Tracer Transport Probes Relaxation and Structure of Attractive and Repulsive Glassy Liquids

The Journal of Physical Chemistry Letters
Ryan C RobertsJacinta C Conrad

Abstract

Dynamic coupling of small penetrants to slow, cooperative relaxations within crowded cells, supercooled liquids, and polymer matrices has broad consequences for applications ranging from drug delivery to nanocomposite processing. Interactions between the constituents of these and other disordered media alter the cooperative relaxations, but their effect on penetrant dynamics remains incompletely understood. We use molecular dynamics simulations to show that the motions of hard-sphere tracer particles probe differences in local structure and cooperative relaxation processes in attractive and repulsive glassy liquid matrices with equal bulk packing fractions and long-time diffusivities. Coupling of the tracer dynamics to collective relaxations in each matrix affects the shape of tracer trajectories, which are fractal within the repulsive matrix and more compact in the attractive. These results reveal that the structure of relaxations controls penetrant transport and dispersion in cooperatively relaxing systems and provide insight into dynamical heterogeneity within glassy liquids.

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Citations

Apr 15, 2020·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Elias M ZirdehiFathollah Varnik
Nov 24, 2019·The Journal of Chemical Physics·Ryan C RobertsJeremy C Palmer
Mar 28, 2019·The Journal of Physical Chemistry Letters·Ryan Poling-SkutvikJacinta C Conrad
Apr 9, 2019·Langmuir : the ACS Journal of Surfaces and Colloids·Ruben HiglerJoris Sprakel

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