4.7 Article

First-principle simulations of electronic structure in semicrystalline polyethylene

期刊

JOURNAL OF CHEMICAL PHYSICS
卷 146, 期 20, 页码 -

出版社

AIP Publishing
DOI: 10.1063/1.4983650

关键词

-

资金

  1. Swedish Research Council [621-2012-2673, 621-2014-5398]
  2. Swedish Governmental Agency for Innovation Systems (Vinnova) [2015-06557]
  3. Vinnova [2015-06557] Funding Source: Vinnova

向作者/读者索取更多资源

In order to increase our fundamental knowledge about high-voltage cable insulation materials, realistic polyethylene (PE) structures, generated with a novel molecular modeling strategy, have been analyzed using first principle electronic structure simulations. The PE structures were constructed by first generating atomistic PE configurations with an off-lattice Monte Carlo method and then equilibrating the structures at the desired temperature and pressure using molecular dynamics simulations. Semicrystalline, fully crystalline and fully amorphous PE, in some cases including crosslinks and short-chain branches, were analyzed. The modeled PE had a structure in agreement with established experimental data. Linear-scaling density functional theory (LS-DFT) was used to examine the electronic structure (e.g., spatial distribution of molecular orbitals, bandgaps and mobility edges) on all the materials, whereas conventional DFT was used to validate the LS-DFT results on small systems. When hybrid functionals were used, the simulated bandgaps were close to the experimental values. The localization of valence and conduction band states was demonstrated. The localized states in the conduction band were primarily found in the free volume (result of gauche conformations) present in the amorphous regions. For branched and crosslinked structures, the localized electronic states closest to the valence band edge were positioned at branches and crosslinks, respectively. At 0 K, the activation energy for transport was lower for holes than for electrons. However, at room temperature, the effective activation energy was very low (similar to 0.1 eV) for both holes and electrons, which indicates that the mobility will be relatively high even belowthe mobility edges and suggests that charge carriers can be hot carriers above the mobility edges in the presence of a high electrical field. (C) 2017 Author(s).

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.7
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据