Communication. Kinetics of scavenging of small, nucleating clusters. First nucleation theorem and sum rules
Abstract
Despite recent advances in monitoring nucleation from a vapor at close-to-molecular resolution, the identity of the critical cluster, forming the bottleneck for the nucleation process, remains elusive. During past twenty years, the first nucleation theorem has been often used to extract the size of the critical cluster from nucleation rate measurements. However, derivations of the first nucleation theorem invoke certain questionable assumptions that may fail, e.g., in the case of atmospheric new particle formation, including absence of subcritical cluster losses and heterogeneous nucleation on pre-existing nanoparticles. Here we extend the kinetic derivation of the first nucleation theorem to give a general framework to include such processes, yielding sum rules connecting the size dependent particle formation and loss rates to the corresponding loss-free nucleation rate and the apparent critical size from a naïve application of the first nucleation theorem that neglects them.
- Authors:
-
- Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
- Brookhaven National Lab. (BNL), Upton, NY (United States). Biological, Environmental & Climate Sciences Dept.
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1169565
- Alternate Identifier(s):
- OSTI ID: 1228465
- Report Number(s):
- BNL-107379-2015-JA
Journal ID: ISSN 0021-9606; JCPSA6; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000; TRN: US1500476
- Grant/Contract Number:
- SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 142; Journal Issue: 1; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; nucleation; kinetic nucleation theorems; law of mass action; atmospheric new particle formation
Citation Formats
Malila, Jussi, McGraw, Robert, Laaksonen, Ari, and Lehtinen, Kari E. J. Communication. Kinetics of scavenging of small, nucleating clusters. First nucleation theorem and sum rules. United States: N. p., 2015.
Web. doi:10.1063/1.4905213.
Malila, Jussi, McGraw, Robert, Laaksonen, Ari, & Lehtinen, Kari E. J. Communication. Kinetics of scavenging of small, nucleating clusters. First nucleation theorem and sum rules. United States. https://doi.org/10.1063/1.4905213
Malila, Jussi, McGraw, Robert, Laaksonen, Ari, and Lehtinen, Kari E. J. Wed .
"Communication. Kinetics of scavenging of small, nucleating clusters. First nucleation theorem and sum rules". United States. https://doi.org/10.1063/1.4905213. https://www.osti.gov/servlets/purl/1169565.
@article{osti_1169565,
title = {Communication. Kinetics of scavenging of small, nucleating clusters. First nucleation theorem and sum rules},
author = {Malila, Jussi and McGraw, Robert and Laaksonen, Ari and Lehtinen, Kari E. J.},
abstractNote = {Despite recent advances in monitoring nucleation from a vapor at close-to-molecular resolution, the identity of the critical cluster, forming the bottleneck for the nucleation process, remains elusive. During past twenty years, the first nucleation theorem has been often used to extract the size of the critical cluster from nucleation rate measurements. However, derivations of the first nucleation theorem invoke certain questionable assumptions that may fail, e.g., in the case of atmospheric new particle formation, including absence of subcritical cluster losses and heterogeneous nucleation on pre-existing nanoparticles. Here we extend the kinetic derivation of the first nucleation theorem to give a general framework to include such processes, yielding sum rules connecting the size dependent particle formation and loss rates to the corresponding loss-free nucleation rate and the apparent critical size from a naïve application of the first nucleation theorem that neglects them.},
doi = {10.1063/1.4905213},
journal = {Journal of Chemical Physics},
number = 1,
volume = 142,
place = {United States},
year = {Wed Jan 07 00:00:00 EST 2015},
month = {Wed Jan 07 00:00:00 EST 2015}
}
Web of Science
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Works referencing / citing this record:
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