TY - JOUR
T1 - Derived Coarse-Grained Potentials for Semicrystalline Polymers with a Blended Multistate Iterative Boltzmann Inversion Method
AU - Eghlidos, Omid
AU - Oswald, Jay
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/12/26
Y1 - 2023/12/26
N2 - In this article, we employ the multistate iterative Boltzmann inversion (MS-IBI) method to develop coarse-grained potentials capable of representing molecular structure in both the amorphous and crystalline phases of semicrystalline polymers with improved accuracy while allowing for tunable control over the dynamics governing the α-relaxation process. A unique feature of this method is that the potentials are blended using the product of the target structural distributions, for example, the radial density function, for each phase and a weighting factor. To demonstrate this approach, a family of potentials for polyethylene is developed where the weighting factor of the crystalline phase ranges is varied from zero, incorporating information only from the amorphous phase, to unity, where the model is trained from only the crystalline phase. The most accurate representation of structural distributions was obtained when the crystalline phases is weighted at 50%. However, we show that when the crystalline phase is weighted at 90%, the model more accurately represents dynamics of the α-relaxation process, with realistic predicted values of activation energy and diffusion rates, with relatively minor impact on accuracy in structure.
AB - In this article, we employ the multistate iterative Boltzmann inversion (MS-IBI) method to develop coarse-grained potentials capable of representing molecular structure in both the amorphous and crystalline phases of semicrystalline polymers with improved accuracy while allowing for tunable control over the dynamics governing the α-relaxation process. A unique feature of this method is that the potentials are blended using the product of the target structural distributions, for example, the radial density function, for each phase and a weighting factor. To demonstrate this approach, a family of potentials for polyethylene is developed where the weighting factor of the crystalline phase ranges is varied from zero, incorporating information only from the amorphous phase, to unity, where the model is trained from only the crystalline phase. The most accurate representation of structural distributions was obtained when the crystalline phases is weighted at 50%. However, we show that when the crystalline phase is weighted at 90%, the model more accurately represents dynamics of the α-relaxation process, with realistic predicted values of activation energy and diffusion rates, with relatively minor impact on accuracy in structure.
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U2 - 10.1021/acs.jctc.3c00935
DO - 10.1021/acs.jctc.3c00935
M3 - Article
C2 - 38083860
AN - SCOPUS:85180093991
SN - 1549-9618
VL - 19
SP - 9445
EP - 9456
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
IS - 24
ER -