Abstract

The equilibrium nonlinear stress-stretch relationships for a monodomain main-chain nematic elastomer (MNE) are investigated by varying the angle between the stretching and initial director axes (θ0). Angle θ0 has pronounced effects on the ultimate elongation as well as on the width of the low stress plateau regime (Λp) during director rotation, whereas θ0 has no appreciable effect on the plateau stress (σp). In the stretching normal to the initial director (θ0 = 90°), the plateau end exceeds 200% strain. At oblique angles of 90° > θ0≥ 35°, Λp decreases with decreasing θ0, whereas the definite plateau regime vanishes at θ0 < 24°. Wide-angle X-ray scattering and polarized optical microscopy measurements reveal that the director rotates uniformly in the biased direction for the MNE of θ0°≪ 90°, whereas directors rotating clockwise and counterclockwise are coexistent for θ0 = 90°. Over the entire plateau regime, the MNEs exhibit pure shear deformation characterized by a Poisson's ratio of zero in the direction of the rotation axis. The Λp for the corresponding polydomain NE (PNE) undergoing a transition to the monodomain alignment is smaller than that of the MNE of θ0 = 90°, while the σp values for both NEs are almost similar. The semi-soft elasticity concept satisfactorily explains the effects of θ0 on Λp, and the Λp value of the PNE, using a single anisotropy parameter which is evaluated from the degree of thermally induced deformation of MNEs.

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