Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectrics

The morphology and adhesion energy of nanosized metal particles supported on dielectrics are a puzzling issue since, due to the increasing contribution of surfaces and interfaces in their energetics, their equilibrium shape escapes the rules established for large objects. The evolution of wetting du...

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Autores: Lazzari, R Rossi M A Saeta, Castilla Gómez, Manuel Sebastián|||0000-0002-8899-0525
Tipo de documento: artigo
Data de publicação:2020
País:España
Recursos:Universitat Politècnica de Catalunya (UPC)
Repositório:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglês
OAI Identifier:oai:upcommons.upc.edu:2117/360208
Acesso em linha:https://hdl.handle.net/2117/360208
https://dx.doi.org/10.1021/acsanm.0c02656
Access Level:Acceso aberto
Palavra-chave:Plasmonics
Metal nanoparticles
Adhesion
Metallic nanoparticles
Wulff-Kaischew-Winterbottom shape
Metal/dielectric
Growth
Differential reactivity
Truncated sphere and spheroid
Plasmons (Física)
Nanopartícules
Àrees temàtiques de la UPC::Física
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spelling Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectricsLazzari, R Rossi M A SaetaCastilla Gómez, Manuel Sebastián|||0000-0002-8899-0525PlasmonicsMetal nanoparticlesAdhesionPlasmonicsMetallic nanoparticlesWulff-Kaischew-Winterbottom shapeMetal/dielectricGrowthDifferential reactivityTruncated sphere and spheroidPlasmons (Física)NanopartículesÀrees temàtiques de la UPC::FísicaThe morphology and adhesion energy of nanosized metal particles supported on dielectrics are a puzzling issue since, due to the increasing contribution of surfaces and interfaces in their energetics, their equilibrium shape escapes the rules established for large objects. The evolution of wetting during Volmer–Weber growth of nanoparticles is herein studied by in situ ultraviolet/visible surface differential reflectivity spectroscopy (SDRS). The integrated s-polarized SDR signal is shown to be proportional to the oscillator strength of the optically excited plasmon resonances parallel to the surface. Dielectric modelings show that this quantity, which is marginally affected by the size and density of the objects, depends mainly on the aspect ratio of the particles from which adhesion energy can be derived. Applied to noble (Ag, Au) or transition metals (Cr, Ni) and Zn on weakly interacting dielectric (Al2O3, SiO2, KBr) and semiconducting (TiO2, ZnO) substrates, this plasmonic approach evidences a robust U-shaped variation of the aspect ratio with film thickness and therefore size. In line with the thorough study of the Ag/Al2O3(0001) growth and linear elasticity predictions of the equilibrium shape of strained epitaxial particles, the first branch of the “U” is assigned to a size-dependent equilibrium shape related to surface/interface stress effects. A significant decrease in adhesion energy parallels a rounding of the particles. The second branch partly stems from flattening due to incomplete coalescence. The common behavior of poorly wetting supported metal nanoparticles that is revealed herein, with strong changes in shape and adhesion as a function of particle size, had not been evidenced so far. Both the proposed optical methodology and the final findings about adhesion at the nanoscale are of interest in the wide field of application of supported metal nanoparticles that involves heterogeneous catalysis and thin film growth.We thank all reviewers for their very constructive comments. R.C., E.C., and Q.H. thank ANRT (Agence Nationale de la Recherche et de la Technologie), Arcelor-Mittal Maizières Research, and Saint-Gobain Recherche for the CIFRE funding of their thesis (grants 2013/0521 and 2016/0650). M.M. and E.M. acknowledge the support of the French state fund managed by the ANR (Agence Nationale de la Recherche) within the Investissements d’Avenir program under reference ANR-11-IDEX-0004-02 and more specifically within the framework of the Cluster of Excellence MATISSE. R.L., I.G., and Q.H. acknowledge the support of ANR (Industrial chair FRAXOS, reference ANR-15-CHIN-0003). The SDRS setup was designed by S. Chenot (INSP, Paris).Peer ReviewedAmerican Chemical Society20202020-12-2420222022-01-20journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/2117/360208https://dx.doi.org/10.1021/acsanm.0c02656reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution-NonCommercial-NoDerivs 3.0 Spainhttp://creativecommons.org/licenses/by-nc-nd/3.0/es/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/3602082026-05-27T15:37:01Z
