Successive phase transitions of [(PyO)(H/D)][AuCl4] (PyO=C5H5NO)

35Cl NQR as well as heat capacity measurements of [(PyO)H][AuCl4] and its deuterated analog [(PyO)D][AuCl4] revealed successive phase transitions at 70.5 and 62.5 K, and at 71 and 63 K, respectively. The NQR frequency varied continuously through the upper transition point while discontinuously through the lower transition point. In the intermediate-temperature phase a remarkable decrease in the signal intensity was observed. These NQR observations as well as the feature of the heat capacity anomaly in which a broad peak is succeeded by a sharp peak with decreasing temperature suggest a possibility of normal-incommensurate-commensurate phase sequence.