Kadlec Filip, Nuzhnyy Dmitry, Kadlec Christelle, Petzelt Jan, Savinov Maxim, Kamba Stanislav
Institute of Physics, Czech Academy of Sciences, Na Slovance 2, 182 21, Prague 8, Czech Republic.
Sci Rep. 2022 Apr 13;12(1):6157. doi: 10.1038/s41598-022-09890-7.
Lattice dynamics of a single crystal of lawsonite were studied over a broad range of frequencies (1 Hz to 20 THz) using impedance, THz time-domain and infrared spectroscopies. Based on polarized spectra of complex permittivity [Formula: see text] measured as a function of temperature between 10 K and 500 K, we analyzed the properties of the two known phase transitions-an antiferrodistortive one near [Formula: see text] and a ferroelectric one, occurring at [Formula: see text]. The former one is accompanied by a flat maximum in the THz-range permittivity [Formula: see text] near [Formula: see text], which is due to an overdamped polar excitation in the [Formula: see text] spectra reflecting the dynamics of water and hydroxyl groups. The strength of this mode decreases on cooling below [Formula: see text], and the mode vanishes below [Formula: see text] due to hydrogen ordering. At the pseudoproper ferroelectric phase transition, two independent anomalies in permittivity were observed. First, [Formula: see text] exhibits a peak at [Formula: see text] due to critical slowing down of a relaxation in the GHz range. Second, infrared and THz spectra revealed an optical phonon softening towards [Formula: see text] which causes a smaller but pronounced maximum in [Formula: see text]. Such anomaly, consisting in a soft mode polarized perpendicularly to the ferroelectric axis, is unusual in ferroelectrics.
利用阻抗、太赫兹时域和红外光谱技术,在很宽的频率范围(1赫兹至20太赫兹)内研究了硬柱石单晶的晶格动力学。基于在10K至500K温度范围内测量的复介电常数[公式:见原文]的偏振光谱,我们分析了两个已知相变的性质——一个在[公式:见原文]附近的反铁电畸变相变和一个在[公式:见原文]发生的铁电相变。前者在太赫兹范围介电常数[公式:见原文]中,在[公式:见原文]附近伴随着一个平坦的最大值,这是由于在[公式:见原文]光谱中一个过阻尼的极性激发,反映了水和羟基的动力学。低于[公式:见原文]冷却时,这种模式的强度降低,并且由于氢有序化,该模式在低于[公式:见原文]时消失。在准固有铁电相变时,观察到介电常数有两个独立的异常。首先,[公式:见原文]由于GHz范围内弛豫的临界减慢在[公式:见原文]处出现一个峰值。其次,红外和太赫兹光谱显示,朝向[公式:见原文]光学声子软化,这在[公式:见原文]中导致一个较小但明显的最大值。这种异常表现为一个垂直于铁电轴偏振的软模,在铁电体中是不常见的。