Coarse-grained molecular dynamics modeling of strongly associating fluids: Thermodynamics, liquid structure, and dynamics of symmetric binary mixture fluids

doi:10.1021/jp0722096

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	Coarse-grained molecular dynamics modeling of strongly associating fluids: Thermodynamics, liquid structure, and dynamics of symmetric binary mixture fluids
	Li, Ting ; Nies, Erik
刊名	JOURNAL OF PHYSICAL CHEMISTRY B
	2007-07-19
卷号	111 期号:28 页码:8131-8144
ISSN号	1520-6106
DOI	10.1021/jp0722096
英文摘要	Symmetric binary mixtures capable of strong association via a highly directional and saturable specific interaction between unlike molecules are investigated by canonical molecular dynamics simulations. The specific interaction of the molecules is defined in a new coarse-grained pair potential that can be applied in continuous molecular dynamics as well as in Monte Carlo simulations. The thermodynamic, structural, and dynamic properties of the associating mixture fluids are investigated as a function of density, temperature, and association strength of the specific interaction. Detailed analysis of the simulation data confirms a two-stage mechanism in the formation of specific bonds with increasing interaction strength, including a fast dimerization process and a subsequent stage of perfecting the bonds. A large heat capacity peak is found during the formation or breaking of the bonds, reflecting the large energy fluctuation introduced by the strong association. The fractions of nonbonded molecules obtained from the simulations as a function of density, temperature, and interaction strength are in excellent agreement with the predictions of Wertheim's thermodynamic perturbation theory. The translational and rotational dynamics of the Tmer mixture are effectively retarded with increasing association strength and are analyzed in terms of autocorrelation functions and a non-Gaussian parameter for the translational dynamics. The lifetimes of molecules in bonded and nonbonded states provide detailed information about the transformation of molecules between the bonded state and the nonbonded state. Finally, simulation sampling problems inherent to strongly interacting systems are easily overcome using the parallel tempering simulation technique. This latter result confirms that with the new continuous coarse-grained simulation potential we have a versatile and flexible interaction potential that can be used with many available molecular dynamics and Monte Carlo algorithms under various ensembles.
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000247966300030
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/62549]
专题	中国科学院化学研究所
通讯作者	Li, Ting
作者单位	1.Katholieke Univ Leuven, Dept Chem, Polymer Res Div, B-3001 Heverlee, Belgium 2.Chinese Acad Sci, Inst Chem, Ctr Mol Sci, State Key Lab Polymer Phys & Chem, Beijing 100080, Peoples R China 3.Eindhoven Univ Technol, Lab Polymer Technol, NL-5600 MB Eindhoven, Netherlands
推荐引用方式 GB/T 7714	Li, Ting,Nies, Erik. Coarse-grained molecular dynamics modeling of strongly associating fluids: Thermodynamics, liquid structure, and dynamics of symmetric binary mixture fluids[J]. JOURNAL OF PHYSICAL CHEMISTRY B,2007,111(28):8131-8144.
APA	Li, Ting,&Nies, Erik.(2007).Coarse-grained molecular dynamics modeling of strongly associating fluids: Thermodynamics, liquid structure, and dynamics of symmetric binary mixture fluids.JOURNAL OF PHYSICAL CHEMISTRY B,111(28),8131-8144.
MLA	Li, Ting,et al."Coarse-grained molecular dynamics modeling of strongly associating fluids: Thermodynamics, liquid structure, and dynamics of symmetric binary mixture fluids".JOURNAL OF PHYSICAL CHEMISTRY B 111.28(2007):8131-8144.