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Confining glassy polymer into films can substantially modify their local and film-averaged properties. We present a lattice model of film geometry with void-mediated facilitation behaviors but free from any elasticity effect. We analyze the…

软凝聚态物质 · 物理学 2024-05-17 Qiang Zhai , Xin-Yuan Gao , Chun-Shing Lee , Chin-Yuan Ong , Ke Yan , Hai-Yao Deng , Sen Yang , Chi-Hang Lam

Thin polymer films have striking dynamical properties that differ from their bulk counterparts. With the simple geometry of a stepped polymer film on a substrate, we probe mobility above and below the glass transition temperature…

The dynamics of polymer surfaces is a controversial subject. Many experimental evidences support the existence of a surface mobile layer, while there are a few equally strong experimental evidences that contradict it. Here we show, through…

材料科学 · 物理学 2014-12-16 Zongyi Qin , K. C. Wong , Z. Yang

We investigate the near-surface relaxation of freestanding atactic \glsdesc{ps} films with molecular dynamics simulations. As in previous coarse-grained simulations, relaxation times for backbone segments and phenyl rings are linked to…

软凝聚态物质 · 物理学 2020-10-19 Derek Fujimoto , W. Andrew MacFarlane , Joerg Rottler

A simple and predictive model is put forward explaining the experimentally observed substantial shift of the glass transition temperature, Tg, of sufficiently thin polymer films. It focuses on the limit of small molecular weight, where…

软凝聚态物质 · 物理学 2009-11-07 Stephan Herminghaus , Karin Jacobs , Ralf Seemann

A free surface induces enhanced dynamics in glass formers. We study the dynamical enhancement of glassy films with a distinguishable-particle lattice model of glass free of elastic effects. We demonstrate that the thickness of the surface…

软凝聚态物质 · 物理学 2025-06-17 Qiang Zhai , Hai-Yao Deng , Xin-Yuan Gao , Leo S. I. Lam , Sen Yang , Ke Yan , Chi-Hang Lam

Surface tension-driven flow techniques have recently emerged as an efficient means of shedding light into the rheology of thin polymer films. Motivated by experimental and theoretical approaches in films bearing a varying surface…

软凝聚态物质 · 物理学 2017-04-26 Ioannis Tanis , Hendrik Meyer , Thomas Salez , Elie Raphaël , Anthony C. Maggs , Jörg Baschnagel

We study the phenomenon of migration of the small molecular weight component of a binary polymer mixture to the free surface using mean field and self-consistent field theories. By proposing a free energy functional that incorporates…

软凝聚态物质 · 物理学 2016-05-25 Jaroslaw Krawczyk , Salvatore Croce , T. C. B. McLeish , Buddhapriya Chakrabarti

We measure the isothermal rejuvenation of stable glass films of poly(styrene) and poly(methylmethacrylate). We demonstrate that the propagation of the front responsible for the transformation to a supercooled-liquid state can serve as a…

软凝聚态物质 · 物理学 2023-12-12 Saba Karimi , Junjie Yin , Thomas Salez , James A Forrest

Free surfaces in glassy polymer films are known to induce surface mobile layers with enhanced dynamics. Using molecular dynamics simulations of a bead-spring model, we study a wide variety of layer-resolved structural and dynamical…

软凝聚态物质 · 物理学 2018-11-14 Chi-Hang Lam

Motivated by recent experimental studies probing i) the existence of a mobile layer at the free surface of glasses, and ii) the capillary leveling of polymer nanofilms, we study the evolution of square-wave patterns at the free surface of a…

软凝聚态物质 · 物理学 2019-09-18 Ioannis Tanis , Kostas Karatasos , Thomas Salez

In an earlier preprint (V. V. Ginzburg, O. V. Gendelman, R. Casalini, and A. Zaccone, arxiv:2409.17291), we demonstrated that the dynamic (relaxation time) and volume equations of state for many amorphous polymers are near-universal -- each…

软凝聚态物质 · 物理学 2025-01-03 Valeriy V. Ginzburg , Oleg V. Gendelman , Riccardo Casalini , Alessio Zaccone

The free surface of glassy polymers exhibits enhanced segmental dynamics compared to the bulk, forming a liquid-like layer that lowers the glass transition temperature (Tg) in nanometersized polymer samples. Recent studies have shown that…

软凝聚态物质 · 物理学 2025-05-12 Xinyu Zhang , Christian Pedersen , Haoqi Zhu , Siming Wang , Yuchen Fu , Liang Dai , Andreas Carlson , Thomas Salez , Yu Chai

Polymer thin films exhibit pronounced interfacial mobility gradients that modify chain relaxation, yet how these gradients govern chain-scale dynamics across depth remains incompletely understood. Using molecular dynamics simulations of…

软凝聚态物质 · 物理学 2026-02-27 Bao T. Ma , David S. Simmons

The presence of a viscoelastic mechanism distinctly different from the segmental a-relaxation and the Rouse modes within the glass-rubber transition zone of polymers had been justified by theoretical considerations, and subsequently…

软凝聚态物质 · 物理学 2014-10-20 K. L. Ngai , S. Capaccioli , Daniele Prevosto , Luigi Grassia

We have studied the liquid-like response of the surface of vapour-deposited glassy films of polystyrene to the introduction of gold nanoparticles on the surface. The build-up of polymer material was measured as a function of time and…

Changes in the dynamics of supported polymer films in comparison to bulk materials involve a complex convolution of effects, such as substrate interactions, roughness and compliance, in addition to film thickness. We consider molecular…

软凝聚态物质 · 物理学 2015-02-11 Paul Z. Hanakata , Beatriz A. Pazmiño Betancourt , Jack F. Douglas , Francis W. Starr

Using molecular dynamics simulation of a polymer glass model we investigate free-standing polymer films focusing on the in-plane shear modulus $\mu$ and the corresponding shear-stress relaxation modulus $G(t)$ as functions of temperature…

软凝聚态物质 · 物理学 2018-12-12 G. George , I. Kriuchevskyi , H. Meyer , J. Baschnagel , J. P. Wittmer

Previously, we developed a minimal model based on random cooperative strings for the relaxation of supercooled liquids in the bulk and near free interfaces, and we recovered some key experimental observations. In this article, after…

无序系统与神经网络 · 物理学 2020-03-25 Maxence Arutkin , Elie Raphaël , James Forrest , Thomas Salez

The viscoelastic properties of thin polymeric films represent a central issue, especially for nanotechnological applications. In particular, it is highly relevant the dependence of viscoelasticity on the temperature. For polystyrene it is…

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