Intramolecular dynamic coupling slows surface relaxation of polymer glasses

Houkuan Tian, Jintian Luo, Qiyun Tang (), Hao Zha, Rodney D. Priestley (), Wenbing Hu and Biao Zuo ()
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Houkuan Tian: Zhejiang Sci-Tech University
Jintian Luo: Zhejiang Sci-Tech University
Qiyun Tang: Southeast University
Hao Zha: Zhejiang Sci-Tech University
Rodney D. Priestley: Princeton University
Wenbing Hu: Nanjing University
Biao Zuo: Zhejiang Sci-Tech University

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract Over the past three decades, studies have indicated a mobile surface layer with steep gradients on glass surfaces. Among various glasses, polymers are unique because intramolecular interactions — combined with chain connectivity — can alter surface dynamics, but their fundamental role has remained elusive. By devising polymer surfaces occupied by chain loops of various penetration depths, combined with surface dissipation experiments and Monte Carlo simulations, we demonstrate that the intramolecular dynamic coupling along surface chains causes the sluggish bulk polymers to suppress the fast surface dynamics. Such effect leads to that accelerated segmental relaxation on polymer glass surfaces markedly slows when the surface polymers extend chain loops deeper into the film interior. The surface mobility suppression due to the intramolecular coupling reduces the magnitude of the reduction in glass transition temperature commonly observed in thin films, enabling new opportunities for tailoring polymer properties at interfaces and under confinement and producing glasses with enhanced thermal stability.

Date: 2024
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DOI: 10.1038/s41467-024-50398-7

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