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Universal Trend of the Non-Exponential Rouse Mode Relaxation in Glass-Forming Polymers Systems: Experimental Facts, MD-Simulation Results and a Theoretical Approach Based on a Generalized Langevin Equation

Published online by Cambridge University Press:  26 January 2016

J. Colmenero
J. Colmenero*
Affiliation:
Materials Research Center (CSIC-UPV/EHU), Pº Manuel de Lardizabal 5, San Sebastian, Spain.
*
*(Email: juan.colmenero@ehu.es)
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Abstract

Nowadays there are clear evidences from both experiments and MD-simulations proving that the chain Rouse modes correlation functions are non-exponential in unentangled polymer blends and also in pure polymers at low temperature (with respect to that of the glass transition Tg) even for the long wavelengths modes where local potentials and chain stiffness should not play any role. In a recent paper [S. Arrese-Igor et al, Phys. Rev. Lett.113, 078302 (2014)] it has been proposed that this non-exponential behavior depends on the ratio between the so-called Rouse time - i.e., the characteristic time of the slowest chain mode relaxation - and the time scale of the α-relaxation. This parameter is in some way ‘universal’ in the meaning that it can encode many different experimental situations. In this paper, we show that this behavior can be quantitatively explained in the framework of a theoretical approach based on: (i) a generalized Langevin equation (GLE) formalism and (ii) a memory function which takes into account the effect of collective dynamics on the chain dynamics of a tagged chain and which was constructed taking inspirations from the original ideas of the reptation model proposed by de Gennes.

Keywords

polymermixturedielectric
Type
Articles
Information
MRS Advances , Volume 1 , Issue 26: Theory, Characterization, and Modeling , 2016 , pp. 1903 - 1913
Copyright
Copyright © Materials Research Society 2016 

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References

REFERENCES

Colmenero, J., J. Phys.: Condens. Matter 27, 103101 (2015).Google Scholar
Doi, M. and Edwards, S., “The theory of Polymer Dynamics” (Oxford Science Publications, 1990).Google Scholar
Rouse, E. P., J. Chem. Phys. 21, 1272 (1953).CrossRefGoogle Scholar
Riedel, C., Alegría, A., Tordjeman, P. and Colmenero, J., Macromolecules 42, 8492 (2009).Google Scholar
Colmenero, J. and Arbe, A., Soft Matter 3, 1 (2007).Google Scholar
Arrese-Igor, S., Alegría, A., Moreno, A. J. and Colmenero, J., Macromolecules 44, 3611 (2011).Google Scholar
Svanberg, C. and Bergman, R., J. Non-Cryst. Solids 283, 225 (2001).Google Scholar
Brodeck, M., Alvarez, F., Moreno, A. J., Colmenero, J. and Richter, D., Macromolecules 43, 3036 (2010).Google Scholar
Colmenero, J., J. Non-Cryst. Solids 407, 302 (2015).Google Scholar
Moreno, A. J. and Colmenero, J., Phys. Rev. Lett. 100, 126001 (2008).Google Scholar
Arrese-Igor, S., Alegría, A. and Colmenero, J., Phys. Rev. Lett. 113, 078302 (2014).Google Scholar
Colmenero, J., Soft Matter 11, 5614 (2015).Google Scholar
Kimmich, R. and Fatkullin, N., “Polymer Chain Dynamics and NMR” (Springer Verlag, 2004, vol. 70, Advances in Polymer Science) pp 1–113.Google Scholar
de Gennes, P. G., J. Chem. Phys. 55, 572 (1971).Google Scholar
Schweizer, K. S., J. Chem. Phys. 91, 5802 (1989).Google Scholar
Berne, B. J. and Pecora, R., “Dynamic Ligth Scattering” (Wiley, 1976).Google Scholar
Novikov, V. N., Schweizer, K. S. and Sokolov, A. P., J. Chem. Phys. 138, 164508 (2013).Google Scholar
Colmenero, J., Alvarez, F., Khairy, Y. and Arbe, A., J. Chem. Phys. 139, 044906 (2013).Google Scholar
Colmenero, J., Alvarez, F. and Arbe, A., EPJ Web Conf. 83, 01001 (2015)Google Scholar
Arrese-Igor, S., Alegría, A., Moreno, A. J. and Colmenero, J., Soft Matter 8, 3739 (2012).Google Scholar