Revealing spatially heterogeneous relaxation in a model nanocomposite

Cheng, Shiwang; Mirigian, Stephen; Carrillo, Jan-Michael Y.; Bocharova, Vera; Sumpter, Bobby G.; Schweizer, Kenneth S.; Sokolov, Alexei P.

doi:10.1063/1.4935595

Title: Revealing spatially heterogeneous relaxation in a model nanocomposite

Journal Article · Wed Nov 18 00:00:00 EST 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4935595· OSTI ID:1265978

Cheng, Shiwang ^[1]; Mirigian, Stephen ^[2]; Carrillo, Jan-Michael Y. ^[1]; Bocharova, Vera ^[1]; Sumpter, Bobby G. ^[1]; Schweizer, Kenneth S. ^[2]; Sokolov, Alexei P. ^[3]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Illinois, Urbana, IL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

The detailed nature of spatially heterogeneous dynamics of glycerol-silica nanocomposites is unraveled by combining dielectric spectroscopy with atomistic simulation and statistical mechanical theory. Analysis of the spatial mobility gradient shows no glassy layer, but the -relaxation time near the nanoparticle grows with cooling faster than the -relaxation time in the bulk and is ~20 times longer at low temperatures. The interfacial layer thickness increases from ~1.8 nm at higher temperatures to ~3.5 nm upon cooling to near bulk T_g. A real space microscopic description of the mobility gradient is constructed by synergistically combining high temperature atomistic simulation with theory. Our analysis suggests that the interfacial slowing down arises mainly due to an increase of the local cage scale barrier for activated hopping induced by enhanced packing and densification near the nanoparticle surface. As a result, the theory is employed to predict how local surface densification can be manipulated to control layer dynamics and shear rigidity over a wide temperature range.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1265978

Alternate ID(s):: OSTI ID: 1421239

Journal Information:: Journal of Chemical Physics, Vol. 143, Issue 19; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 43 works

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