Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystals

Bottom-up and top-down derived nanoparticle structures refined by accurate ab initio calculations are used to investigate the size dependent emergence of crystallinity in titania from the monomer upwards. Global optimisation and data mining are used to provide a series of ( TiO2) N global minima can...

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Autores: Lamiel Garcia, Josep Oriol, Cuko, Andi, Calatayud, Mònica, Illas i Riera, Francesc, Bromley, Stefan Thomas
Tipo de documento: artigo
Estado:Versão publicada
Data de publicação:2017
País:España
Recursos:Universidad de Barcelona
Repositório:Dipòsit Digital de la UB
OAI Identifier:oai:diposit.ub.edu:2445/118828
Acesso em linha:https://hdl.handle.net/2445/118828
Access Level:Acceso aberto
Palavra-chave:Diòxid de titani
Nanopartícules
Nanocristalls semiconductors
Nanoestructures
Titanium dioxide
Nanoparticles
Semiconductor nanocrystals
Nanostructures
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spelling Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystalsLamiel Garcia, Josep OriolCuko, AndiCalatayud, MònicaIllas i Riera, FrancescBromley, Stefan ThomasDiòxid de titaniNanopartículesNanocristalls semiconductorsNanoestructuresTitanium dioxideNanoparticlesSemiconductor nanocrystalsNanostructuresBottom-up and top-down derived nanoparticle structures refined by accurate ab initio calculations are used to investigate the size dependent emergence of crystallinity in titania from the monomer upwards. Global optimisation and data mining are used to provide a series of ( TiO2) N global minima candidates in the range N = 1-38, where our approach provides many new low energy structures for N > 10. A range of nanocrystal cuts from the anatase crystal structure are also considered up to a size of over 250 atoms. All nanocrystals considered are predicted to be metastable with respect to non-crystalline nanoclusters, which has implications with respect to the limitations of the cluster approach to modelling large titania nanosystems. Extrapolating both data sets using a generalised expansion of a top-down derived energy expression for nanoparticles, we obtain an estimate of the non-crystalline to crystalline crossover size for titania. Our results compare well with the available experimental results and imply that anatase-like crystallinity emerges in titania nanoparticles of approximately 2-3 nm diameter.Royal Society of Chemistry2017info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttps://hdl.handle.net/2445/118828Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaInglésReproducció del document publicat a: https://doi.org/10.1039/c6nr05788hNanoscale, 2017, vol. 9, num. 3, p. 1049-1058https://doi.org/10.1039/c6nr05788hinfo:eu-repo/grantAgreement/EC/H2020/676580info:eu-repo/grantAgreement/EC/H2020/642294cc-by (c) Lamiel-Garcia, Oriol et al., 2017http://creativecommons.org/licenses/by/3.0/esinfo:eu-repo/semantics/openAccessoai:diposit.ub.edu:2445/1188282026-05-27T06:46:51Z
dc.title.none.fl_str_mv Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystals
title Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystals
spellingShingle Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystals
Lamiel Garcia, Josep Oriol
Diòxid de titani
Nanopartícules
Nanocristalls semiconductors
Nanoestructures
Titanium dioxide
Nanoparticles
Semiconductor nanocrystals
Nanostructures
title_short Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystals
title_full Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystals
title_fullStr Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystals
title_full_unstemmed Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystals
title_sort Predicting size-dependent emergence of crystallinity in nanomaterials: titania nanoclusters versus nanocrystals
dc.creator.none.fl_str_mv Lamiel Garcia, Josep Oriol
Cuko, Andi
Calatayud, Mònica
Illas i Riera, Francesc
Bromley, Stefan Thomas
author Lamiel Garcia, Josep Oriol
author_facet Lamiel Garcia, Josep Oriol
Cuko, Andi
Calatayud, Mònica
Illas i Riera, Francesc
Bromley, Stefan Thomas
author_role author
author2 Cuko, Andi
Calatayud, Mònica
Illas i Riera, Francesc
Bromley, Stefan Thomas
author2_role author
author
author
author
dc.subject.none.fl_str_mv Diòxid de titani
Nanopartícules
Nanocristalls semiconductors
Nanoestructures
Titanium dioxide
Nanoparticles
Semiconductor nanocrystals
Nanostructures
topic Diòxid de titani
Nanopartícules
Nanocristalls semiconductors
Nanoestructures
Titanium dioxide
Nanoparticles
Semiconductor nanocrystals
Nanostructures
description Bottom-up and top-down derived nanoparticle structures refined by accurate ab initio calculations are used to investigate the size dependent emergence of crystallinity in titania from the monomer upwards. Global optimisation and data mining are used to provide a series of ( TiO2) N global minima candidates in the range N = 1-38, where our approach provides many new low energy structures for N > 10. A range of nanocrystal cuts from the anatase crystal structure are also considered up to a size of over 250 atoms. All nanocrystals considered are predicted to be metastable with respect to non-crystalline nanoclusters, which has implications with respect to the limitations of the cluster approach to modelling large titania nanosystems. Extrapolating both data sets using a generalised expansion of a top-down derived energy expression for nanoparticles, we obtain an estimate of the non-crystalline to crystalline crossover size for titania. Our results compare well with the available experimental results and imply that anatase-like crystallinity emerges in titania nanoparticles of approximately 2-3 nm diameter.
publishDate 2017
dc.date.none.fl_str_mv 2017
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/118828
url https://hdl.handle.net/2445/118828
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció del document publicat a: https://doi.org/10.1039/c6nr05788h
Nanoscale, 2017, vol. 9, num. 3, p. 1049-1058
https://doi.org/10.1039/c6nr05788h
info:eu-repo/grantAgreement/EC/H2020/676580
info:eu-repo/grantAgreement/EC/H2020/642294
dc.rights.none.fl_str_mv cc-by (c) Lamiel-Garcia, Oriol et al., 2017
http://creativecommons.org/licenses/by/3.0/es
info:eu-repo/semantics/openAccess
rights_invalid_str_mv cc-by (c) Lamiel-Garcia, Oriol et al., 2017
http://creativecommons.org/licenses/by/3.0/es
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Dipòsit Digital de la UB
instname:Universidad de Barcelona
instname_str Universidad de Barcelona
reponame_str Dipòsit Digital de la UB
collection Dipòsit Digital de la UB
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,301603

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