“…Recently, it has been shown that terahertz spectroscopy can provide rich information regarding crystallization and hydrogen bond formation in polymeric materials. , Because various macromolecular vibration modes including the intramolecular vibration modes and the lattice vibration modes of crystalline states of polymers ,,− exist in the terahertz frequency range (0.1–10 THz or in terms of wavenumbers, 3.3–330 cm –1 ), the terahertz light can be used to directly probe the macromolecular vibration modes. For example, the determination of the crystallinity of materials like cellulose and poly(vinyl chloride) has been achieved by the quantitative measurement of terahertz absorption caused by the lattice vibration modes. − Furthermore, the hydrogen bond formation in polymeric materials has been investigated by the comparison between terahertz and infrared spectra and quantum chemical calculations. ,, We note that spectroscopic studies of PLA in the terahertz regime have been performed to reveal the crystallization process ,,, and the strain-induced crystallization . Although there are several reports on terahertz spectroscopy of PLA, quantitative estimation of the crystallinity and detailed analysis of the hydrogen bond formation in sc-PLA, especially in the case of low crystallinity, are still lacking.…”