Hexagonal antiferromagnets Cs$_2$Cu$_3$MF$_{12}$ (M = Zr, Hf and Sn) have uniform Kagome lattices of Cu$^{2+}$ with S = 1/2, whereas Rb$_2$Cu$_3$SnF$_{12}$ has a 2a by 2a enlarged cell as compared with the uniform Kagome lattice. The crystal data of
Cs$_2$Cu$_3$SnF$_{12}$ synthesized first in the present work are reported. We performed magnetic susceptibility measurements on this family of Kagome antiferromagnet using single crystals. In the Cs$_2$Cu$_3$MF$_{12}$ systems, structural phase transitions were observed at $T_t = 225$ K, 172 K and 185 K for M = Zr, Hf and Sn, respectively. The magnetic susceptibilities observed for $T > T_t$ are almost perfectly described using theoretical results obtained by exact diagonalization for the 24-site Kagome cluster with $J/k_B = 244$ K, 266 K and 240 K, respectively. Magnetic ordering accompanied by the weak ferromagnetic moment occurs at $T_N = 23.5$ K, 24.5 K and 20.0 K, respectively. The origins of the weak ferromagnetic moment should be ascribed to the lattice distortion that breaks the hexagonal symmetry of the exchange network for $T < T_t$ and the Dzyaloshinsky-Moriya interaction. Rb$_2$Cu$_3$SnF$_{12}$ is magnetically described as a modified Kagome antiferromagnet with four types of neighboring exchange interaction. Neither structural nor magnetic phase transition was observed in Rb$_2$Cu$_3$SnF$_{12}$. Its magnetic ground state was found to be a spin singlet with a triplet gap. Using exact diagonalization for a 12-site Kagome cluster, we analyzed the magnetic susceptibility and evaluated individual exchange interactions. The causes leading to the different ground states in Cs$_2$Cu$_3$SnF$_{12}$ and Rb$_2$Cu$_3$SnF$_{12}$ are discussed.
We synthesized single crystals of the new hexagonal compounds A$_2$Cu$_3$SnF$_{12}$ with A=Cs and Rb, and investigated their magnetic properties. These compounds are composed of Kagom{e} layers of corner-sharing CuF$_6$-octahedra. Cs$_2$Cu$_3$SnF$_{1
2}$ has the proper Kagom{e} layer at room temperature, and undergoes structural phase transition at $T_mathrm{t}simeq 185$ K. The temperature dependence of the magnetic susceptibility in Cs$_2$Cu$_3$SnF$_{12}$ agrees well with the result of the numerical calculation for $S=1/2$ two-dimensional Heisenberg Kagom{e} antiferromagnet down to $T_mathrm{t}$ with the nearest exchange interaction $J/k_mathrm{B}simeq 240$ K. Although the magnetic susceptibility deviates from the calculated result below $T<T_mathrm{t}$, the rounded maxima were observed at approximately $Tsimeq (1/6)J/k_mathrm{B}$ as predicted by the theory. Cs$_2$Cu$_3$SnF$_{12}$ undergoes three-dimensional magnetic ordering at $T_mathrm{N} = 20$ K.
We investigated the crystal structure of Rb$_2$Cu$_3$SnF$_{12}$ and its magnetic properties using single crystals. This compound is composed of Kagome layers of corner-sharing CuF$_{6}$ octahedra with a 2a x 2a enlarged cell as compared with the prop
er Kagome layer. Rb$_2$Cu$_3$SnF$_{12}$ is magnetically described as an $S$=1/2 modified Kagome antiferromagnet with four kinds of neighboring exchange interaction. From magnetic susceptibility and high-field magnetization measurements, it was found that the ground state is a disordered singlet with the spin gap, as predicted from a recent theory. Exact diagonalization for a 12-site Kagome cluster was performed to analyze the magnetic susceptibility, and individual exchange interactions were evaluated.
