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تسجيل مستخدم جديدNew S=1/2 Kagome Antiferromagnets A$_2$Cu$_3$SnF$_{12}$: A=Cs and Rb
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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$_{12}$ 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.
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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.
Magnetization and specific heat measurements have been carried out on Cs$_2$Cu$_3$ZrF$_{12}$ and Cs$_2$Cu$_3$HfF$_{12}$ single crystals, in which Cu$^{2+}$ ions with spin-1/2 form a regular Kagom{e} lattice. The antiferromagnetic exchange interaction
between neighboring Cu$^{2+}$ spins is $J/k_{rm B}simeq 360$ K and 540 K for Cs$_2$Cu$_3$ZrF$_{12}$ and Cs$_2$Cu$_3$HfF$_{12}$, respectively. Structural phase transitions were observed at $T_{rm t}simeq 210$ K and 175 K for Cs$_2$Cu$_3$ZrF$_{12}$ and Cs$_2$Cu$_3$HfF$_{12}$, respectively. The specific heat shows a small bend anomaly indicative of magnetic ordering at $T_mathrm{N}= 23.5$ K and 24.5 K in Cs$_2$Cu$_3$ZrF$_{12}$ and Cs$_2$Cu$_3$HfF$_{12}$, respectively. Weak ferromagnetic behavior was observed below $T_mathrm{N}$. This weak ferromagnetism should be ascribed to the antisymmetric interaction of the Dzyaloshinsky-Moriya type that are generally allowed in the Kagom{e} lattice.
High-resolution time-of-flight powder neutron diffraction and high-field magnetization were measured to investigate the magnetic structure and existence of a field-induced magnetic phase transition in the distorted kagome antiferromagnet Cs$_2$Cu$_3$
SnF$_{12}$. Upon cooling from room temperature, the compound undergoes a structural phase transition at $T_textrm{t}=185$ K from the rhombohedral space group $Rbar{3}m$ with the perfect kagome spin network to the monoclinic space group $P2_1/n$ with the distorted kagome planes. The distortion results in three inequivalent exchange interactions among the $S=1/2$ Cu$^{2+}$ spins that magnetically order below $T_textrm{N}=20.2$ K. Magnetization measured with a magnetic field applied within the kagome plane reveals small in-plane ferromagnetism resulting from spin canting. On the other hand, the out-of-plane magnetization does not show a clear hysteresis loop of the ferromagnetic component nor a prominent anomaly up to 170 T, with the exception of the subtle knee-like bend around 90 T, which could indicate the 1/3 magnetization plateau. The combined analysis using the irreducible representations of the magnetic space groups and magnetic structure refinement on the neutron powder diffraction data suggests that the magnetic moments order in the magnetic space group $P2_1/n$ with the all-in-all-out spin structure, which by symmetry allows for the in-plane canting, consistent with the in-plane ferromagnetism observed in the magnetization.
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