Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble

Autores
Balbuena, Cristian; Gianetti, Melisa Mariel; Soulé, Ezequiel Rodolfo
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The dynamic correlations that emerge in a polymer system in supercooling conditions have been studied using molecular dynamic simulations. It is known that when a glass former approaches the glass transition temperature, the dynamics of the system (in terms of the mobilities of the particles) not only significantly slows down but also becomes more heterogeneous. Several theories relate this slowing down to increasing spatial (structural) correlations, for example, through the onset of cooperative relaxation regions in the Adam-Gibbs theory. In this work, we employ Pearson’s coefficient in the isoconfigurational ensemble (ICE) which allows us to study the dynamic correlations of the monomers in the ICE and establish the relation between the structure of the monomers and its dynamic behavior. Similar to what happens with mobility, monomers with highest correlation are clustered, and the clustering increases with decreasing temperature. An interesting result is that regions with high ICE dynamic correlation are not coincident with highly mobile or immobile regions. These results represent a new approach to the study of dynamic heterogeneity that emerges in glass forming liquids, complementing the more traditional characterization in terms of mobility. The methodology proposed in this work that characterize the connected dynamic regions to structural causes can represent an alternative way to observe the cooperative relaxation regions.
Fil: Balbuena, Cristian. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina
Fil: Gianetti, Melisa Mariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina
Fil: Soulé, Ezequiel Rodolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina
Materia
Supercooled
Isoconfigurational ensemble
Dynamical heterogeneity
Dynamic correlation
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/82182
Acceder
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spelling Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensembleBalbuena, CristianGianetti, Melisa MarielSoulé, Ezequiel RodolfoSupercooledIsoconfigurational ensembleDynamical heterogeneityDynamic correlationhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1https://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2The dynamic correlations that emerge in a polymer system in supercooling conditions have been studied using molecular dynamic simulations. It is known that when a glass former approaches the glass transition temperature, the dynamics of the system (in terms of the mobilities of the particles) not only significantly slows down but also becomes more heterogeneous. Several theories relate this slowing down to increasing spatial (structural) correlations, for example, through the onset of cooperative relaxation regions in the Adam-Gibbs theory. In this work, we employ Pearson’s coefficient in the isoconfigurational ensemble (ICE) which allows us to study the dynamic correlations of the monomers in the ICE and establish the relation between the structure of the monomers and its dynamic behavior. Similar to what happens with mobility, monomers with highest correlation are clustered, and the clustering increases with decreasing temperature. An interesting result is that regions with high ICE dynamic correlation are not coincident with highly mobile or immobile regions. These results represent a new approach to the study of dynamic heterogeneity that emerges in glass forming liquids, complementing the more traditional characterization in terms of mobility. The methodology proposed in this work that characterize the connected dynamic regions to structural causes can represent an alternative way to observe the cooperative relaxation regions.Fil: Balbuena, Cristian. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; ArgentinaFil: Gianetti, Melisa Mariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; ArgentinaFil: Soulé, Ezequiel Rodolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; ArgentinaAmerican Institute of Physics2018-09info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/82182Balbuena, Cristian; Gianetti, Melisa Mariel; Soulé, Ezequiel Rodolfo; Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble; American Institute of Physics; Journal of Chemical Physics; 149; 9; 9-2018; 1-9; 0945060021-9606CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1063/1.5039644info:eu-repo/semantics/altIdentifier/url/https://aip.scitation.org/doi/10.1063/1.5039644info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T12:05:25Zoai:ri.conicet.gov.ar:11336/82182instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-10-22 12:05:25.666CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble
title Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble
spellingShingle Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble
Balbuena, Cristian
Supercooled
Isoconfigurational ensemble
Dynamical heterogeneity
Dynamic correlation
