Progress towards a phenomenological picture and theoretical understanding of glassy dynamics and vitrification near interfaces and under nanoconfinement

Schweizer, Kenneth S.; Simmons, David S.

doi:10.1063/1.5129405

Title: Progress towards a phenomenological picture and theoretical understanding of glassy dynamics and vitrification near interfaces and under nanoconfinement

Journal Article · 29 December 2019 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5129405 · OSTI ID:1607394

^[1];

^[2]

Univ. of Illinois at Urbana-Champaign, IL (United States); University of Illinois at Urbana-Champaign
Univ. of South Florida, Tampa, FL (United States)

The nature of alterations to dynamics and vitrification in the nanoscale vicinity of interfaces-commonly referred to as "nanoconfinement" effects on the glass transition-has been an open question for a quarter century. We first analyze experimental and simulation results over the last decade to construct an overall phenomenological picture. Key features include the following: after a metrology- and chemistry-dependent onset, near-interface relaxation times obey a fractional power law decoupling relation with bulk relaxation; relaxation times vary in a double-exponential manner with distance from the interface, with an intrinsic dynamical length scale appearing to saturate at low temperatures; the activation barrier and vitrification temperature T-g approach bulk behavior in a spatially exponential manner; and all these behaviors depend quantitatively on the nature of the interface. We demonstrate that the thickness dependence of film-averaged T-g for individual systems provides a poor basis for discrimination between different theories, and thus we assess their merits based on the above dynamical gradient properties. Entropy-based theories appear to exhibit significant inconsistencies with the phenomenology. Diverse free-volume-motivated theories vary in their agreement with observations, with approaches invoking cooperative motion exhibiting the most promise. The elastically cooperative nonlinear Langevin equation theory appears to capture the largest portion of the phenomenology, although important aspects remain to be addressed. A full theoretical understanding requires improved confrontation with simulations and experiments that probe spatially heterogeneous dynamics within the accessible 1-ps to 1-year time window, minimal use of adjustable parameters, and recognition of the rich quantitative dependence on chemistry and interface. Published under license by AIP Publishing.

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Research Organization:: Univ. of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: FG02-07ER46471

OSTI ID:: 1607394

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 24 Vol. 151; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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