Diffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquids
Autor(a) principal: | |
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Data de Publicação: | 2007 |
Outros Autores: | , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UFBA |
Texto Completo: | http://www.repositorio.ufba.br/ri/handle/ufba/580 |
Resumo: | We calculate, employing the classical theory of nucleation and growth, the effective diffusion coefficients controlling crystal nucleation of nano-size clusters and the subsequent growth of micron-size crystals at very deep undercoolings, below and above Tg, using experimental nucleation and growth data obtained for stoichiometric Li2O 2SiO2 and Na2O 2CaO 3SiO2 glasses. The results show significant differences in the magnitude and temperature dependence of these kinetic coefficients. We explain this difference showing that the composition and/or structure of the nucleating critical clusters deviate from those of the stable crystalline phase. These results for diffusion coefficients corroborate our previous conclusion for the same glasses, based on different experiments, and support the view that, even for the so-called case of stoichiometric (polymorphic) crystallization, the nucleating phase may have a different composition and/or structure as compared to the parent glass and the evolving macroscopic crystalline phase. This finding gives a key to explain the discrepancies between calculated (by Classical Nucleation Theory) and experimentally observed nucleation rates in these systems, in particular, and in deeply undercooled glass-forming liquids, in general. |
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Fokin, Vladimir MihailovichSchmelzer, Jurn Williard P.Nascimento, Marcio Luis FerreiraZanotto, Edgar DutraFokin, Vladimir MihailovichSchmelzer, Jurn Williard P.Nascimento, Marcio Luis FerreiraZanotto, Edgar Dutra2010-11-10T19:35:09Z2010-11-10T19:35:09Z2007-01-0100219606http://www.repositorio.ufba.br/ri/handle/ufba/580Journal of Chemical Physics, v. 126, p. 234507We calculate, employing the classical theory of nucleation and growth, the effective diffusion coefficients controlling crystal nucleation of nano-size clusters and the subsequent growth of micron-size crystals at very deep undercoolings, below and above Tg, using experimental nucleation and growth data obtained for stoichiometric Li2O 2SiO2 and Na2O 2CaO 3SiO2 glasses. The results show significant differences in the magnitude and temperature dependence of these kinetic coefficients. We explain this difference showing that the composition and/or structure of the nucleating critical clusters deviate from those of the stable crystalline phase. These results for diffusion coefficients corroborate our previous conclusion for the same glasses, based on different experiments, and support the view that, even for the so-called case of stoichiometric (polymorphic) crystallization, the nucleating phase may have a different composition and/or structure as compared to the parent glass and the evolving macroscopic crystalline phase. This finding gives a key to explain the discrepancies between calculated (by Classical Nucleation Theory) and experimentally observed nucleation rates in these systems, in particular, and in deeply undercooled glass-forming liquids, in general.Submitted by Marcio Luis Ferreira Nascimento (mlfn@ufba.br) on 2010-11-10T19:35:09Z No. of bitstreams: 1 DiffusionCoefficientsNucleationGrowth-JCP126-Nascimento.pdf: 113732 bytes, checksum: b5e8f91d99fa6a0f0f7840c5bbf6dc33 (MD5)Made available in DSpace on 2010-11-10T19:35:09Z (GMT). No. of bitstreams: 1 DiffusionCoefficientsNucleationGrowth-JCP126-Nascimento.pdf: 113732 bytes, checksum: b5e8f91d99fa6a0f0f7840c5bbf6dc33 (MD5) Previous issue date: 2007-01-01Estados UnidosVidroCristalizaçãoCrescimento de CristaisVogel-Fulcher-Tammann-HesseViscosidadeNucleaçãoDiffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquidsArtigo de Periódicoinfo:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionengreponame:Repositório Institucional da UFBAinstname:Universidade Federal da Bahia (UFBA)instacron:UFBAinfo:eu-repo/semantics/openAccessORIGINALDiffusionCoefficientsNucleationGrowth-JCP126-Nascimento.pdfDiffusionCoefficientsNucleationGrowth-JCP126-Nascimento.pdfapplication/pdf113732https://repositorio.ufba.br/bitstream/ufba/580/1/DiffusionCoefficientsNucleationGrowth-JCP126-Nascimento.pdfb5e8f91d99fa6a0f0f7840c5bbf6dc33MD51LICENSElicense.txtlicense.txttext/plain1908https://repositorio.ufba.br/bitstream/ufba/580/2/license.txta39e1e35e4baad82fe5647d3bd66c139MD52TEXTDiffusionCoefficientsNucleationGrowth-JCP126-Nascimento.pdf.txtDiffusionCoefficientsNucleationGrowth-JCP126-Nascimento.pdf.txtExtracted texttext/plain27831https://repositorio.ufba.br/bitstream/ufba/580/3/DiffusionCoefficientsNucleationGrowth-JCP126-Nascimento.pdf.txta090865546c797558c5a2b8a3692cda0MD53ufba/5802022-08-26 11:47:06.323oai:repositorio.ufba.br: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ório InstitucionalPUBhttp://192.188.11.11:8080/oai/requestopendoar:19322022-08-26T14:47:06Repositório Institucional da UFBA - Universidade Federal da Bahia (UFBA)false |
