Abstract
Dynamic behavior of various polymer melts is studied on the basis of a comparison of viscoelastic properties with the information obtained from dielectric spectroscopy. The experimental observations are compared with results of computer simulation of corresponding systems. The studies include simple melts of linear chains, block copolymer systems of miscible components, as well as the behavior of melts with molecular objects of complex topology-like stars or microgels. In the case of polyisoprene linear chain melts an equivalence of terminal relaxation times determined from mechanical and dielectric measurements is demonstrated. Using linear block copolymers of isoprene and butadiene, relaxation times of chain fragments (isoprene blocks) in relation to relaxation times of whole copolymer chains are determined and compared with theory and simulation. Both the experimentally determined block relaxation times and relaxation times of chain fragments in simulated linear chain melts show a disagreement with predictions of the reptation theory. In the case of multiarm star polymers and microgel melts, the slow relaxation modes observed in viscoelastic spectra are assigned to cooperative translational motions detected in corresponding simulated systems in which an ordering of such molecules is demonstrated. This suggests that the terminal relaxation in multiarm star or microgel melts is governed by another relaxation mechanism than in linear chain melts. High efficiency of the Cooperative Motion Algorithm in simulation of dense systems of complex molecules is demonstrated.
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References
Ferry JD (1980) Viscoelastic properties of polymers. Wiley, New York
Adachi K, Kotaka T (1993) Prog Polym Sci 18:589
Ewen B, Richter D, Farago B, Fetters LJ, Huang JS, Maschke U (1992) Proc Am Chem Soc Div Polym Mater Sci Eng 67:211
Doi M, Edwards SF (1986) The theory of polymer dynamics. Clarendon Press, Oxford, UK
“Monte Carlo and molecular dynamics simulations in polymer science” (Binder K, ed.). Oxford Univ Press 1995
Hansen JP, McDonald IR (1986) “Theory of simple liquids”. Academic Press, London
Brawer S, “Relaxation in viscous liquids and glasses”. Amer Ceram Soc, Columbus, 1985
Verdier PH, Stockmayer WH (1967) J Chem Phys 36:227;
Lal M (1969) Mol Phys 17:57;
Wall FT, Mandel F (1975) J Chem Phys 63:4592;
Carmesin I, Kremer K (1988) Macromolecules 21:2819;
Binder K, Kremer K (1988) Comput Phys Rep 7:261
Reiter J, Edling T, Pakula T (1990) J Chem Phys 93:837
Pakula T (1987) Macromolecules 20:679;
Pakula T, Geyler S (1987) Macromolecules 20:2909
De Gennes PG (1991) J Chem Phys 55:572
Graesley WW (1982) Adv Polym Sci 47:67
Onogi S, Masuda T, Kitagawa K (1970) Macromolecules 3:109
Boese D, Kremer F (1990) Macromolecules 23:8298
Boese D, Kremer F, Fetters LJ (1990) Macromolecules 23:1826
Richter D, Butera R, Fetters LJ, Huang JS, Farago B, Ewen B (1992) Macromolecules 25:6167
Ewen B, Maschke U, Richter D, Farago B (1994) Acta Polym 45:143
McKenna GB, Hadzioannou G, Lutz P, Held G, Strazielle C, Straupe C, Remp P, Kovacs AJ (1987) Macromolecules 20:489
Fetters LJ, Kiss AD, Pearson DS, Quack GF, Vitus FJ (1993) Macromolecules 26:647
Roovers J, Zbou Lin-Lin, Toporowski PM, van der Zwan M, Iatron H, Hadjichristidis N (1993) Macromolecules 25:4324; Roovers J, Vlassopoulos D, Pakula T, in preparation
McCarthy TF, Witteler H, Pakula T, Wegner G (1995) Macromolecules 28:8350
Antonietti M, Pakula T, Bremser W (1995) Macromolecules 28:4227
Geyler S, PhD Thesis, Mainz 1990
Kremer F, Boese D, Meier G, Fischer EW (1989) Prog Coll Polym Sci 129:80
Edling T, PhD Thesis, Mainz 1994
Stockmayer WH (1967) Pure Appl Chem 15:539
Reiter J (1991) J Chem Phys 94:3222
Ronca G (1983) J Chem Phys 79:1031
Gauger A, Weyersberg A, Pakula T (1993) Macromol Chem Theory Simul 2:531
Gauger A, Pakula T (1995) Macromolecules 28:190
Pakula T, Geyler S (1988) Macromolecules 21:1665
Grest GS, Kremer K, Milner ST, Witten TA (1989) Macromolecules 22:1904
Pakula T (1991) J Chem Phys 94:2104
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Dedicated to the memory of Professor Tasos C. Papanastasiou
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Pakula, T., Geyler, S., Edling, T. et al. Relaxation and viscoelastic properties of complex polymer systems. Rheola Acta 35, 631–644 (1996). https://doi.org/10.1007/BF00396512
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DOI: https://doi.org/10.1007/BF00396512