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arXiv · 1808.06566

Synthesis-Dependent Properties of Barlowite and Zn-Substituted Barlowite

Rebecca W. Smaha·Wei He·John P. Sheckelton·Jiajia Wen·Young S. Lee
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Abstract

The mineral barlowite, Cu$_4$(OH)$_6$FBr, has been the focus of recent attention due to the possibility of substituting the interlayer Cu$^{2+}$ site with non-magnetic ions to develop new quantum spin liquid materials. We re-examine previous methods of synthesizing barlowite and describe a novel hydrothermal synthesis method that produces large single crystals of barlowite and Zn-substituted barlowite (Cu$_3$Zn$_x$Cu$_{1-x}$(OH)$_6$FBr). The two synthesis techniques yield barlowite with indistinguishable crystal structures and spectroscopic properties at room temperature; however, the magnetic ordering temperatures differ by 4 K and the thermodynamic properties are clearly different. The dependence of properties upon synthetic conditions implies that the defect chemistry of barlowite and related materials is complex and significant. Zn-substituted barlowite exhibits a lack of magnetic order down to T = 2 K, characteristic of a quantum spin liquid, and we provide a synthetic route towards producing large crystals suitable for neutron scattering.

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Rebecca W. Smaha, Wei He, John P. Sheckelton, Jiajia Wen, Young S. Lee. 2018-08-20. Synthesis-Dependent Properties of Barlowite and Zn-Substituted Barlowite. https://doi.org/10.1016/j.jssc.2018.08.016

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