For branched polymers, the curvilinear motion of the branch point along the backbone is a significant relaxation source but details of this motion have not been well understood. This study conducts multi-chain sliplink simulations to examine effects of the spatial fluctuation and curvilinear hopping of the branch point on the viscoelastic relaxation. The simulation is based on the primitive chain network model that allows the spatial fluctuations of sliplink and branch point and the chain sliding along the backbone according to the subchain tension, chemical potential gradients, drag force against medium, and random force. The sliplinks are created and/or disrupted through the motion of chain ends. The curvilinear hopping of the branch point along the backbone is allowed to occur when all sliplinks on a branched arm are lost. The simulations considering the fluctuation and the hopping of the branch point described well the viscoelastic data for symmetric and asymmetric star polymers with a parameter set common to the linear polymer. On the other hand, the simulations without the branch point motion predicted unreasonably slow relaxation for asymmetric star polymers. For asymmetric star polymers, further tests with and without the branch point hopping revealed that the hopping is much less important compared to the branch point fluctuation when the lengths of the short and long backbone arms are not very different and the waiting time for the branch point hopping (time for removal of all sliplinks on the short arm) is larger than the backbone relaxation time. Although this waiting time changes with the hopping condition, the above results suggest a significance of the branch point fluctuation in the actual relaxation of branch polymers.
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21 May 2011
Research Article|
May 17 2011
Primitive chain network simulations for asymmetric star polymers
Yuichi Masubuchi;
Yuichi Masubuchi
a)
1Institute for Chemical Research,
Kyoto University
, Gokasyo, Uji, Kyoto 611-0011, Japan
2
JST-CREST
, Kyoto 611-0011, Japan
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Takatoshi Yaoita;
Takatoshi Yaoita
1Institute for Chemical Research,
Kyoto University
, Gokasyo, Uji, Kyoto 611-0011, Japan
3
Material Science Laboratory
, Mitsui Chemicals Inc., Chiba 299-0265, Japan
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Yumi Matsumiya;
Yumi Matsumiya
1Institute for Chemical Research,
Kyoto University
, Gokasyo, Uji, Kyoto 611-0011, Japan
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Hiroshi Watanabe
Hiroshi Watanabe
1Institute for Chemical Research,
Kyoto University
, Gokasyo, Uji, Kyoto 611-0011, Japan
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a)
Author to whom correspondence should be addressed. Electronic mail: mas@scl.kyoto-u.ac.jp, Tel .:+81-774-38-3136, FAX: +81-774-38-3139.
J. Chem. Phys. 134, 194905 (2011)
Article history
Received:
March 22 2011
Accepted:
April 21 2011
Citation
Yuichi Masubuchi, Takatoshi Yaoita, Yumi Matsumiya, Hiroshi Watanabe; Primitive chain network simulations for asymmetric star polymers. J. Chem. Phys. 21 May 2011; 134 (19): 194905. https://doi.org/10.1063/1.3590276
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