title_short Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble
title_full Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble
title_fullStr Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble
title_full_unstemmed Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble
title_sort Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble
dc.creator.none.fl_str_mv Balbuena, Cristian
Gianetti, Melisa Mariel
Soulé, Ezequiel Rodolfo
author Balbuena, Cristian
author_facet Balbuena, Cristian
Gianetti, Melisa Mariel
Soulé, Ezequiel Rodolfo
author_role author
author2 Gianetti, Melisa Mariel
Soulé, Ezequiel Rodolfo
author2_role author
author
dc.subject.none.fl_str_mv Supercooled
Isoconfigurational ensemble
Dynamical heterogeneity
Dynamic correlation
topic Supercooled
Isoconfigurational ensemble
Dynamical heterogeneity
Dynamic correlation
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv The dynamic correlations that emerge in a polymer system in supercooling conditions have been studied using molecular dynamic simulations. It is known that when a glass former approaches the glass transition temperature, the dynamics of the system (in terms of the mobilities of the particles) not only significantly slows down but also becomes more heterogeneous. Several theories relate this slowing down to increasing spatial (structural) correlations, for example, through the onset of cooperative relaxation regions in the Adam-Gibbs theory. In this work, we employ Pearson’s coefficient in the isoconfigurational ensemble (ICE) which allows us to study the dynamic correlations of the monomers in the ICE and establish the relation between the structure of the monomers and its dynamic behavior. Similar to what happens with mobility, monomers with highest correlation are clustered, and the clustering increases with decreasing temperature. An interesting result is that regions with high ICE dynamic correlation are not coincident with highly mobile or immobile regions. These results represent a new approach to the study of dynamic heterogeneity that emerges in glass forming liquids, complementing the more traditional characterization in terms of mobility. The methodology proposed in this work that characterize the connected dynamic regions to structural causes can represent an alternative way to observe the cooperative relaxation regions.
Fil: Balbuena, Cristian. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina
Fil: Gianetti, Melisa Mariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina
Fil: Soulé, Ezequiel Rodolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina
description The dynamic correlations that emerge in a polymer system in supercooling conditions have been studied using molecular dynamic simulations. It is known that when a glass former approaches the glass transition temperature, the dynamics of the system (in terms of the mobilities of the particles) not only significantly slows down but also becomes more heterogeneous. Several theories relate this slowing down to increasing spatial (structural) correlations, for example, through the onset of cooperative relaxation regions in the Adam-Gibbs theory. In this work, we employ Pearson’s coefficient in the isoconfigurational ensemble (ICE) which allows us to study the dynamic correlations of the monomers in the ICE and establish the relation between the structure of the monomers and its dynamic behavior. Similar to what happens with mobility, monomers with highest correlation are clustered, and the clustering increases with decreasing temperature. An interesting result is that regions with high ICE dynamic correlation are not coincident with highly mobile or immobile regions. These results represent a new approach to the study of dynamic heterogeneity that emerges in glass forming liquids, complementing the more traditional characterization in terms of mobility. The methodology proposed in this work that characterize the connected dynamic regions to structural causes can represent an alternative way to observe the cooperative relaxation regions.
publishDate 2018
dc.date.none.fl_str_mv 2018-09
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/82182
Balbuena, Cristian; Gianetti, Melisa Mariel; Soulé, Ezequiel Rodolfo; Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble; American Institute of Physics; Journal of Chemical Physics; 149; 9; 9-2018; 1-9; 094506
0021-9606
CONICET Digital
CONICET
url http://hdl.handle.net/11336/82182
identifier_str_mv Balbuena, Cristian; Gianetti, Melisa Mariel; Soulé, Ezequiel Rodolfo; Looking at the dynamical heterogeneity in a supercooled polymer system through isoconfigurational ensemble; American Institute of Physics; Journal of Chemical Physics; 149; 9; 9-2018; 1-9; 094506
0021-9606
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1063/1.5039644
info:eu-repo/semantics/altIdentifier/url/https://aip.scitation.org/doi/10.1063/1.5039644
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Institute of Physics
publisher.none.fl_str_mv American Institute of Physics
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 12.982451

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