分子聚乙烯类似物中辐射损伤的量子模拟。

IF 4.2 3区 化学 Q2 POLYMER SCIENCE Macromolecular Rapid Communications Pub Date : 2024-10-22 DOI:10.1002/marc.202400669
Nathaniel Troup, Matthew P Kroonblawd, Davide Donadio, Nir Goldman
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引用次数: 0

摘要

要确定这些化学变化如何改变塑料等重要技术材料的物理和机械特性,就必须从原子层面了解聚乙烯等简单聚合物中的辐射诱导损伤。使用密度功能紧密结合方法对聚乙烯类似物中的辐射损伤进行了量子模拟组合,以帮助结合其辐射分解和随后的降解,使其成为辐射剂量的函数。采用图论方法对化学降解产物进行了分类,并计算了不饱和碳键形成、交联、循环形成、链式裂解反应和放气产物的发生率。产品对之间的统计相关性表明,链断裂反应、不饱和碳键形成和排气产品之间存在显著的相关性,但这些相关性随着原子反冲能的增加而降低。研究结果提出了相对简单的化学描述符,作为在中等激发能量范围内网络重排的可能指标。最终,这项研究提供了一个计算框架,用于确定聚合物中的非平衡化学与宏观尺度特性的潜在变化之间的耦合关系,有助于解释未来塑料材料的辐射损伤实验。
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Quantum Simulations of Radiation Damage in a Molecular Polyethylene Analog.

An atomic-level understanding of radiation-induced damage in simple polymers like polyethylene is essential for determining how these chemical changes can alter the physical and mechanical properties of important technological materials such as plastics. Ensembles of quantum simulations of radiation damage in a polyethylene analog are performed using the Density Functional Tight Binding method to help bind its radiolysis and subsequent degradation as a function of radiation dose. Chemical degradation products are categorized with a graph theory approach, and occurrence rates of unsaturated carbon bond formation, crosslinking, cycle formation, chain scission reactions, and out-gassing products are computed. Statistical correlations between product pairs show significant correlations between chain scission reactions, unsaturated carbon bond formation, and out-gassing products, though these correlations decrease with increasing atom recoil energy. The results present relatively simple chemical descriptors as possible indications of network rearrangements in the middle range of excitation energies. Ultimately, the work provides a computational framework for determining the coupling between nonequilibrium chemistry in polymers and potential changes to macro-scale properties that can aid in the interpretation of future radiation damage experiments on plastic materials.

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来源期刊
Macromolecular Rapid Communications
Macromolecular Rapid Communications 工程技术-高分子科学
CiteScore
7.70
自引率
6.50%
发文量
477
审稿时长
1.4 months
期刊介绍: Macromolecular Rapid Communications publishes original research in polymer science, ranging from chemistry and physics of polymers to polymers in materials science and life sciences.
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