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...
Main Authors: | , , |
---|---|
Format: | Article |
Language: | English |
Published: |
Nature Portfolio
2017-12-01
|
Series: | Scientific Reports |
Online Access: | https://doi.org/10.1038/s41598-017-16692-9 |
_version_ | 1818343789165543424 |
---|---|
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). |
first_indexed | 2024-12-13T16:36:10Z |
format | Article |
id | doaj.art-b6e50eecad364d91a76807abfebf984d |
institution | Directory Open Access Journal |
issn | 2045-2322 |
language | English |
last_indexed | 2024-12-13T16:36:10Z |
publishDate | 2017-12-01 |
publisher | Nature Portfolio |
record_format | Article |
series | Scientific Reports |
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 |
work_keys_str_mv | AT robertlmcgraw temperaturedependenceinheterogeneousnucleationwithapplicationtothedirectdeterminationofclusterenergyonnearlymolecularscale AT paulmwinkler temperaturedependenceinheterogeneousnucleationwithapplicationtothedirectdeterminationofclusterenergyonnearlymolecularscale AT paulewagner temperaturedependenceinheterogeneousnucleationwithapplicationtothedirectdeterminationofclusterenergyonnearlymolecularscale |