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Synthetic barlowite, Cu4(OH)6BrF, has emerged as a new quantum spin liquid(QSL) host, containing kagome layers of S=1/2 Cu2+ ions separated by interlayerCu2+ ions. Similar to synthetic herbertsmithite, ZnCu3(OH)6Cl2, it has beenreported that Zn2+ substitution for the interlayer Cu2+ induces a QSL groundstate. Here we report a scalable synthesis of single crystals of Cu4(OH)6BrF.Through x-ray, neutron, and electron diffraction measurements coupled withmagic angle spinning 19F and 1H NMR spectroscopy, we resolve the previouslyreported positional disorder of the interlayer Cu2+ ions and find that thestructure is best described in the orthorhombic space group, Cmcm, with latticeparameters a = 6.665(13) A, b = 11.521(2) A, c = 9.256(18) A and an orderedarrangement of interlayer Cu2+ ions. Infrared spectroscopy measurements of theO-H and F-H stretching frequencies demonstrate that the orthorhombic symmetrypersists upon substitution of Zn2+ for Cu2+. Specific heat and magneticsusceptibility measurements of Zn-substituted barlowite, ZnxCu4-x(OH)6BrF,reveal striking similarities with the behavior of ZnxCu4-x(OH)6Cl2. Theseparallels imply universal behavior of copper kagome lattices even in thepresence of small symmetry breaking distortions. Thus synthetic barlowitedemonstrates universality of the physics of synthetic Cu2+ kagome minerals andfurthers the development of real QSL states.

Single crystal growth of Cu4(OH)6BrF and universal behavior in quantum spin liquid candidates synthetic barlowite and herbertsmithite