Rapid Formation of Sulfuric Acid Particles at Near-Atmospheric Conditions

Berndt, Torsten; Böge, Olaf; Stratmann, Frank; Heintzenberg, Jost; Kulmala, Markku

doi:10.1126/science.1104054

Cited by 186 publications

(254 citation statements)

References 33 publications

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“…We compared our results to previous experiments of α-pinene ozonolysis conducted in the Tropos Laminar Flow Tube (Berndt et al, 2005) and the…”

Section: Methodssupporting

confidence: 55%

Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber

Sarnela¹,

Jokinen²,

Duplissy³

et al. 2017

Preprint

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Abstract. Atmospheric oxidation is an important phenomenon, which produces large quantities of low-volatile 30 compounds such as sulphuric acid and oxidised organic compounds. Such species may be involved in nucleation of particles and enhance their subsequent growth to reach the size of cloud condensation nuclei (CCN). In this study, we investigate α-pinene, the most abundant monoterpene globally, and its oxidation products formed through the ozonolysis in the Cosmic Leaving OUtdoors Droplets (CLOUD) chamber at CERN (the European Organization for Nuclear Research). By scavenging hydroxyl radicals (OH) with hydrogen (H2), we were able to 2 calculated with a dynamic model. We found molar yields in the range of 3.5 -6.5% for the HOM formation and 22 -32% for the formation of stabilized Criegee Intermediates by fitting our model to the measured concentrations.The simulated time evolution of the ozonolysis products was in good agreement with measured concentrations except that in some of the experiments sulphuric acid formation was faster than simulated. The results shown here are consistent with the recently published yields for HOM formation from different laboratory experiments. 5Together with the sCI yields, these results help to understand atmospheric oxidation processes better and make the reaction parameters more comprehensive for broader use.

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“…We compared our results to previous experiments of α-pinene ozonolysis conducted in the Tropos Laminar Flow Tube (Berndt et al, 2005) and the…”

Section: Methodssupporting

confidence: 55%

Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber

Sarnela¹,

Jokinen²,

Duplissy³

et al. 2017

Preprint

Self Cite

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“…On the other hand, recent laboratory experiments showed that at atmospheric pressure, 288 K and 10-55% RH, the threshold [H 2 SO 4 ] needed for unit J value is in the range of 10 8 -10 9 cm −3 and the measured J was proportional to [H 2 SO 4 ] with the second to tenth powers [Benson et al, 2008]. Other laboratory studies, on the other hand, showed that nucleation takes place at lower [H 2 SO 4 ] concentration [Berndt et al, 2005] and with J proportional to [H 2 SO 4 ] to the first to second power [Metzger et al, 2010] (Figure 7c). This may indicate that NH 3 effects on aerosol nucleation are already saturated at this measured [NH 3 ] (sub-ppbv), as predicted from modeling studies [Merikanto et al, 2007].…”

Section: H 2 So 4 Effects On Nucleationmentioning

confidence: 99%

Correlation of aerosol nucleation rate with sulfuric acid and ammonia in Kent, Ohio: An atmospheric observation

