Klein Ryan A, Walsh James P S, Clarke Samantha M, Liu Zhenxian, Alp E Ercan, Bi Wenli, Meng Yue, Altman Alison B, Chow Paul, Xiao Yuming, Norman M R, Rondinelli James M, Jacobsen Steven D, Puggioni Danilo, Freedman Danna E
Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA.
Lawrence Livermore National Laboratory, 7000 East Ave, Livermore, California 94550, USA.
Phys Rev Lett. 2020 Aug 14;125(7):077202. doi: 10.1103/PhysRevLett.125.077202.
We report a pressure-induced phase transition in the frustrated kagomé material jarosite at ∼45 GPa, which leads to the disappearance of magnetic order. Using a suite of experimental techniques, we characterize the structural, electronic, and magnetic changes in jarosite through this phase transition. Synchrotron powder x-ray diffraction and Fourier transform infrared spectroscopy experiments, analyzed in aggregate with the results from density functional theory calculations, indicate that the material changes from a R3[over ¯]m structure to a structure with a R3[over ¯]c space group. The resulting phase features a rare twisted kagomé lattice in which the integrity of the equilateral Fe^{3+} triangles persists. Based on symmetry arguments we hypothesize that the resulting structural changes alter the magnetic interactions to favor a possible quantum paramagnetic phase at high pressure.
我们报道了在约45吉帕压力下,受挫的 Kagomé 材料黄钾铁矾中发生的压力诱导相变,该相变导致磁有序消失。我们使用一系列实验技术,表征了黄钾铁矾在该相变过程中的结构、电子和磁性变化。同步辐射粉末X射线衍射和傅里叶变换红外光谱实验,结合密度泛函理论计算结果进行综合分析,表明该材料从R3[¯]m结构转变为具有R3[¯]c空间群的结构。所得相具有罕见的扭曲Kagomé晶格,其中等边Fe³⁺三角形的完整性得以保留。基于对称性论证,我们推测由此产生的结构变化改变了磁相互作用,有利于在高压下形成可能的量子顺磁相。