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The time‐dependence of birefringence was investigated in experiments involving relaxation at constant strain, extension at constant rate of strain, and periodically varying strain. The results of constant strain relaxation are calculated from the other two types of experiments using the linear phenomenological theory of birefringence relaxation. Strain‐optical coefficient spectra are calculated for a number of low‐ and high‐density polyethylenes and characteristics of the spectra are correlated with sample density. A simple molecular theory is presented. The time‐dependence of birefringence is believed to principally arise from the finite relaxation time for crystal orientation.