Abstract
Spatial heterogeneity in a polymer melt has been divided into two distributions that are distinguished by different relaxation behaviors of single-molecule probes near the nominal calorimetric glass-transition temperature (Tg). The fluorescence intensity and lifetime of individual molecules in a polymer film each exhibited a bimodal histogram that involved fast- and slow-relaxation sites at Tg − 8 K and Tg + 7 K, whereas a monomodal histogram composed of fast-relaxation sites was observed at Tg + 30 K. Temperature has no important effect on the center of each distribution in these histograms. Instead, occurrences of slow-relaxation sites decreased as the temperature increased from Tg − 8 K to Tg + 7 K and disappeared at Tg + 30 K. Furthermore, a change in the single-molecule fluorescence intensity was traced at fast- and slow-relaxation sites in a polymer film. At Tg − 8 K and Tg + 30 K, no substantial change in fluorescence intensity was observed at each site for ≥3 h, whereas, at Tg + 7 K, the fluoresce...
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