Coak Matthew J, Haines Charles R S, Liu Cheng, Rowley Stephen E, Lonzarich Gilbert G, Saxena Siddharth S
Cavendish Laboratory, Cambridge University, Cambridge CB3 0HE, United Kingdom;
Cavendish Laboratory, Cambridge University, Cambridge CB3 0HE, United Kingdom.
Proc Natl Acad Sci U S A. 2020 Jun 9;117(23):12707-12712. doi: 10.1073/pnas.1922151117. Epub 2020 May 26.
The dielectric and magnetic polarizations of quantum paraelectrics and paramagnetic materials have in many cases been found to initially increase with increasing thermal disorder and hence, exhibit peaks as a function of temperature. A quantitative description of these examples of "order-by-disorder" phenomena has remained elusive in nearly ferromagnetic metals and in dielectrics on the border of displacive ferroelectric transitions. Here, we present an experimental study of the evolution of the dielectric susceptibility peak as a function of pressure in the nearly ferroelectric material, strontium titanate, which reveals that the peak position collapses toward absolute zero as the ferroelectric quantum critical point is approached. We show that this behavior can be described in detail without the use of adjustable parameters in terms of the Larkin-Khmelnitskii-Shneerson-Rechester (LKSR) theory, first introduced nearly 50 y ago, of the hybridization of polar and acoustic modes in quantum paraelectrics, in contrast to alternative models that have been proposed. Our study allows us to construct a detailed temperature-pressure phase diagram of a material on the border of a ferroelectric quantum critical point comprising ferroelectric, quantum critical paraelectric, and hybridized polar-acoustic regimes. Furthermore, at the lowest temperatures, below the susceptibility maximum, we observe a regime characterized by a linear temperature dependence of the inverse susceptibility that differs sharply from the quartic temperature dependence predicted by the LKSR theory. We find that this non-LKSR low-temperature regime cannot be accounted for in terms of any detailed model reported in the literature, and its interpretation poses an empirical and conceptual challenge.
在许多情况下,人们发现量子顺电体和顺磁材料的介电极化和磁极化最初会随着热无序的增加而增大,因此会表现出随温度变化的峰值。在近铁磁金属以及处于位移型铁电转变边界的电介质中,对这些“无序致有序”现象的定量描述一直难以实现。在此,我们对近铁电材料钛酸锶中介电常数峰值随压力的演化进行了实验研究,结果表明随着铁电量子临界点的临近,峰值位置向绝对零度坍塌。我们表明,与已提出的其他模型相比,这种行为可以在不使用可调参数的情况下,根据近50年前首次引入的关于量子顺电体中极性模式与声学模式杂化的拉金 - 赫姆林茨基 - 什涅尔森 - 雷切斯特(LKSR)理论进行详细描述。我们的研究使我们能够构建出一种处于铁电量子临界点边界的材料的详细温度 - 压力相图,该相图包括铁电、量子临界顺电以及杂化极性 - 声学区域。此外,在最低温度下,低于磁化率最大值时,我们观察到一个区域,其特征是磁化率倒数与温度呈线性关系,这与LKSR理论预测的四次方温度依赖关系截然不同。我们发现,这种非LKSR低温区域无法用文献中报道的任何详细模型来解释,其解释在经验和概念上都构成了挑战。