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Poly(L-lactic acid) was crystallized from theglassy state at different temperatures to produce fullytransformed semi-crystalline specimens exhibiting differentlamellar morphologies. The materials were tested bydynamic mechanical analysis, where a Tg decrease wasfound with an increasing crystallization temperature. Consideringa three-phase model, this tendency was related tothe corresponding increase in the thickness of the rigidamorphous phase. It is suggested that this phase could, insome extent, accommodate through local translational/rotational motions the cooperative motions taking placewithin the mobile amorphous phase. This could be due tothe non-compact structure of the cooperatively rearrangingregions, which can present a string-like or fractal structurein their edges. The width of the loss factor peak associatedto the glass transition increases with increasing crystallizationtemperature, suggesting an increase in the broadness ofthe distribution of relaxation times. The drop in the storagemodulus across Tg varies systematically with the crystallizationtemperature in the different materials and could becorrelated with the crystalline content. Above Tg, the lossfactor exhibits a plateau-like behaviour at significantly highvalues, which seems to be a rather general behaviour insemi-crystalline systems that could be related to thecontribution of pure irreversible flow in the overallviscoelastic behaviour

Glass transition of semi-crystalline PLLA with different morphologies as studied by dynamic mechanical analysis