Abstract
The order−disorder ferrielectric−paraelectric transition in lamellar CuInP2S6 is studied using 31P solid-state MAS NMR spectroscopy. Spectra from a powder sample were recorded at various temperatures between 255 and 355 K with a probe precalibrated for heating or cooling due to magic angle spinning. Two center bands are observed at the lowest measured temperature while only one is detected at the highest temperature. The former two represent the inequivalent positions for the P atoms of the P2S6 group which reflect the antiparallel displacements of the polar CuI and InIII sublattices in the ferrielectric phase. The latter corresponds to the appearance of a 2-fold axis through the P−P bond as the CuI ions undergo double-well hopping motions, and the InIII ions occupy on-center sites in the paraelectric phase. At intermediate temperatures, both ferrielectric and paraelectric type resonances contribute to the spectrum at ratios which are T-dependent, indicating a transition temperature Tc = 312 ± 1 K (310 ± ...
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