Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations

Among the numerous anomalies of water, the acceleration of dynamics under pressure is particularly puzzling. Whereas the diffusivity anomaly observed in experiments has been reproduced in several computer studies, the parallel viscosity anomaly has received less attention. Here we simulate viscosity...

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Detalles Bibliográficos
Autores: Montero De Hijes, Pablo, Sanz García, Eduardo Santiago, Joly, Laurent, Valeriani, Chantal, Caupin, Frederic
Tipo de recurso: artículo
Fecha de publicación:2018
País:España
Institución:Universidad Complutense de Madrid (UCM)
Repositorio:Docta Complutense
Idioma:inglés
OAI Identifier:oai:docta.ucm.es:20.500.14352/13080
Acceso en línea:https://hdl.handle.net/20.500.14352/13080
Access Level:acceso abierto
Palabra clave:539.1
Stokes-Einstein relation
Liquid water
Pressure-dependence
Density anomalies
Glass-transition
Relaxation
Model
Mobility
Temperature
Breakdown
Física nuclear
2207 Física Atómica y Nuclear
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oai_identifier_str oai:docta.ucm.es:20.500.14352/13080
network_acronym_str ES
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repository_id_str
spelling Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulationsMontero De Hijes, PabloSanz García, Eduardo SantiagoJoly, LaurentValeriani, ChantalCaupin, Frederic539.1Stokes-Einstein relationLiquid waterPressure-dependenceDensity anomaliesGlass-transitionRelaxationModelMobilityTemperatureBreakdownFísica nuclear2207 Física Atómica y NuclearAmong the numerous anomalies of water, the acceleration of dynamics under pressure is particularly puzzling. Whereas the diffusivity anomaly observed in experiments has been reproduced in several computer studies, the parallel viscosity anomaly has received less attention. Here we simulate viscosity and the self-diffusion coefficient of the TIP4P/2005 water model over a broad temperature and pressure range. We reproduce the experimental behavior and find additional anomalies at negative pressure. The anomalous effect of pressure on dynamic properties becomes more pronounced upon cooling, reaching two orders of magnitude for viscosity at 220 K. We analyze our results with a dynamic extension of a thermodynamic two-state model, an approach which has proved successful in describing experimental data. Water is regarded as a mixture of interconverting species with contrasting dynamic behaviors, one being strong (Arrhenius) and the other fragile (non-Arrhenius). The dynamic parameters of the two-state models are remarkably close between experiment and simulations. The larger pressure range accessible to simulations suggests a modification of the dynamic two-state model, which in turn also improves the agreement with experimental data. Furthermore, our simulations demonstrate the decoupling between viscosity eta and self-diffusion coefficient D as a function of temperature T. The Stokes-Einstein relation, which predicts a constant D eta/T, is violated when T is lowered, in connection with the Widom line defined by an equal fraction of the two interconverting species. These results provide a unifying picture of thermodynamics and dynamics in water and call for experiments at negative pressure. Published by AIP Publishing.Amer Inst PhysicsUniversidad Complutense de Madrid20182018-09-0720182018-09-07journal articlehttp://purl.org/coar/resource_type/c_6501info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/20.500.14352/13080reponame:Docta Complutenseinstname:Universidad Complutense de Madrid (UCM)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:docta.ucm.es:20.500.14352/130802026-06-02T12:44:21Z
dc.title.none.fl_str_mv Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations
title Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations
spellingShingle Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations
Montero De Hijes, Pablo
539.1
Stokes-Einstein relation
Liquid water
Pressure-dependence
Density anomalies
Glass-transition
Relaxation
Model
Mobility
Temperature
Breakdown
Física nuclear
2207 Física Atómica y Nuclear
title_short Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations
title_full Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations
title_fullStr Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations
title_full_unstemmed Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations
title_sort Viscosity and self-diffusion of supercooled and stretched water from molecular dynamics simulations
dc.creator.none.fl_str_mv Montero De Hijes, Pablo
Sanz García, Eduardo Santiago
Joly, Laurent
Valeriani, Chantal
Caupin, Frederic
author Montero De Hijes, Pablo
author_facet Montero De Hijes, Pablo
Sanz García, Eduardo Santiago
Joly, Laurent
Valeriani, Chantal
Caupin, Frederic
author_role author
author2 Sanz García, Eduardo Santiago
Joly, Laurent
Valeriani, Chantal
Caupin, Frederic
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Universidad Complutense de Madrid
dc.subject.none.fl_str_mv 539.1
Stokes-Einstein relation
Liquid water
Pressure-dependence
Density anomalies
Glass-transition
Relaxation
Model
Mobility
Temperature
Breakdown
Física nuclear
2207 Física Atómica y Nuclear
topic 539.1
Stokes-Einstein relation
Liquid water
Pressure-dependence
Density anomalies
Glass-transition
Relaxation
Model
Mobility
Temperature
Breakdown
Física nuclear
2207 Física Atómica y Nuclear
description Among the numerous anomalies of water, the acceleration of dynamics under pressure is particularly puzzling. Whereas the diffusivity anomaly observed in experiments has been reproduced in several computer studies, the parallel viscosity anomaly has received less attention. Here we simulate viscosity and the self-diffusion coefficient of the TIP4P/2005 water model over a broad temperature and pressure range. We reproduce the experimental behavior and find additional anomalies at negative pressure. The anomalous effect of pressure on dynamic properties becomes more pronounced upon cooling, reaching two orders of magnitude for viscosity at 220 K. We analyze our results with a dynamic extension of a thermodynamic two-state model, an approach which has proved successful in describing experimental data. Water is regarded as a mixture of interconverting species with contrasting dynamic behaviors, one being strong (Arrhenius) and the other fragile (non-Arrhenius). The dynamic parameters of the two-state models are remarkably close between experiment and simulations. The larger pressure range accessible to simulations suggests a modification of the dynamic two-state model, which in turn also improves the agreement with experimental data. Furthermore, our simulations demonstrate the decoupling between viscosity eta and self-diffusion coefficient D as a function of temperature T. The Stokes-Einstein relation, which predicts a constant D eta/T, is violated when T is lowered, in connection with the Widom line defined by an equal fraction of the two interconverting species. These results provide a unifying picture of thermodynamics and dynamics in water and call for experiments at negative pressure. Published by AIP Publishing.
publishDate 2018
dc.date.none.fl_str_mv 2018
2018-09-07
2018
2018-09-07
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/20.500.14352/13080
url https://hdl.handle.net/20.500.14352/13080
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
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
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Amer Inst Physics
publisher.none.fl_str_mv Amer Inst Physics
dc.source.none.fl_str_mv reponame:Docta Complutense
instname:Universidad Complutense de Madrid (UCM)
instname_str Universidad Complutense de Madrid (UCM)
reponame_str Docta Complutense
collection Docta Complutense
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869404684409634816
score 15.301603

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