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dc.contributor.author
Gianetti, Melisa Mariel
dc.contributor.author
Haji Akbari, Amir
dc.contributor.author
Longinotti, María Paula
dc.contributor.author
Debenedetti, Pablo Gastón
dc.date.available
2018-09-10T21:13:28Z
dc.date.issued
2016-01
dc.identifier.citation
Gianetti, Melisa Mariel; Haji Akbari, Amir; Longinotti, María Paula; Debenedetti, Pablo Gastón; Computational investigation of structure, dynamics and nucleation kinetics of a family of modified Stillinger-Weber model fluids in bulk and free-standing thin films; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 18; 5; 1-2016; 4102-4111
dc.identifier.issn
1463-9076
dc.identifier.uri
http://hdl.handle.net/11336/58995
dc.description.abstract
In recent years, computer simulations have found increasingly widespread use as powerful tools for studying phase transitions in wide variety of systems. In the particular and very important case of aqueous systems, the commonly used force-fields tend to offer quite different predictions with respect to a wide range of thermodynamic and kinetic properties, including the ease of ice nucleation, the propensity to freeze at a vapor-liquid interface, and the existence of a liquid-liquid phase transition. It is thus of fundamental and practical interest to understand how different features of a given water model affect its thermodynamic and kinetic properties. In this work, we use the forward-flux sampling technique to study the crystallization kinetics of a family of modified Stillinger-Weber (SW) potentials with energy (ε) and length (σ) scales taken from the monoatomic water (mW) model, but with different tetrahedrality parameters (λ). By increasing λ from 21 to 24, we observe the nucleation rate increases by 48 orders of magnitude at a supercooling of ζ = T/Tm = 0.845. Using classical nucleation theory, we are able to demonstrate that this change can largely be accounted for by the increase in Δμ, the thermodynamic driving force. We also perform rate calculations in freestanding thin films of the supercooled liquid, and observe a crossover from surface-enhanced crystallization at λ = 21 to bulk-dominated crystallization for λ ≥ 22.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
Royal Society of Chemistry
dc.rights
info:eu-repo/semantics/openAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
Nucleation
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Ice
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Forward Flux Sampling
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Simulations
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Otras Ciencias Químicas
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Ciencias Químicas
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CIENCIAS NATURALES Y EXACTAS
dc.title
Computational investigation of structure, dynamics and nucleation kinetics of a family of modified Stillinger-Weber model fluids in bulk and free-standing thin films
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2018-09-04T19:06:19Z
dc.journal.volume
18
dc.journal.number
5
dc.journal.pagination
4102-4111
dc.journal.pais
Reino Unido
dc.journal.ciudad
Cambridge
dc.description.fil
Fil: Gianetti, Melisa Mariel. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
dc.description.fil
Fil: Haji Akbari, Amir. University of Princeton; Estados Unidos
dc.description.fil
Fil: Longinotti, María Paula. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
dc.description.fil
Fil: Debenedetti, Pablo Gastón. University of Princeton; Estados Unidos
dc.journal.title
Physical Chemistry Chemical Physics
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/https://dx.doi.org/10.1039/c5cp06535f
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/http://pubs.rsc.org/en/Content/ArticleLanding/2016/CP/C5CP06535F
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