-6-4079-2006

Cited by 462 publications

(619 citation statements)

References 49 publications

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“…By rearranging the terms, and denoting the first term on the right hand side of Eq. (2) by J 3 , the previous studies (Sihto et al, 2006;Paasonen et al, 2009) gave the Eq. (3) to calculate the particle formation rate at 3 nm:…”

Section: Particle Formation Ratesmentioning

confidence: 99%

“…In order to investigate the role of sulfuric acid in the nucleation process, based on recent observations the relationship between observed nucleation rates and ambient gaseous sulfuric acid concentrations with an exponent between 1 (J =A × [H 2 SO 4 ]) and 2 (J =K × [H 2 SO 4 ] 2 ) have been reported (Sihto et al, 2006;Riipinen et al, 2007;Boy et al, 2008;Kuang et al, 2008;Nieminen et al, 2009;Paasonen et al, 2009). In these publications the authors pointed out that the activation and kinetic nucleation maybe the potential formation mechanisms.…”

Section: Introductionmentioning

confidence: 99%

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Evaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case

Wang

Yue

et al. 2011

Atmos. Chem. Phys.

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Abstract. New particle formation (NPF) is considered as an important mechanism for gas-to-particle transformation, and gaseous sulfuric acid is believed as a crucial precursor. Up to now few field-based studies on nucleation mechanisms and the role of sulfuric acid were conducted in China. In this study, simultaneously measurements of particle number size distributions and gaseous sulfuric acid concentrations were performed from July to September in 2008. Totally, 22 new particle formation events were observed during the entire 85 campaign days. The results show that in the case of both higher source and sink values, the result of the competition between source and sink is more likely the key limiting factor to determine the observation of NPF events in Beijing. The concentrations of gaseous sulfuric acid show good correlations with freshly nucleated particles (N 3−6 ) and formation rates (J 3 and J 1.5 ). The power-law relationship between H 2 SO 4 concentration and N 3−6 or J is adopted to explore the nucleation mechanism. The exponents are showed a great range (from 1 to 7). More than half of the NPF events exhibit an exponent larger than 2.5. For these cases, the thermodynamic process works better than the activation or kinetic nucleation theories to explain the nucleation events in urban atmosphere of Beijing.

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Section: Particle Formation Ratesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Evaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case

Wang

Yue

et al. 2011

Atmos. Chem. Phys.

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“…Ambient and laboratory studies have shown that sulfuric acid participates in the first steps of new particle formation (Weber et al, 1996;Sihto et al, 2006;Riipinen et al, 2007;Kuang et al, 2008;Sipilä et al, 2010;Vehkamäki and Riipinen, 2012;Kulmala et al, 2013), but sulfuric acid condensation is not enough to reproduce particle growth rates observed in the ambient conditions (Kuang et al, 2010;Sipilä et al, 2010;Pierce et al, 2011Pierce et al, , 2012Riipinen et al, 2011Riipinen et al, , 2012Kulmala et al, 2013). Therefore other compounds, e.g., organics or ammonia/amines, are expected to be important in the early growth of freshly nucleated particles (O'Dowd et al, 2002;Smith et al, 2005Smith et al, , 2008Pierce et al, 2011;Riipinen et al, 2012;Vehkamäki and Riipinen, 2012;Kulmala et al, 2013).…”

Section: S a K Häkkinen Et Al: Semi-empirical Parameterization Ofmentioning

confidence: 99%

Semi-empirical parameterization of size-dependent atmospheric nanoparticle growth in continental environments

et al. 2013

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The capability to accurately yet efficiently represent atmospheric nanoparticle growth by biogenic and anthropogenic secondary organics is a challenge for current atmospheric large-scale models. It is, however, crucial to predict nanoparticle growth accurately in order to reliably estimate the atmospheric cloud condensation nuclei (CCN) concentrations. In this work we introduce a simple semi-empirical parameterization for sub-20 nm particle growth that distributes secondary organics to the nanoparticles according to their size and is therefore able to reproduce particle growth observed in the atmosphere. The parameterization includes particle growth by sulfuric acid, secondary organics from monoterpene oxidation (SORG_MT) and an additional condensable vapor of non-monoterpene organics ("background"). The performance of the proposed parameterization was investigated using ambient data on particle growth rates in three diameter ranges (1.5–3 nm, 3–7 nm and 7–20 nm). The growth rate data were acquired from particle/air ion number size distribution measurements at six continental sites over Europe. The longest time series of 7 yr (2003–2009) was obtained from a boreal forest site in Hyytiälä, Finland, while about one year of data (2008–2009) was used for the other stations. The extensive ambient measurements made it possible to test how well the parameterization captures the seasonal cycle observed in sub-20 nm particle growth and to determine the weighing factors for distributing the SORG_MT for different sized particles as well as the background mass flux (concentration). Besides the monoterpene oxidation products, background organics with a concentration comparable to SORG_MT, around 6 × 10⁷ cm⁻³ (consistent with an additional global SOA yield of 100 Tg yr⁻¹) was needed to reproduce the observed nanoparticle growth. Simulations with global models suggest that the "background" could be linked to secondary biogenic organics that are formed in the presence of anthropogenic pollution

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“…However, the uncertainty in this number is large and it is still unclear which vapors are participating in the formation of the critical nucleus under certain conditions and which species contribute to its early growth. In most cases atmospheric boundary layer nucleation events cannot be explained solely by the binary system of sulfuric acid and water, although a correlation with the sulfuric acid concentration is generally observed 2,3 . Consequently, ternary vapors need to participate and it has been suggested that ammonia plays a key role 4,5 .…”

Section: Ternary H 2 So 4 -H 2 O-dimethylamine Nucleationmentioning

confidence: 99%

Measurement of neutral sulfuric acid-dimethylamine clusters using CI-APi-TOF-MS

Simon¹,

Kürten²,

Jokinen³

et al. 2013

AIP Conference Proceedings

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Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms

Cited by 462 publications

References 49 publications

Evaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case

Evaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case

Semi-empirical parameterization of size-dependent atmospheric nanoparticle growth in continental environments

Measurement of neutral sulfuric acid-dimethylamine clusters using CI-APi-TOF-MS

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