dc.title.en.fl_str_mv |
Diffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquids |
title |
Diffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquids |
spellingShingle |
Diffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquids Fokin, Vladimir Mihailovich Vidro Cristalização Crescimento de Cristais Vogel-Fulcher-Tammann-Hesse Viscosidade Nucleação |
title_short |
Diffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquids |
title_full |
Diffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquids |
title_fullStr |
Diffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquids |
title_full_unstemmed |
Diffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquids |
title_sort |
Diffusion coefficients for crystal nucleation and growth in deeply undercooled glass-forming liquids |
author |
Fokin, Vladimir Mihailovich |
author_facet |
Fokin, Vladimir Mihailovich Schmelzer, Jurn Williard P. Nascimento, Marcio Luis Ferreira Zanotto, Edgar Dutra |
author_role |
author |
author2 |
Schmelzer, Jurn Williard P. Nascimento, Marcio Luis Ferreira Zanotto, Edgar Dutra |
author2_role |
author author author |
dc.contributor.author.fl_str_mv |
Fokin, Vladimir Mihailovich Schmelzer, Jurn Williard P. Nascimento, Marcio Luis Ferreira Zanotto, Edgar Dutra Fokin, Vladimir Mihailovich Schmelzer, Jurn Williard P. Nascimento, Marcio Luis Ferreira Zanotto, Edgar Dutra |
dc.subject.eng.fl_str_mv |
Vidro Cristalização Crescimento de Cristais Vogel-Fulcher-Tammann-Hesse Viscosidade Nucleação |
topic |
Vidro Cristalização Crescimento de Cristais Vogel-Fulcher-Tammann-Hesse Viscosidade Nucleação |
description |
We calculate, employing the classical theory of nucleation and growth, the effective diffusion coefficients controlling crystal nucleation of nano-size clusters and the subsequent growth of micron-size crystals at very deep undercoolings, below and above Tg, using experimental nucleation and growth data obtained for stoichiometric Li2O 2SiO2 and Na2O 2CaO 3SiO2 glasses. The results show significant differences in the magnitude and temperature dependence of these kinetic coefficients. We explain this difference showing that the composition and/or structure of the nucleating critical clusters deviate from those of the stable crystalline phase. These results for diffusion coefficients corroborate our previous conclusion for the same glasses, based on different experiments, and support the view that, even for the so-called case of stoichiometric (polymorphic) crystallization, the nucleating phase may have a different composition and/or structure as compared to the parent glass and the evolving macroscopic crystalline phase. This finding gives a key to explain the discrepancies between calculated (by Classical Nucleation Theory) and experimentally observed nucleation rates in these systems, in particular, and in deeply undercooled glass-forming liquids, in general. |
publishDate |
2007 |
dc.date.issued.fl_str_mv |
2007-01-01 |
dc.date.accessioned.fl_str_mv |
2010-11-10T19:35:09Z |
dc.date.available.fl_str_mv |
2010-11-10T19:35:09Z |
dc.type.driver.fl_str_mv |
Artigo de Periódico info:eu-repo/semantics/article |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://www.repositorio.ufba.br/ri/handle/ufba/580 |
dc.identifier.issn.none.fl_str_mv |
00219606 |
dc.identifier.number.en.fl_str_mv |
Journal of Chemical Physics, v. 126, p. 234507 |
identifier_str_mv |
00219606 Journal of Chemical Physics, v. 126, p. 234507 |
url |
http://www.repositorio.ufba.br/ri/handle/ufba/580 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
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openAccess |
dc.source.none.fl_str_mv |
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Repositório Institucional da UFBA |
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Repositório Institucional da UFBA |
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