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Intramolecular dynamic coupling slows surface relaxation of polymer glasses.
Tian, Houkuan; Luo, Jintian; Tang, Qiyun; Zha, Hao; Priestley, Rodney D; Hu, Wenbing; Zuo, Biao.
Afiliación
  • Tian H; School of Chemistry and Chemical Engineering, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, Hangzhou, 310018, China.
  • Luo J; School of Chemistry and Chemical Engineering, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, Hangzhou, 310018, China.
  • Tang Q; Key Laboratory of Quantum Materials and Devices of Ministry of Education, School of Physics, Southeast University, Nanjing, 211189, China. qtang@seu.edu.cn.
  • Zha H; School of Chemistry and Chemical Engineering, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, Hangzhou, 310018, China.
  • Priestley RD; Department of Chemical and Biological Engineering, Princeton Institute for the Science and Technology of Materials, Princeton University, Princeton, NJ, 08544, USA. rpriestl@princeton.edu.
  • Hu W; Department of Polymer Science, School of Chemistry and Chemical Engineering, State Key Lab of Coordination Chemistry, Nanjing University, Nanjing, 210023, China.
  • Zuo B; School of Chemistry and Chemical Engineering, Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province, Zhejiang Sci-Tech University, Hangzhou, 310018, China. chemizuo@zstu.edu.cn.
Nat Commun ; 15(1): 6082, 2024 Jul 19.
Article en En | MEDLINE | ID: mdl-39030198
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.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Reino Unido