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Title: Communication. Kinetics of scavenging of small, nucleating clusters. First nucleation theorem and sum rules

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4905213· OSTI ID:1169565
 [1];  [2];  [1];  [1]
  1. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Biological, Environmental & Climate Sciences Dept.

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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
SC00112704
OSTI ID:
1169565
Alternate ID(s):
OSTI ID: 1228465
Report Number(s):
BNL-107379-2015-JA; JCPSA6; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000; TRN: US1500476
Journal Information:
Journal of Chemical Physics, Vol. 142, Issue 1; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science

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Cited By (5)