Translational versus rotational energy flow in water solvation dynamics

Early molecular dynamics simulations discovered an important asymmetry in the speed of water solvation dynamics for charge extinction and charge creation for an immersed solute, a feature representing a first demonstration of the breakdown of linear response theory. The molecular level mechanism of...

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Detalles Bibliográficos
Autores: Rey Oriol, Rosendo|||0000-0002-3586-4568, Hynes, James T.
Tipo de recurso: artículo
Fecha de publicación:2017
País:España
Institución:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/107837
Acceso en línea:https://hdl.handle.net/2117/107837
https://dx.doi.org/10.1016/j.cplett.2017.02.064
Access Level:acceso abierto
Palabra clave:Molecular dynamics
Water solvation dynamics
Dinàmica molecular
Àrees temàtiques de la UPC::Física::Física de fluids
Descripción
Sumario:Early molecular dynamics simulations discovered an important asymmetry in the speed of water solvation dynamics for charge extinction and charge creation for an immersed solute, a feature representing a first demonstration of the breakdown of linear response theory. The molecular level mechanism of this asymmetry is examined here via a novel energy flux theoretical approach coupled to geometric probes. The results identify the effect as arising from the translational motions of the solute-hydrating water molecules rather than their rotational/librational motions, even though the latter are more rapid and dominate the energy flow.