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亚稳钴蜂窝状 KCoAsO 的合成与表征

Synthesis and Characterization of Metastable Cobalt Honeycomb KCoAsO.

作者信息

Pressley Lucas A, Sarkis Colin L, Felder Justin, Dela Cruz Clarina R, Unocic Raymond R, Gai Zheng, Einkauf Jeffrey D, Pethe Saurabh P, Paranthaman Mariappan P, Berlijn Tom, Villanova John W, Okamoto Satoshi, McGuire Michael A, Tennant D Alan, Nagler Stephen E, Bridges Craig A

机构信息

Chemical Sciences Division, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37831, United States.

Quantum Science Center, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37831, United States.

出版信息

Inorg Chem. 2025 Jul 14;64(27):13696-13704. doi: 10.1021/acs.inorgchem.5c00932. Epub 2025 Jun 27.

Abstract

The Kitaev model has served as a long-sought-after target in the realization of a quantum spin liquid that could host Majorana Fermions. Such non-Abelian anyons could revolutionize quantum computing if properly implemented to overcome decoherence. A 3d electronic configuration, like Co, has been explored by theory and experimental work to design Kitaev materials. Here, we report the synthesis of a new cobaltate honeycomb material KCoAsO. The compound is synthesized through a low-temperature solution route and crystallized in space group ¯3 with lattice parameters = 5.0394(1) and = 28.6790(1) as determined by neutron powder diffraction. The crystal structure follows motifs similar to those of the honeycomb compound BaCo(AsO) but presents differing magnetic behavior. Magnetization/heat capacity measurements on the powder show antiferromagnetic transition = 14 K. Two lower-temperature transitions are present in susceptibility at low field that resemble spin reorientations. Magnetization data as a function of field have curvature indicative of metamagnetic behavior below the magnetic ordering temperature, with the magnetic ordering suppressed upon application of a higher magnetic field. Computational studies suggest the presence of a weak nearest-neighbor Kitaev term, K, consistent with related honeycomb cobaltates. Together, the data suggest that this material should present a new platform for developing Kitaev quantum spin liquids.

摘要

基泰耶模型一直是实现可能容纳马约拉纳费米子的量子自旋液体的长期追求目标。如果能妥善实现以克服退相干,这种非阿贝尔任意子可能会彻底改变量子计算。理论和实验工作已探索了像钴这样的3d电子构型来设计基泰耶材料。在此,我们报告了一种新型钴酸盐蜂窝材料KCoAsO的合成。该化合物通过低温溶液法合成,并通过中子粉末衍射确定其在空间群(\overline{3})中结晶,晶格参数(a = 5.0394(1))和(c = 28.6790(1))。其晶体结构遵循与蜂窝化合物BaCo(AsO)类似的模式,但呈现出不同的磁行为。对粉末进行的磁化/热容量测量显示反铁磁转变温度(T_N = 14)K。在低场下的磁化率中存在两个较低温度的转变,类似于自旋重取向。作为磁场函数的磁化数据具有曲率,表明在磁有序温度以下存在亚磁行为,在施加更高磁场时磁有序被抑制。计算研究表明存在较弱的最近邻基泰耶项(K),与相关的蜂窝钴酸盐一致。综合来看,这些数据表明这种材料应为开发基泰耶量子自旋液体提供一个新平台。

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