A robust comparison of dynamical scenarios in a glass-forming liquid

We use Bayesian inference methods to provide fresh insights into the sub-nanosecond dynamics of glycerol, a prototypical glass-forming liquid. To this end, quasielastic neutron scattering data as a function of temperature have been analyzed using a minimal set of underlying physical assumptions. On...

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Detalles Bibliográficos
Autores: Vispa, Alessandro, Busch, Sebastian, Tamarit Mur, José Luis|||0000-0002-7965-0000, Unruh, Tobias, Fernandez-Alonso, Felix, Pardo Soto, Luis Carlos|||0000-0002-2768-0013
Tipo de recurso: artículo
Fecha de publicación:2016
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:2117/103625
Acceso en línea:https://hdl.handle.net/2117/103625
https://dx.doi.org/10.1039/c5cp05143f
Access Level:acceso abierto
Palabra clave:Chemistry, Physical and theoretical
Secondary relaxations
Nuetron-scattering
Light-scattering
Viscous liquids
Glycerol
Diffusion
Trnasition
Spectroscopy
Crossover
Fisicoquímica
Àrees temàtiques de la UPC::Enginyeria química::Química física
Descripción
Sumario:We use Bayesian inference methods to provide fresh insights into the sub-nanosecond dynamics of glycerol, a prototypical glass-forming liquid. To this end, quasielastic neutron scattering data as a function of temperature have been analyzed using a minimal set of underlying physical assumptions. On the basis of this analysis, we establish the unambiguous presence of three distinct dynamical processes in glycerol, namely, translational diffusion of the molecular centre of mass and two additional localized and temperature-independent modes. The neutron data also provide access to the characteristic length scales associated with these motions in a model-independent manner, from which we conclude that the faster (slower) localized motions probe longer (shorter) length scales. Careful Bayesian analysis of the entire scattering law favors a heterogeneous scenario for the microscopic dynamics of glycerol, where molecules undergo either the faster and longer or the slower and shorter localized motions.