SynopsisA rheo-optical investigation has been carried out on a sample of high-density polyethylene (HDPE) in an attempt to examine the nature of the a-relaxation mechanism. Dynamic mechanical and birefringence behavior was measured over the frequency range of 0.008-4.3 Hz and temperature range -40 to 100°C. The dynamic mechanical and birefringence data were reduced to a reference temperature of 50°C by a combination of horizontal and vertical superposition. The significance of the vertical shift factor has been discussed extensively in previous papers and is not dealt with here. An Arrhenius plot was made of the log of the horizontal shift factor versus reciprocal Emperature for the mechanical and optical data. The mechanical data exhibited three distinct regions, the slopes of which led to activation energies of 70,90, and 150 kJ mol-'. The temperature at which these dispersions occurred suggested the observation of the / 3, a', and a2 relaxation processes. The optical data contained two distinct regions from which activation energies of 55 and 95 kJ mol-' were obtained. The high-temperature ap process was not observed in the Arrhenius plot; however, a maximum in K' and a change in sign of K" probably reflects a contribution from the a2 relaxation mechanism. K', the real part of the modulus E', the birefringence-strain phase angle a, and