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Title: Systematic and simulation-free coarse graining of homopolymer melts: A structure-based study

Abstract

We propose a systematic and simulation-free strategy for coarse graining of homopolymer melts, where each chain of N{sub m} monomers is uniformly divided into N segments, with the spatial position of each segment corresponding to the center-of-mass of its monomers. We use integral-equation theories suitable for the study of equilibrium properties of polymers, instead of many-chain molecular simulations, to obtain the structural and thermodynamic properties of both original and coarse-grained (CG) systems, and quantitatively examine how the effective pair potentials between CG segments and the thermodynamic properties of CG systems vary with N. Our systematic and simulation-free strategy is much faster than those using many-chain simulations, thus effectively solving the transferability problem in coarse graining, and provides the quantitative basis for choosing the appropriate N-values. It also avoids the problems caused by finite-size effects and statistical uncertainties in many-chain simulations. Taking the simple hard-core Gaussian thread model [K. S. Schweizer and J. G. Curro, Chem. Phys. 149, 105 (1990)] as the original system, we demonstrate our strategy applied to structure-based coarse graining, which is quite general and versatile, and compare in detail the various integral-equation theories and closures for coarse graining. Our numerical results show that the effective CG potentialsmore » for various N and closures can be collapsed approximately onto the same curve, and that structure-based coarse graining cannot give thermodynamic consistency between original and CG systems at any N < N{sub m}.« less

Authors:
;  [1]
  1. Department of Chemical and Biological Engineering, Colorado State University, Fort Collins, Colorado 80523-1370 (United States)
Publication Date:
OSTI Identifier:
22416087
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 142; Journal Issue: 5; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; COMPARATIVE EVALUATIONS; DIAGRAMS; EQUILIBRIUM; INTEGRAL EQUATIONS; MASS; MONOMERS; POLYMERS; POTENTIALS; SIMULATION; THERMODYNAMIC PROPERTIES

Citation Formats

Yang, Delian, and Wang, Qiang. Systematic and simulation-free coarse graining of homopolymer melts: A structure-based study. United States: N. p., 2015. Web. doi:10.1063/1.4906493.
Yang, Delian, & Wang, Qiang. Systematic and simulation-free coarse graining of homopolymer melts: A structure-based study. United States. https://doi.org/10.1063/1.4906493
Yang, Delian, and Wang, Qiang. Sat . "Systematic and simulation-free coarse graining of homopolymer melts: A structure-based study". United States. https://doi.org/10.1063/1.4906493.
@article{osti_22416087,
title = {Systematic and simulation-free coarse graining of homopolymer melts: A structure-based study},
author = {Yang, Delian and Wang, Qiang},
abstractNote = {We propose a systematic and simulation-free strategy for coarse graining of homopolymer melts, where each chain of N{sub m} monomers is uniformly divided into N segments, with the spatial position of each segment corresponding to the center-of-mass of its monomers. We use integral-equation theories suitable for the study of equilibrium properties of polymers, instead of many-chain molecular simulations, to obtain the structural and thermodynamic properties of both original and coarse-grained (CG) systems, and quantitatively examine how the effective pair potentials between CG segments and the thermodynamic properties of CG systems vary with N. Our systematic and simulation-free strategy is much faster than those using many-chain simulations, thus effectively solving the transferability problem in coarse graining, and provides the quantitative basis for choosing the appropriate N-values. It also avoids the problems caused by finite-size effects and statistical uncertainties in many-chain simulations. Taking the simple hard-core Gaussian thread model [K. S. Schweizer and J. G. Curro, Chem. Phys. 149, 105 (1990)] as the original system, we demonstrate our strategy applied to structure-based coarse graining, which is quite general and versatile, and compare in detail the various integral-equation theories and closures for coarse graining. Our numerical results show that the effective CG potentials for various N and closures can be collapsed approximately onto the same curve, and that structure-based coarse graining cannot give thermodynamic consistency between original and CG systems at any N < N{sub m}.},
doi = {10.1063/1.4906493},
url = {https://www.osti.gov/biblio/22416087}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 5,
volume = 142,
place = {United States},
year = {2015},
month = {2}
}