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A simple theory for glassy polymeric mechanical response which accounts forlarge scale chain relaxation is presented. It captures the crossover fromperfect-plastic response to strong strain hardening as the degree ofpolymerization $N$ increases, without invoking entanglements. By relatinghardening to interactions on the scale of monomers and chain segments, wecorrectly predict its magnitude. Strain activated relaxation arising from theneed to maintain constant chain contour length reduces the $N$ dependence ofthe characteristic relaxation time by a factor $\sim \dot\epsilon N$ duringactive deformation at strain rate $\dot\epsilon$. This prediction is consistentwith results from recent experiments and simulations, and we suggest how it maybe further tested experimentally.

Viscoplasticity and large-scale chain relaxation in glassy-polymeric strain hardening