dc.title.none.fl_str_mv Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectrics
title Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectrics
spellingShingle Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectrics
Lazzari, R Rossi M A Saeta
Plasmonics
Metal nanoparticles
Adhesion
Plasmonics
Metallic nanoparticles
Wulff-Kaischew-Winterbottom shape
Metal/dielectric
Growth
Differential reactivity
Truncated sphere and spheroid
Plasmons (Física)
Nanopartícules
Àrees temàtiques de la UPC::Física
title_short Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectrics
title_full Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectrics
title_fullStr Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectrics
title_full_unstemmed Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectrics
title_sort Plasmonics of supported nanoparticles reveals adhesion at the nanoscale: implications for metals on dielectrics
dc.creator.none.fl_str_mv Lazzari, R Rossi M A Saeta
Castilla Gómez, Manuel Sebastián|||0000-0002-8899-0525
author Lazzari, R Rossi M A Saeta
author_facet Lazzari, R Rossi M A Saeta
Castilla Gómez, Manuel Sebastián|||0000-0002-8899-0525
author_role author
author2 Castilla Gómez, Manuel Sebastián|||0000-0002-8899-0525
author2_role author
dc.subject.none.fl_str_mv Plasmonics
Metal nanoparticles
Adhesion
Plasmonics
Metallic nanoparticles
Wulff-Kaischew-Winterbottom shape
Metal/dielectric
Growth
Differential reactivity
Truncated sphere and spheroid
Plasmons (Física)
Nanopartícules
Àrees temàtiques de la UPC::Física
topic Plasmonics
Metal nanoparticles
Adhesion
Plasmonics
Metallic nanoparticles
Wulff-Kaischew-Winterbottom shape
Metal/dielectric
Growth
Differential reactivity
Truncated sphere and spheroid
Plasmons (Física)
Nanopartícules
Àrees temàtiques de la UPC::Física
description The morphology and adhesion energy of nanosized metal particles supported on dielectrics are a puzzling issue since, due to the increasing contribution of surfaces and interfaces in their energetics, their equilibrium shape escapes the rules established for large objects. The evolution of wetting during Volmer–Weber growth of nanoparticles is herein studied by in situ ultraviolet/visible surface differential reflectivity spectroscopy (SDRS). The integrated s-polarized SDR signal is shown to be proportional to the oscillator strength of the optically excited plasmon resonances parallel to the surface. Dielectric modelings show that this quantity, which is marginally affected by the size and density of the objects, depends mainly on the aspect ratio of the particles from which adhesion energy can be derived. Applied to noble (Ag, Au) or transition metals (Cr, Ni) and Zn on weakly interacting dielectric (Al2O3, SiO2, KBr) and semiconducting (TiO2, ZnO) substrates, this plasmonic approach evidences a robust U-shaped variation of the aspect ratio with film thickness and therefore size. In line with the thorough study of the Ag/Al2O3(0001) growth and linear elasticity predictions of the equilibrium shape of strained epitaxial particles, the first branch of the “U” is assigned to a size-dependent equilibrium shape related to surface/interface stress effects. A significant decrease in adhesion energy parallels a rounding of the particles. The second branch partly stems from flattening due to incomplete coalescence. The common behavior of poorly wetting supported metal nanoparticles that is revealed herein, with strong changes in shape and adhesion as a function of particle size, had not been evidenced so far. Both the proposed optical methodology and the final findings about adhesion at the nanoscale are of interest in the wide field of application of supported metal nanoparticles that involves heterogeneous catalysis and thin film growth.
publishDate 2020
dc.date.none.fl_str_mv 2020
2020-12-24
2022
2022-01-20
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/2117/360208
https://dx.doi.org/10.1021/acsanm.0c02656
url https://hdl.handle.net/2117/360208
https://dx.doi.org/10.1021/acsanm.0c02656
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution-NonCommercial-NoDerivs 3.0 Spain
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution-NonCommercial-NoDerivs 3.0 Spain
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:UPCommons. Portal del coneixement obert de la UPC
instname:Universitat Politècnica de Catalunya (UPC)
instname_str Universitat Politècnica de Catalunya (UPC)
reponame_str UPCommons. Portal del coneixement obert de la UPC
collection UPCommons. Portal del coneixement obert de la UPC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,301603

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