Effect of cyclic stress on structural changes in polycarbonate as probed by positron annihilation lifetime spectroscopy

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Abstract
Positron annihilation lifetime spectroscopy (PALS) is used to probe structural changes in glassy polycarbonate in terms of changes in the hole volume and the number density of holes during fatigue (cyclic stress) aging. The ortho‐positronium (o‐Ps) pickoff annihilation lifetime τ3, as well as the intensity I3, were measured as a function of cyclic stresses and various previous thermophysical aging histories. It is found that τ3, the longest of the three lifetime components resolved in the PALS of glassy polycarbonate, increases when a cyclic stress is applied. These results indicate that there is a structural change during fatigue aging. The “holes” where o‐Ps can localize become larger upon fatigue aging. These results also suggest that a significant distinction exists between structural changes induced by thermophysical aging and fatigue aging. The o‐Ps annihilation intensity, which is a relative measure of the hole density in a material, showed a continuous decrease upon fatigue aging, indicating the possibility of hole coalescence, which could be a precursor of crazing. The interaction between thermophysical aging and fatigue aging corresponds very well with the enthalpy relaxation behavior as reported previously, viz., a well‐aged sample is much more sensitive to cyclic stress. More importantly, it is hypothesized that fatigue failure initiation is probably closely related to hole size and density fluctuation.