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Equilibration of High Molecular Weight Polymer Melts: A Hierarchical Strategy

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    Equilibration of High Molecular Weight Polymer Melts: A Hierarchical Strategy
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    † Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany
    ‡ Innovation Lab GmbH, Speyerer Strasse 4, 69115 Heidelberg, Germany
    *E-mail: [email protected]
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    ACS Macro Letters

    Cite this: ACS Macro Lett. 2014, 3, 2, 198–203
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    https://doi.org/10.1021/mz5000015
    Published January 30, 2014
    Copyright © 2014 American Chemical Society
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    Abstract

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    A strategy is developed for generating equilibrated high molecular weight polymer melts described with microscopic detail by sequentially backmapping coarse-grained (CG) configurations. The microscopic test model is generic but retains features like hard excluded volume interactions and realistic melt densities. The microscopic representation is mapped onto a model of soft spheres with fluctuating size, where each sphere represents a microscopic subchain with Nb monomers. By varying Nb, a hierarchy of CG representations at different resolutions is obtained. Within this hierarchy, CG configurations equilibrated with Monte Carlo at low resolution are sequentially fine-grained into CG melts described with higher resolution. A Molecular Dynamics scheme is employed to slowly introduce the microscopic details into the latter. All backmapping steps involve only local polymer relaxation; thus, the computational efficiency of the scheme is independent of molecular weight, being just proportional to system size. To demonstrate the robustness of the approach, microscopic configurations containing up to n = 1000 chains with polymerization degrees N = 2000 are generated and equilibration is confirmed by monitoring key structural and conformational properties. The extension to much longer chains or branched polymers is straightforward.

    Copyright © 2014 American Chemical Society

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    Parameterization of soft sphere model for different resolutions. Deviation of internal distance plots as a function of s. This material is available free of charge via the Internet at http://pubs.acs.org.

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    This article is cited by 70 publications.

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    Cite this: ACS Macro Lett. 2014, 3, 2, 198–203
    Click to copy citationCitation copied!
    https://doi.org/10.1021/mz5000015
    Published January 30, 2014
    Copyright © 2014 American Chemical Society
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