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

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.
 [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.
Publication Date:
OSTI Identifier:
Report Number(s):
Journal ID: ISSN 0021-9606; JCPSA6; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000; TRN: US1500476
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 142; Journal Issue: 1; Journal ID: ISSN 0021-9606
American Institute of Physics (AIP)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
54 ENVIRONMENTAL SCIENCES nucleation; kinetic nucleation theorems; law of mass action; atmospheric new particle formation