Abstract
Proton spin relaxation measurements above the glass transition temperature have been used to investigate the effect of crosslinking on local and coherent segmental dynamics in cis-1,4-polybutadiene samples. The polymer chains in bulk polybutadiene were crosslinked by exposure to ionizing radiation. The transition of the 1H-NMR signal from a liquid-like spin system response to a solid-like one is due to crosslinking and network formation by the irradiation and depends on the radiation dose. The description of the relaxation data is based on a stochastic model of translational diffusion of structural defects between fluctuating and fixed junctions of polymer chains. The assigned composite stochastic process has non-Markovian character. It is shown that the radiation yields changes in the constrained defect diffusion processes modelling the chain dynamics. Correlation time and memory time for the local and coherent segmental motion strongly depend on radiation dose.
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