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Register a new userOrigin of Magnetic Ordering in a Structurally-Perfect Quantum Kagome Antiferromagnet
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The ground state of the simple Heisenberg nearest-neighbor quantum kagome antiferromagnetic model is a magnetically disordered spin liquid, yet various perturbations may lead to fundamentally different states. Here we disclose the origin of magnetic ordering in the structurally-perfect kagome material YCu$_3$(OH)$_6$Cl$_3$, which is free of the widespread impurity problem. {it Ab-initio} calculations and modeling of its magnetic susceptibility reveal that, similar to the archetypal case of herbertsmithite, the nearest-neighbor exchange is by far the dominant isotropic interaction. Dzyaloshinskii-Moriya (DM) magnetic anisotropy deduced from electron spin resonance and specific-heat measurements is, however, significantly larger than in herbertsmithite. By enhancing spin correlations within kagome planes, this anisotropy is essential for magnetic ordering. Our study isolates the effect of DM anisotropy from other perturbations and unambiguously confirms the theoretical phase diagram.
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We present thermodynamic studies of a new spin-1/2 antiferromagnet containing undistorted kagome lattices---barlowite Cu$_{4}$(OH)$_{6}$FBr. Magnetic susceptibility gives $theta_{CW}$ = $-$136 K, while long-range order does not happen until $T_{N}$ = 15 K with a weak ferromagnetic moment $mu$ $<$ 0.1$mu_{B}$/Cu. A 60 T magnetic field induces a moment less than 0.5$mu_{B}$/Cu at $T$ = 0.6 K. Specific-heat measurements have observed multiple phase transitions at $T ll$ $mid$$theta_{CW}$$mid$. The magnetic entropy of these transitions is merely 18% of $k_{B}$ln2 per Cu spin. These observations suggest that nontrivial spin textures are realized in barlowite with magnetic frustration. Comparing with the leading spin-liquid candidate herbertsmithite, the superior interkagome environment of barlowite sheds light on new spin-liquid compounds with minimum disorder. The robust perfect geometry of the kagome lattice makes charge doping promising.
The emergent behavior of spin liquids that are born out of geometrical frustration makes them an intriguing state of matter. We show that in the quantum kagome antiferromagnet ZnCu$_3$(OH)$_6$SO$_4$ several different correlated, yet fluctuating states exist. By combining complementary local-probe techniques with neutron scattering, we discover a crossover from a critical regime into a gapless spin-liquid phase with decreasing temperature. An additional unconventional instability of the latter phase leads to a second, distinct spin-liquid state that is stabilized at the lowest temperatures. We advance such complex behavior as a feature common to different frustrated quantum magnets.
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 report bulk magnetization, and elastic and inelastic neutron scattering measurements under an external magnetic field, $H$, on the weakly coupled distorted kagome system, Cu_{2}(OD)_3Cl. Our results show that the ordered state below 6.7 K is a canted antiferromagnet and consists of large antiferromagnetic $ac$-components and smaller ferromagnetic $b$-components. By first-principle calculations and linear spin wave analysis, we present a simple spin hamiltonian with non-uniform nearest neighbor exchange interactions resulting in a system of coupled spin trimers with a single-ion anisotropy that can qualitatively reproduce the spin dynamics of Cu_{2}(OD)_3Cl.
We present powder and single-crystal neutron diffraction and bulk measurements of the Kagome-staircase compound Ni3V2O8 (NVO) in fields up to 8.5T applied along the c-direction. (The Kagome plane is the a-c plane.) This system contains two types of Ni ions, which we call spine and cross-tie. Our neutron measurements can be described with the paramagnetic space group Cmca for T < 15K and each observed magnetically ordered phase is characterized by the appropriate irreducible representation(s). Our zero-field measurements show that at T_PH=9.1K NVO undergoes a transition to an incommensurate order which is dominated by a longitudinally-modulated structure with the spine spins mainly parallel to the a-axis. Upon further cooling, a transition is induced at T_HL=6.3K to an elliptically polarized incommensurate structure with both spine and cross-tie moments in the a-b plane. At T_LC=4K the system undergoes a first-order phase transition, below which the magnetic structure is a commensurate antiferromagnet with the staggered magnetization primarily along the a-axis and a weak ferromagnetic moment along the c-axis. A specific heat peak at T_CC=2.3K indicates an additional transition, which we were however not able to relate to a change of the magnetic structure. Neutron, specific heat, and magnetization measurements produce a comprehensive temperature-field phase diagram. The symmetries of the two incommensurate magnetic phases are consistent with the observation that only one phase has a spontaneous ferroelectric polarization. All the observed magnetic structures are explained theoretically using a simplified model Hamiltonian, involving competing nearest- and next-nearest-neighbor exchange interactions, spin anisotropy, Dzyaloshinskii-Moriya and pseudo-dipolar interactions.
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