References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-10-8469-2010

An improved criterion for new particle formation in diverse atmospheric environments

Kuang

¹ ² Riipinen

³ ⁴ Sihto

S.-L.

⁴ Kulmala

⁴ McCormick

A. V.

¹ McMurry

P. H.

Department of Chemical Engineering & Materials Science, University of Minnesota, 151 Amundson Hall, 421 Washington Avenue SE, Minneapolis, Minnesota 55455, USA

Department of Mechanical Engineering, University of Minnesota, 1100 Mechanical Engineering, 111 Church Street SE, Minneapolis, Minnesota 55455, USA

Department of Chemical Engineering, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburg, Pennsylvania 15213, USA

Department of Physics, University of Helsinki, P.O. Box 64, 00014, Helsinki, Finland

08 09 2010

10 17 8469 8480

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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A dimensionless theory for new particle formation (NPF) was developed, using an aerosol population balance model incorporating recent developments in nucleation rates and measured particle growth rates. Based on this theoretical analysis, it was shown that a dimensionless parameter LΓ, characterizing the ratio of the particle scavenging loss rate to the particle growth rate, exclusively determined whether or not NPF would occur on a particular day. This parameter determines the probability that a nucleated particle will grow to a detectable size before being lost by coagulation with the pre-existing aerosol. Cluster-cluster coagulation was shown to contribute negligibly to this survival probability under conditions pertinent to the atmosphere. Data acquired during intensive measurement campaigns in Tecamac (MILAGRO), Atlanta (ANARChE), Boulder, and Hyytiälä (QUEST II, QUEST IV, and EUCAARI) were used to test the validity of LΓ as an NPF criterion. Measurements included aerosol size distributions down to 3 nm and gas-phase sulfuric acid concentrations. The model was applied to seventy-seven NPF events and nineteen non-events (characterized by growth of pre-existing aerosol without NPF) measured in diverse environments with broad ranges in sulfuric acid concentrations, ultrafine number concentrations, aerosol surface areas, and particle growth rates (nearly two orders of magnitude). Across this diverse data set, a nominal value of LΓ=0.7 was found to determine the boundary for the occurrence of NPF, with NPF occurring when LΓ<0.7 and being suppressed when LΓ>0.7. Moreover, nearly 45% of measured LΓ values associated with NPF fell in the relatively narrow range of 0.1<LΓ<0.3.

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