Erupe¹,

Benson²,

Li³

et al. 2010

J. Geophys. Res.

115

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[1] New particle formation (NPF) occurs in various atmospheric environments, and these newly formed particles have the potential to grow to cloud condensation nuclei. But at present it is unclear which chemical species are involved in aerosol nucleation and growth, in part because there are only a limited number of simultaneous measurements of aerosol precursors and aerosol size distributions. Observations of ambient aerosol size distributions, sulfuric acid, and ammonia were made for over a year in Kent, Ohio, a relatively less polluted continental environment. Particle sizes in the diameter range from 3 to 1000 nm were measured continuously through the whole year, while sulfuric acid and ammonia were measured seasonally with two chemical ionization mass spectrometers. Strong NPF events were more frequently found during the spring and fall and less frequently during the summer and winter. The median of measured sulfuric acid was higher in spring (5.2 × 10 6 cm −3 ) and summer (2.9 × 10 6 cm −3 ) than in winter (6 × 10 5 cm −3 ) and fall (5 × 10 5 cm −3 ). We have used the inverse model Particle Growth and Nucleation to derive aerosol nucleation and growth rates from the measured aerosol size distributions. Nucleation rates derived during the NPF events ranged from 1.4 to 12.9 cm −3 s −1 and were proportional to the measured sulfuric acid concentration with a power of 0.6-2.3. Our results show that sulfuric acid is an important aerosol nucleation precursor, but only a small fraction of the aerosol growth rates could be explained by the condensation of sulfuric acid alone. Ammonia mixing ratios did not have a diurnal trend but had some seasonal variations, higher in spring than in fall and winter, typically at sub-ppbv level; aerosol nucleation rates did not show a clear correlation with ammonia at least at this sub-ppbv level, mostly because the ammonia mixing ratios were nearly constant. Our observations also indicate that the role that ammonia plays in aerosol nucleation is more complicated than is currently understood by the aerosol nucleation theories.Citation: Erupe, M. E., et al. (2010), Correlation of aerosol nucleation rate with sulfuric acid and ammonia in Kent, Ohio: An atmospheric observation,

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“…OH radicals were produced from UV dissociation of water vapor; this allows for an ozone-free system and hence provides an advantage compared to other studies where OH was produced from ozone photolysis (Berndt et al, 2005(Berndt et al, , 2006Sipilä et al, 2010).…”

Section: Methodsmentioning

confidence: 99%

“…These newly formed particles further grow by condensation and coagulation and can contribute to a large fraction (15-55 %) of CCN concentrations at the global scale (Merikanto, 2009), but the nucleation mechanisms are not well understood. Atmospheric observations (Erupe et al, 2010;Kulmala et al, 2004;McMurry et al, 2005) and laboratory studies Berndt et al, 2005;Sipilä et al, 2010; have shown that sulfuric acid (H 2 SO 4 ) is the main nucleation precursor, but the role of other ternary species such as ammonia (NH 3 ) and organic compounds is not well understood.…”

Section: Introductionmentioning

confidence: 99%

Ternary homogeneous nucleation of H2SO4, NH3, and H2O under conditions relevant to the lower troposphere

et al. 2011

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Abstract. Ternary homogeneous nucleation (THN) of [NH 3 ] are 3-5, 1-4, and 1, respectively. These slopes and the threshold of [H 2 SO 4 ] required for the unity nucleation vary only fractionally in the presence and absence of NH 3 . These observations can be used to improve aerosol nucleation models to assess how man-made SO 2 and NH 3 affect aerosol formation and CCN production at the global scale.

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Rapid Formation of Sulfuric Acid Particles at Near-Atmospheric Conditions

Cited by 186 publications

References 33 publications

Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber

Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber

Correlation of aerosol nucleation rate with sulfuric acid and ammonia in Kent, Ohio: An atmospheric observation

Ternary homogeneous nucleation of H<sub>2</sub>SO<sub>4</sub>, NH<sub>3</sub>, and H<sub>2</sub>O under conditions relevant to the lower troposphere

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Rapid Formation of Sulfuric Acid Particles at Near-Atmospheric Conditions

Cited by 186 publications

References 33 publications

Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber

Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber

Correlation of aerosol nucleation rate with sulfuric acid and ammonia in Kent, Ohio: An atmospheric observation

Ternary homogeneous nucleation of H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;, NH&lt;sub&gt;3&lt;/sub&gt;, and H&lt;sub&gt;2&lt;/sub&gt;O under conditions relevant to the lower troposphere

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Ternary homogeneous nucleation of H<sub>2</sub>SO<sub>4</sub>, NH<sub>3</sub>, and H<sub>2</sub>O under conditions relevant to the lower troposphere