A Replica Exchange Molecular Dynamics Simulation of a Single Polyethylene Chain: Temperature Dependence of Structural Properties and Chain Conformational Study at the Equilibrium Melting Temperature
文献类型：期刊论文
| 作者 | Li, Ting1,2; Yang, Xiaozhen3; Nies, Erik1,2,4 |
| 刊名 | JOURNAL OF CHEMICAL THEORY AND COMPUTATION
 |
| 出版日期 | 2011 |
| 卷号 | 7期号:1页码:188-202 |
| ISSN号 | 1549-9618 |
| DOI | 10.1021/ct100513y |
| 英文摘要 | The conformational properties of a finite length polyethylene chain were explored over a wide range of temperatures using a replica exchange molecular dynamics simulation providing high quality simulation data representative for the equilibrium behavior of the chain molecule. The radial distribution function (RDF) and the structure factor S(q) of the chain as a function of temperature are analyzed in detail. The different characteristic peaks in the RDF and S(q) were assigned to specific distances in the chain and structural changes occurring with the temperature. In S(q), a peak characteristic for the order in the solid state was found and used to determine the equilibrium melting temperature. A detailed scaling analysis of the structure factor covering the full q range was performed according to the work of Hammouda. In the Theta region, a quantitative analysis of the full structure factor was done using the equivalent Kuhn chain, which enabled us to assign the Theta region of our chain and to demonstrate, in our particular case, the failure of the Gaussian chain approach. The chain conformational properties at the equilibrium melting temperature are discussed using conformational distribution functions, using the largest principal component of the radius of gyration and shape parameters as order parameters. We demonstrate that for the system studied here, the Landau free energy expression based on this conformational distribution information leads to erroneous conclusions concerning the thermodynamic transition behavior. Finally, we focus on the instantaneous conformational properties at the equilibrium melting temperature and give a detailed analysis of the conformational shapes using different shape parameters and a simulation snapshot. We show that the chain does not only take the lamellar rod-like and globular conformational shapes, typical of the solid and liquid states, but can also explore many other conformational states, including the toroidal conformational state. It is the first demonstration that a flexible molecule like PE can also take a toroidal conformational state, which is normally linked to stiffer chains. |
| 语种 | 英语 |
| WOS记录号 | WOS:000285990300021 |
| 出版者 | AMER CHEMICAL SOC |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/71429]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | Nies, Erik |
| 作者单位 | 1.Katholieke Univ Leuven, Polymer Res Div, Leuven Math Modeling & Computat Sci Ctr LMCC, B-3001 Heverlee, Belgium 2.Katholieke Univ Leuven, LMRC, B-3001 Heverlee, Belgium 3.Chinese Acad Sci, Inst Chem, State Key Lab Polymer Phys & Chem, Ctr Mol Sci, Beijing 100080, Peoples R China 4.Eindhoven Univ Technol, Lab Polymer Technol, NL-5600 MB Eindhoven, Netherlands |
| 推荐引用方式 GB/T 7714 | Li, Ting,Yang, Xiaozhen,Nies, Erik. A Replica Exchange Molecular Dynamics Simulation of a Single Polyethylene Chain: Temperature Dependence of Structural Properties and Chain Conformational Study at the Equilibrium Melting Temperature[J]. JOURNAL OF CHEMICAL THEORY AND COMPUTATION,2011,7(1):188-202. |
| APA | Li, Ting,Yang, Xiaozhen,&Nies, Erik.(2011).A Replica Exchange Molecular Dynamics Simulation of a Single Polyethylene Chain: Temperature Dependence of Structural Properties and Chain Conformational Study at the Equilibrium Melting Temperature.JOURNAL OF CHEMICAL THEORY AND COMPUTATION,7(1),188-202. |
| MLA | Li, Ting,et al."A Replica Exchange Molecular Dynamics Simulation of a Single Polyethylene Chain: Temperature Dependence of Structural Properties and Chain Conformational Study at the Equilibrium Melting Temperature".JOURNAL OF CHEMICAL THEORY AND COMPUTATION 7.1(2011):188-202. |
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来源：化学研究所
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