Reactive force field molecular dynamics simulation of structure and mechanical property of Si-doped glow discharge polymer
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摘要: 构建了硅掺杂辉光放电聚合物（Si-GDP）模型，采用反应力场分子动力学模拟（ReaxFF MD）探讨了硅含量、碳氢比及密度对其杂化碳键合与力学性能的影响。研究结果表明：随着硅含量增加，聚合物中sp3C含量增加，趋向于形成一个大分子，同时小分子种类和数目减少，促进了碳硅原子成键并抑制端基CH3生成，进而提高材料力学性能；随着氢含量的增加，sp3C和端基CH3比例增加，生成的端基CH3降低了分子间交联程度，进而降低了材料力学性能，而分子基团数目变化不明显；随着密度的提升，聚合物中sp2C比例提升明显，sp3C比例有少量提升，分子基团数目变化不大，密度主要通过提升sp2C比例提升材料力学性能。研究结果为评估和理解硅掺杂辉光放电聚合物的结构和力学性能提供了新的视角和方法。Abstract: The structural models of Si-doped glow discharge polymer (Si-GDP) were established using reactive force field molecular dynamics simulation (ReaxFF MD), and the effects of silicon content, hydrogen content, and density on its hybrid carbon bonding and mechanical properties were investigated. The results show that with the silicon content increasing, the molecules tend to form a silicon-containing macromolecule, and the types and number of small molecules decrease, the silicon content improves the mechanical properties by promoting the binding of carbon and silicon atoms and inhibiting the formation of end-group sp3CH3. Besides, species such as ·C2H3, ·C3H5 and ·Si(CH3)3 were found during the formation of Si-GDP, which were in good agreement with the thin film deposition experiment of glow discharge polymer. The hydrogen content is measured as the atomic ratio of hydrogen to carbon and silicon, as the ratio grows, the number of model molecules did not change significantly, the ratio of sp3C and sp3CH3 increased, and the hydrogen content decreased the mechanical properties mainly by promoting the formation of sp3CH3. With the density increasing, the number of molecular species in the model did not change much, and the proportion of sp2C in the model was significantly increased, while the proportion of sp3C was slightly increased, the mechanical properties of Si-doped hydrogenated amorphous carbon were mainly improved by increasing the proportion of sp2C. This study provides an example for constructing Si-GDP by ReaxFF MD, and may provide a new method and reference for evaluating the structure and mechanical properties of Si-GDP.
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图 3 Si-GDP模型最长分子链示意图(右侧透明部分为最长分子链，深色部分为其他分子碎片)
Figure 3. Diagram of the longest molecular chains of Si-GDP
表 1 Si-GDP模型参数
Table 1. Model parameters of Si-GDP
model name number of atoms Si atom fraction/% RH:(Si+C) density/(g·cm−3) all C H Si Si-1.2 1488 645 825 18 1.2 1.19 ± 0.03 0.95 Si-3.8 1418 597 767 54 3.8 1.19 ± 0.03 0.95 Si-6.3 1420 567 763 90 6.3 1.19 ± 0.03 0.98 Si-8.6 1461 548 787 126 8.6 1.19 ± 0.03 1.03 Si-10.6 1524 525 837 162 10.6 1.19 ± 0.03 1.07 H-0.95 1419 613 692 114 8.6 ± 0.4 0.95 1.08 H-1.00 1396 580 698 118 8.6 ± 0.4 1.00 1.04 H-1.07 1402 554 725 123 8.6 ± 0.4 1.07 1.02 H-1.23 1471 534 810 127 8.6 ± 0.4 1.23 1.01 H-1.29 1436 496 808 132 8.6 ± 0.4 1.29 0.97 D-0.79 1108 463 573 72 6.3 ± 0.1 1.10 ± 0.02 0.79 D-0.91 1306 533 693 80 6.3 ± 0.1 1.10 ± 0.02 0.91 D-0.99 1401 580 733 88 6.3 ± 0.1 1.10 ± 0.02 0.99 D-1.09 1538 638 804 96 6.3 ± 0.1 1.10 ± 0.02 1.09 D-1.19 1693 703 886 104 6.3 ± 0.1 1.10 ± 0.02 1.19 
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