Journal article

Identification and quantification of particle growth channels during new particle formation

Pennington M, Bzdek B, Depalma J, Smith J, Kortelainen A, Hildebrandt Ruiz L, Pet??j?? T, Kulmala M, Worsnop D, Johnston M ...see all

Atmospheric Chemistry and Physics, vol. 13, issue 20 (2013) pp. 10215-10225

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Abstract

Atmospheric new particle formation (NPF) is a key source of ambient
ultrafine particles that may contribute substantially to the global
production of cloud condensation nuclei (CCN). While NPF is driven by
atmospheric nucleation, its impact on CCN concentration depends strongly
on atmospheric growth mechanisms since the growth rate must exceed the
loss rate due to scavenging in order for the particles to reach the CCN
size range. In this work, chemical composition measurements of 20 nm
diameter particles during NPF in Hyytiala, Finland, in March-April 2011
permit identification and quantitative assessment of important growth
channels. In this work we show the following: (A) sulfuric acid, a key
species associated with atmospheric nucleation, accounts for less than
half of particle mass growth during this time period; (B) the sulfate
content of a growing particle during NPF is quantitatively explained by
condensation of gas-phase sulfuric acid molecules (i.e., sulfuric acid
uptake is collision-limited); (C) sulfuric acid condensation
substantially impacts the chemical composition of preexisting
nanoparticles before new particles have grown to a size sufficient to be
measured; (D) ammonium and sulfate concentrations are highly correlated,
indicating that ammonia uptake is driven by sulfuric acid uptake; (E)
sulfate neutralization by ammonium does not reach the predicted
thermodynamic end point, suggesting that a barrier exists for ammonia
uptake; (F) carbonaceous matter accounts for more than half of the
particle mass growth, and its oxygen-to-carbon ratio (similar to 0.5) is
characteristic of freshly formed secondary organic aerosol; and (G)
differences in the overall growth rate from one formation event to
another are caused by variations in the growth rates of all major
chemical species, not just one individual species.

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Authors

  • M. Ross Pennington

  • B. R. Bzdek

  • J. W. Depalma

  • J. N. Smith

  • A. M. Kortelainen

  • L. Hildebrandt Ruiz

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