Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular Scale

Abstract A re-examination of measurements of heterogeneous nucleation of water vapor on silver nanoparticles is presented here using a model-free framework that derives the energy of critical cluster formation directly from measurements of nucleation probability. Temperature dependence is correlated...

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Main Authors: Robert L. McGraw, Paul M. Winkler, Paul E. Wagner
Format: Article
Language:English
Published: Nature Portfolio 2017-12-01
Series:Scientific Reports
Online Access:https://doi.org/10.1038/s41598-017-16692-9
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author Robert L. McGraw
Paul M. Winkler
Paul E. Wagner
author_facet Robert L. McGraw
Paul M. Winkler
Paul E. Wagner
author_sort Robert L. McGraw
collection DOAJ
description Abstract A re-examination of measurements of heterogeneous nucleation of water vapor on silver nanoparticles is presented here using a model-free framework that derives the energy of critical cluster formation directly from measurements of nucleation probability. Temperature dependence is correlated with cluster stabilization by the nanoparticle seed and previously found cases of unusual increasing nucleation onset saturation ratio with increasing temperature are explained. A necessary condition for the unusual positive temperature dependence is identified, namely that the critical cluster be more stable, on a per molecule basis, than the bulk liquid to exhibit the effect. Temperature dependence is next examined in the classical Fletcher model, modified here to make the energy of cluster formation explicit in the model.  The contact angle used in the Fletcher model is identified as the microscopic contact angle, which can be directly obtained from heterogeneous nucleation experimental data by a recently developed analysis method. Here an equivalent condition, increasing contact angle with temperature, is found necessary for occurrence of unusual temperature dependence. Our findings have immediate applications to atmospheric particle formation and nanoparticle detection in condensation particle counters (CPCs).
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spelling doaj.art-b6e50eecad364d91a76807abfebf984d2022-12-21T23:38:24ZengNature PortfolioScientific Reports2045-23222017-12-017111110.1038/s41598-017-16692-9Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular ScaleRobert L. McGraw0Paul M. Winkler1Paul E. Wagner2Environmental, and Climate Sciences Department, Brookhaven National LaboratoryUniversity of Vienna, Faculty of PhysicsUniversity of Vienna, Faculty of PhysicsAbstract A re-examination of measurements of heterogeneous nucleation of water vapor on silver nanoparticles is presented here using a model-free framework that derives the energy of critical cluster formation directly from measurements of nucleation probability. Temperature dependence is correlated with cluster stabilization by the nanoparticle seed and previously found cases of unusual increasing nucleation onset saturation ratio with increasing temperature are explained. A necessary condition for the unusual positive temperature dependence is identified, namely that the critical cluster be more stable, on a per molecule basis, than the bulk liquid to exhibit the effect. Temperature dependence is next examined in the classical Fletcher model, modified here to make the energy of cluster formation explicit in the model.  The contact angle used in the Fletcher model is identified as the microscopic contact angle, which can be directly obtained from heterogeneous nucleation experimental data by a recently developed analysis method. Here an equivalent condition, increasing contact angle with temperature, is found necessary for occurrence of unusual temperature dependence. Our findings have immediate applications to atmospheric particle formation and nanoparticle detection in condensation particle counters (CPCs).https://doi.org/10.1038/s41598-017-16692-9
spellingShingle Robert L. McGraw
Paul M. Winkler
Paul E. Wagner
Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular Scale
Scientific Reports
title Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular Scale
title_full Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular Scale
title_fullStr Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular Scale
title_full_unstemmed Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular Scale
title_short Temperature Dependence in Heterogeneous Nucleation with Application to the Direct Determination of Cluster Energy on Nearly Molecular Scale
title_sort temperature dependence in heterogeneous nucleation with application to the direct determination of cluster energy on nearly molecular scale
url https://doi.org/10.1038/s41598-017-16692-9
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