Citation: Yao, P.; Feng, L. K.; Guo, H. X. Combined molecular dynamics simulation and rouse model analysis of static and dynamic properties of unentangled polymer melts with different chain architectures. Chinese J. Polym. Sci. 2021, 39, 512–524 doi: 10.1007/s10118-020-2489-4 shu

Combined Molecular Dynamics Simulation and Rouse Model Analysis of Static and Dynamic Properties of Unentangled Polymer Melts with Different Chain Architectures

  • Corresponding author: Hong-Xia Guo, E-mail:
  • Received Date: 2020-07-18
    Available Online: 2020-09-29

Figures(6) / Tables(1)

  • Chain architecture effect on static and dynamic properties of unentangled polymers is explored by molecular dynamics simulation and Rouse mode analysis based on graph theory. For open chains, although they generally obey ideal scaling in chain dimensions, local structure exhibits nonideal behavior due to the incomplete excluded volume (EV) screening, the reduced mean square internal distance (MSID) can be well described by Wittmer’ theory for linear chains and the resulting chain swelling is architecture dependent, i.e., the more branches a bit stronger swelling. For rings, unlike open chains they are compact in term of global sizes. Due to EV effect and nonconcatenated constraints their local structure exhibits a quite different non-Gaussian behavior from open chains, i.e., reduced MSID curves do not collapse to a single master curve and fail to converge to a chain-length-independent constant, which makes the direct application of Wittmer’s theory to rings quite questionable. Deviation from ideality is further evidenced by limited applicability of Rouse prediction to mode amplitude and relaxation time at high modes as well as the non-constant and mode-dependent scaled Rouse mode amplitudes, while the latter is architecture-dependent and even molecular weight dependent for rings. The chain relaxation time is architecture-dependent, but the same scaling dependence on chain dimensions does hold for all studied architectures. Despite mode orthogonality at static state, the role of cross-correlation in orientation relaxation increases with time and the time-dependent coupling parameter rises faster for rings than open chains even at short time scales it is lower for rings.
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