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Pom-pom model predictions on nonlinear stress relaxation in single-step strain flow

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Abstract

A phenomenological pom-pom model, which utilizes linear stress relaxation data as an input, is proposed for simulating the detailed retraction behavior of a full pom-pom chain as well as the associated nonlinear stress relaxation in single-step shear flows. Specifically, the initial, Rouse-like arm and/or backbone retraction as well as the long-time, renormalized (dumbbell-like) backbone retraction is simulated at one time, and a possible coupling between linear orientation relaxation and nonlinear stretch relaxation due to diffusive or convective constraint release is self-consistently accounted for. The model’s predictions are systematically tested against nonlinear stress relaxation data on three nearly monodisperse pom-pom melts, including two six-arm pom-pom polybutadienes (PPBDs) and an H-shaped polyisoprene (PPI). The model can describe the present data reasonably well by incorporating a previously proposed effect of drag–strain coupling. Accounting further for the effect of constraint release, due primarily to arm diffusive motion and its coupling with a known polydispersity in arm molecular weight distribution, appreciably broadens the predicted nonlinear stress relaxation and substantially improves the results of theory/data comparisons. The significance of the current findings is discussed.

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Acknowledgement

The authors thank the constructive comments of all reviewers. Financial support from MOE Program for Promoting Academic Excellence of Universities under the Grant no. 96-2752-E-007-006-PAE as well as from the National Science Council of the ROC under Grant no. 95-2221-E-194-049 is gratefully acknowledged. The resource provided by the National Center for High-Performance Computing of the ROC for performing part of the preliminary investigation is also acknowledged.

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  1. Department of Chemical Engineering, National Chung Cheng University, Chia Yi, 621, Taiwan, Republic of China

    Sheng Cheng Shie, Tzy Ming Yang & Chi Chung Hua

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  1. Sheng Cheng Shie
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  2. Tzy Ming Yang
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  3. Chi Chung Hua
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Corresponding author

Correspondence to Chi Chung Hua.

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Fig. S1

An overall comparison of nonlinear stress relaxation between experimental data and the simulation, Eqs. 1–5 with ν* = 0, for the PPBD-2 sample; note in particular the deviation starting at γ ≈ 5. Data have all been shifted for clarity (DOC 707 KB)

Fig. S2

An overall comparison of nonlinear stress relaxation between experimental data and the simulation, Eqs. 1–5 with ν* = 0, for the PPI sample; note in particular the deviation starting at γ ≈ 3. Data have all been shifted for clarity (DOC 669 KB)

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Shie, S.C., Yang, T.M. & Hua, C.C. Pom-pom model predictions on nonlinear stress relaxation in single-step strain flow. J Polym Res 15, 213–224 (2008). https://doi.org/10.1007/s10965-007-9161-3

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  • DOI: https://doi.org/10.1007/s10965-007-9161-3

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