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Powder X-ray diffraction (PXRD) and single-crystal neutron scattering wereused to study in detail the structural properties of the Cs2CuCl(4-x)Br(x)series, good realizations of layered triangular antiferromagnets. Detailedtemperature-dependent PXRD reveal a pronounced anisotropy of the thermalexpansion for the three different crystal directions of the orthorhombicstructure without any structural phase transition down to 20 K. Remarkably, theanisotropy of the thermal expansion varies for different $x$, leading todistinct changes of the geometry of the local Cu environment as a function oftemperature and composition. The refinement of the atomic positions confirmsthat for x=1 and 2, the Br atoms occupy distinct halogen sites in the[CuX4]-tetrahedra (X = Cl, Br). The precise structure data are used tocalculate the magnetic exchange couplings using density functional methods forx=0. We observe a pronounced temperature dependence of the calculated magneticexchange couplings, reflected in the strong sensitivity of the magneticexchange couplings on structural details. These calculations are in goodagreement with the experimentally established values for Cs2CuCl4 if one takesthe low-temperature structure data as a starting point.

Low-temperature structural investigations of the frustrated quantum antiferromagnets Cs2CuCl(4-x)Br(x)