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End-linked polydimethysiloxane (PDMS) networks were prepared by end-linking vinyl-terminated PDMS chains with tetrafunctional silanes. Dielectric α-relaxation spectra, thermal expansivities, and the (rubbery) elastic modulus were measured for these materials. From the cross-link density at which marked changes occur in the segmental relaxation times and the Tα-scaled temperature dependence (fragility), a characteristic length for the α-relaxation was determined. The result, 14 A at Tα, is quite close to the length scale associated with constraint of crystallization in similar PDMS networks. Cross-linking also affects the thermal expansion and elastic modulus, although these properties exhibit a smoother variation with cross-link density.

Segmental Relaxation in End-Linked Poly(dimethylsiloxane) Networks