Bidisperse melts of linear, entangled polymer chains were studied using dissipative particle dynamics. The entanglement constraints were mimicked with our newly developed slip-spring approach. The compositions cover blends with short matrix chains, slightly above the molecular entanglement weight as well as blends were both chain lengths exhibit distinct entangled dynamics at various weight fractions. The Struglinsky-Graessley parameter Gr, which is the ratio between the relaxation time of the long chains due to pure reptation and the relaxation time of the tube caused by constraint release, ranges between values high above and below unity. We compare our slip-spring model with simulations that use conventional generic polymer models where bond crossings are prevented by excluded-volume interactions and find fairly good agreement in terms of the mean squared displacement. However, the slip-spring approach requires only a fraction of the computational time, making large scale systems feasible. The dynamical interference of the two different chain lengths is discussed in terms of reptation and constraint release dynamics. For bidisperse melt compositions with Gr < 1.0 the relaxation time of the long chain component is not affected by constraint release. However, for compositions where constraint release is supposed to contribute significantly to the relaxation mechanism (Gr > 1.0), we find strong evidence that the long chains reptate inside a dilated tube whose diameter increases with an exponent of 1/2 towards lower weight fraction of the long chains. Furthermore we observe a linear relation between the relaxation time and weight fraction. Therefore, based on the relaxation times, our results support the validity of the tube dilation model as proposed by Doi et al. [Macromolecules 20, 1900–1906 (1987)].
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21 November 2014
Research Article|
November 17 2014
Reptation and constraint release dynamics in bidisperse polymer melts
Michael Langeloth;
Michael Langeloth
a)
1Eduard-Zintl-Institut für Anorganische und Physikalische Chemie and Center of Smart Interfaces,
Technische Universität Darmstadt
, Alarich-Weiss-Straße 4, D-64287 Darmstadt, Germany
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Yuichi Masubuchi;
Yuichi Masubuchi
2Institute for Chemical Research,
Kyoto University
, Gokasho, Uji 611-0011, Japan
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Michael C. Böhm;
Michael C. Böhm
1Eduard-Zintl-Institut für Anorganische und Physikalische Chemie and Center of Smart Interfaces,
Technische Universität Darmstadt
, Alarich-Weiss-Straße 4, D-64287 Darmstadt, Germany
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Florian Müller-Plathe
Florian Müller-Plathe
1Eduard-Zintl-Institut für Anorganische und Physikalische Chemie and Center of Smart Interfaces,
Technische Universität Darmstadt
, Alarich-Weiss-Straße 4, D-64287 Darmstadt, Germany
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Michael Langeloth
1,a)
Yuichi Masubuchi
2
Michael C. Böhm
1
Florian Müller-Plathe
1
1Eduard-Zintl-Institut für Anorganische und Physikalische Chemie and Center of Smart Interfaces,
Technische Universität Darmstadt
, Alarich-Weiss-Straße 4, D-64287 Darmstadt, Germany
2Institute for Chemical Research,
Kyoto University
, Gokasho, Uji 611-0011, Japan
a)
Author to whom correspondence should be addressed. Electronic mail: [email protected]
J. Chem. Phys. 141, 194904 (2014)
Article history
Received:
July 09 2014
Accepted:
October 29 2014
Citation
Michael Langeloth, Yuichi Masubuchi, Michael C. Böhm, Florian Müller-Plathe; Reptation and constraint release dynamics in bidisperse polymer melts. J. Chem. Phys. 21 November 2014; 141 (19): 194904. https://doi.org/10.1063/1.4901425
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