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Multiscale simulations of the structure and dynamics of stereoregular poly(methyl methacrylate)s

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Abstract

The chain tacticity of a polymer is a key influence on its structure and dynamics, which ultimately determine its properties. While they have great potential to elucidate the influence of chain tacticity, all-atom molecular simulations are often restricted to short chains and small systems. In this work, two typical stereoregular poly(methyl methacrylate) melts were investigated via multiscale simulations. To improve computational efficiency, systematic coarse-graining was first performed. While the coarse-grained molecular dynamics simulations were able to show the effects of tacticity on intramolecular structure and intermolecular interactions, they were not able to reproduce the exact structural distribution or even the effects of tacticity on the dynamics. An alternative reverse-mapping scheme was therefore developed specifically to treat chain configurations in a direct geometric way. The backmapped all-atomistic simulations were found to accurately reproduce the microscopic features of the polymers. Since the effects of tacticity are rather subtle and therefore difficult to discern, this multiscale simulation scheme is a very important method of investigating complex high molecular weight polymer systems.

A multiscale simulation scheme for polymer structure and dynamicsᅟ

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Acknowledgments

This work was financially supported by the Natural Science Foundation of China (NSFC) under grant 21104018/B040613, the Innovative Research Team in the Higher Educational Institute of Hunan Province, the Training Plan for Young Backbone Teachers of Hunan Province, and the Talent Support Plan of Hunan University of Humanities, Science and Technology (HUHST). The author is indebted to the Molecular Simulation Center of Hunan Province (located at Hunan University), which provided the commercial software (Materials Studio 4.0) that was used to build the initial structural models, and the Laboratory for High Performance Computing (HPC) of the key discipline “Computer Applied Techniques” of Hunan Province (located at HUHST), which provided generous CPU time that enabled the completion of this work. Also, the author greatly appreciates Mrs. Zhihua Zeng for providing valuable help in revising the expressions, and Prof. Michel Petitjean for fruitful discussions of the algorithms.

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  1. Department of Chemistry and Materials Science, Hunan University of Humanities Science & Technology, Loudi, 417000, Hunan Province, People’s Republic of China

    Chaofu Wu

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Wu, C. Multiscale simulations of the structure and dynamics of stereoregular poly(methyl methacrylate)s. J Mol Model 20, 2377 (2014). https://doi.org/10.1007/s00894-014-2377-3

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