Theory of the Transition in KH2PO4

凝聚态物理 相变 过渡点 铁学 Crystal(编程语言) 居里温度 过渡态理论 极化(电化学) 偶极子 化学 物理 结晶学 材料科学 热力学 量子相变 量子临界点 量子力学 铁磁性 物理化学 计算机科学 反应速率常数 动力学 程序设计语言
作者
J. C. Slater
出处
期刊:Journal of Chemical Physics [American Institute of Physics]
卷期号:9 (1): 16-33 被引量:628
标识
DOI:10.1063/1.1750821
摘要

Potassium dihydrogen phosphate contains phosphate groups connected by hydrogen bonds. Different possible arrangements of the hydrogens result effectively in different orientations of the (H2PO4)— dipoles. Since these have the lowest energy when pointing along the axis of the crystal, there is a tendency toward spontaneous polarization along this axis, resulting in the well-known transition, similar to Rochelle salt, with polarization below the Curie point. The theory of this transition is worked out, using statistical methods to count the number of arrangements of hydrogens consistent with each total polarization of the crystal, and deriving the free energy. It is found that the theory predicts a phase change of the first order, with sudden transition from the polarized state at low temperature to the unpolarized state at high temperature, rather than the lambda-point transition or phase change of the second order which is observed. However, the observed transition is confined to a very narrow temperature range compared to that predicted, for instance, by the Weiss theory, so that it seems as if it might be merely a broadened transition of the first order. It is suggested that the broadening may result from the irregular shifts of transition temperatures of individual domains in the crystal on account of stresses resulting from the large piezoelectric effect and the resulting deformation of the crystal below the transition point. The susceptibility above the Curie point comes out by the theory to be 4.33 times as great as it should according to the Weiss theory, a result which seems to be in general agreement with experiment. The entropy change in the transition is given by the theory as 0.69 unit, somewhat smaller than the observed value of about 0.8 unit. No explanation is suggested for this discrepancy.
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