Elastically Cooperative Activated Hopping Theory of Relaxation in Viscous Liquids. I. General Formulation and Application to Hard Sphere Fluids.

Mirigian, Stephen; Schweizer, Kenneth

doi:10.1063/1.4874842

Title: Elastically Cooperative Activated Hopping Theory of Relaxation in Viscous Liquids. I. General Formulation and Application to Hard Sphere Fluids.

Journal Article · Thu May 01 00:00:00 EDT 2014 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4874842· OSTI ID:1136834

Mirigian, Stephen ^[1]; Schweizer, Kenneth ^[2]

University of Illinois at Urbana-Champaign
University of Illinois

We generalize the force-level nonlinear Langevin equation theory of single particle hopping to includecollective effects associated with long range elastic distortion of the liquid. The activated alpharelaxation event is of a mixed spatial character, involving two distinct, but inter-related, local and collectivebarriers. There are no divergences at volume fractions below jamming or temperatures abovezero Kelvin. The ideas are first developed and implemented analytically and numerically in the contextof hard sphere fluids. In an intermediate volume fraction crossover regime, the local cage processis dominant in a manner consistent with an apparent Arrhenius behavior. The super-Arrhenius collectivebarrier is more strongly dependent on volume fraction, dominates the highly viscous regime,and is well described by a nonsingular law below jamming. The increase of the collective barrieris determined by the amplitude of thermal density fluctuations, dynamic shear modulus or transientlocalization length, and a growing microscopic jump length. Alpha relaxation time calculations arein good agreement with recent experiments and simulations on dense fluids and suspensions of hardspheres. Comparisons of the theory with elastic models and entropy crisis ideas are explored. Thepresent work provides a foundation for constructing a quasi-universal, fit-parameter-free theory forrelaxation in thermal molecular liquids over 14 orders of magnitude in time.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-00OR22725

OSTI ID:: 1136834

Journal Information:: Journal of Chemical Physics, Vol. 140, Issue n/a; ISSN 0021-9606

Country of Publication:: United States

Language:: English

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