Revealing the Role of Microstructure and Strain Heterogeneities in the Elastic–Plastic Transition of Glassy Polymers

IF 5.2 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2025-07-03 DOI:10.1021/acs.macromol.5c00694

Hilal Reda*, Panayiota Katsamba, Anthony Chazirakis and Vagelis Harmandaris*,

引用次数: 0

Abstract

In this work, we investigate the atomic and microstructural underpinnings of glassy polymers, focusing on the transition from elastic to plastic regimes under tensile strain and the underlying mechanisms at the atomic scale via detailed atomistic simulations. We highlight the role of local heterogeneities and their interplay in stress, strain, and density fields. Our key message is that the coupling between the microstructure (density) and strain heterogeneities is crucial for the elastic–plastic transition. Regions with increased free volume facilitate activation of vitreous segments, reorganization of polymer atoms to minimize nonbonded interactions and stress dissipation, leading to enhanced mobility and delayed strain-hardening of low-density regions.

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揭示微观结构和应变非均质性在玻璃聚合物弹塑性转变中的作用

在这项工作中，我们研究了玻璃聚合物的原子和微观结构基础，重点研究了拉伸应变下从弹性到塑性的转变，以及通过详细的原子模拟在原子尺度上的潜在机制。我们强调了局部非均质性及其在应力场、应变场和密度场中的相互作用。我们的关键信息是微观结构（密度）和应变非均质性之间的耦合对于弹塑性转变至关重要。自由体积增加的区域促进了玻璃体片段的激活，聚合物原子的重组以减少非键相互作用和应力消散，从而提高了低密度区域的迁移率和延迟应变硬化。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.