Particle Nucleation in the Tropical Boundary Layer and Its Coupling to Marine Sulfur Sources

Clarke, A. D.; Davis, Douglas D.; Kapustin, V. N.; Eisele, F. L.; Chen, G.; Paluch, Ilga R.; Lenschow, Donald H.; Bandy, A. R.; Thornton, D. C.; Moore, Katharine F.; Mauldin, L.; Tanner, David J.; Litchy, M.; Carroll, Mary Anne; Collins, J. E.; Albercook, George M.

doi:10.1126/science.282.5386.89

Cited by 216 publications

(181 citation statements)

References 23 publications

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“…There are also measurements that have shown that [H 2 SO 4 ] can be at the 10 8 cm −3 range in the polluted environment [Bardouki et al, 2003;Berresheim et al, 2002]. While these studies were mostly ground-based or in the boundary layer, H 2 SO 4 measurements also exist for the free troposphere [Clarke et al, 1998;Weber et al, 1998] and for the upper troposphere and lower stratosphere [Lee et al, 2003].…”

Section: Introductionmentioning

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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Section: Introductionmentioning

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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“…While probably the most spectacular bursts of particle formation have been observed at coastal sites, they have also been observed in the tropical marine boundary layer [Clarke et al, 1998] and at a remote continental site [Marti et al, 1997].…”

Section: Introductionmentioning

confidence: 99%

Observations of new particle production in the atmosphere of a moderately polluted site in eastern England

Harrison¹,

Grenfell²,

Savage³

et al. 2000

J. Geophys. Res.

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Abstract. Measurements of particle number density and Fuchs surface area, together with a range of gaseous pollutant concentrations, have been made in June 1995 at a coastal site in eastern England which receives air from a range of polluted and less polluted origins. Periods of enhanced local particle production were identified and found to be associated predominantly with relatively polluted air sectors. An examination of the factors contributing to homogeneous nucleation and hence new particle production suggests that those most important at this location are probably the production of hydroxyl radicals and the availability of ammonia. A numerical modeling study calculating characteristic timescales for new particle production and for condensation onto existing aerosol surfaces is able to predict periods of new particle production. The model suggests that oxidation of dimethyl sulphide and sulphur dioxide and homogeneous nucleation of sulphuric acid and water, probably in combination with ammonia, are the source of new particles at this site.

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“…H 2 SO 4 is thought to participate in binary homogeneous nucleation with H 2 O, and more recently, in ternary nucleation with H 2 O and NH 3 . While Clarke et al (1998) found evidence for particle production linked to high DMS emissions in the Pacific, a more robust analysis of particle production from H 2 SO 4 by Pirjola et al (2000) pointed out that while binary nucleation was likely to occur in the polar regions, and ternary nucleation likely to occur in many other marine environments, there is typically insufficient H 2 SO 4 vapour to contribute to growth of stable clusters into aerosol particles (operationally defined as particles with DO3 nm). O'Dowd et al (2002a) demonstrated that unless newly formed stable clusters can grow sufficiently fast, the clusters are scavenged by the preexisting aerosol coagulation sink.…”

Section: Introductionmentioning

confidence: 99%

Marine aerosol production: a review of the current knowledge

O’Dowd

Leeuw

2007

Phil. Trans. R. Soc. A.

647

568

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The current knowledge in primary and secondary marine aerosol formation is reviewed. For primary marine aerosol source functions, recent source functions have demonstrated a significant flux of submicrometre particles down to radii of 20 nm. Moreover, the source functions derived from different techniques up to 10 mm have come within a factor of two of each other. For secondary marine aerosol formation, recent advances have identified iodine oxides and isoprene oxidation products, in addition to sulphuric acid, as contributing to formation and growth, although the exact roles remains to be determined. While a multistep process seems to be required, isoprene oxidation products are more likely to participate in growth and sulphuric acid is more likely to participate in nucleation. Iodine oxides are likely to participate in both nucleation and growth.

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Particle Nucleation in the Tropical Boundary Layer and Its Coupling to Marine Sulfur Sources

Cited by 216 publications

References 23 publications

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

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

Observations of new particle production in the atmosphere of a moderately polluted site in eastern England

Marine aerosol production: a review of the current knowledge

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