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Register a new userBarlowite: A Spin-1/2 Antiferromagnet with a Geometrically Perfect Kagome Motif
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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.
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We study the zero-temperature phase diagram of the spin-$frac{1}{2}$ Heisenberg model with breathing anisotropy (i.e., with different coupling strength on the upward and downward triangles) on the kagome lattice. Our study relies on large scale tensor network simulations based on infinite projected entangled-pair state and infinite projected entangled-simplex state methods adapted to the kagome lattice. Our energy analysis suggests that the U(1) algebraic quantum spin-liquid (QSL) ground-state of the isotropic Heisenberg model is stable up to very large breathing anisotropy until it breaks down to a critical lattice-nematic phase that breaks rotational symmetry in real space through a first-order quantum phase transition. Our results also provide further insight into the recent experiment on vanadium oxyfluoride compounds which has been shown to be relevant platforms for realizing QSL in the presence of breathing anisotropy.
We believe that a necessary first step in understanding the ground state properties of the spin-${scriptstylefrac{1}{2}}$ kagome Heisenberg antiferromagnet is a better understanding of this models very large number of low energy singlet states. A description of the low energy states that is both accurate and amenable for numerical work may ultimately prove to have greater value than knowing only what these properties are, in particular when these turn on the delicate balance of many small energies. We demonstrate how this program would be implemented using the basis of spin-singlet dimerized states, though other bases that have been proposed may serve the same purpose. The quality of a basis is evaluated by its participation in all the low energy singlets, not just the ground state. From an experimental perspective, and again in light of the small energy scales involved, methods that can deliver all the low energy states promise more robust predictions than methods that only refine a fraction of these states.
The topological quantum spin liquids (SL) and the nature of quantum phase transitions between them have attracted intensive attentions for the past twenty years. The extended kagome spin-1/2 antiferromagnet emerges as the primary candidate for hosting both time reversal symmetry (TRS) preserving and TRS breaking SLs based on density matrix renormalization group simulations. To uncover the nature of the novel quantum phase transition between the SL states, we study a minimum XY model with the nearest neighbor (NN) ($J_{xy}$), the second and third NN couplings ($J_{2xy}=J_{3xy}=J_{xy}$). We identify the TRS broken chiral SL (CSL) with the turn on of a small perturbation $J_{xy}sim 0.06 J_{xy}$, which is fully characterized by the fractionally quantized topological Chern number and the conformal edge spectrum as the $ u=1/2$ fractional quantum Hall state. On the other hand, the NN XY model ($J_{xy}=0$) is shown to be a critical SL state adjacent to the CSL, characterized by the gapless spin singlet excitations and also vanishing small spin triplet excitations. The quantum phase transition from the CSL to the gapless critical SL is driven by the collapsing of the neutral (spin singlet) excitation gap. By following the evolution of entanglement spectrum, we find that the transition takes place through the coupling of the edge states with opposite chiralities, which merge into the bulk and become gapless neutral excitations. The effect of the NN spin-$z$ coupling $J_z$ is also studied, which leads to a quantum phase diagram with an extended regime for the gapless SL.
The spin-$frac{1}{2}$ kagome antiferromagnet is an archetypal frustrated system predicted to host a variety of exotic magnetic states. We show using neutron scattering measurements that deuterated vesignieite BaCu$_{3}$V$_{2}$O$_{8}$(OD)$_{2}$, a fully stoichiometric $S=1/2$ kagome magnet with $<$1% lattice distortion, orders magnetically at $T_{mathrm{N}}=9$K into a multi-k coplanar variant of the predicted triple-k octahedral structure. We find this structure is stabilized by a dominant antiferromagnetic 3$^{mathrm{rd}}$-neighbor exchange $J_3$ with minor 1$^{mathrm{st}}$- or 2$^{mathrm{nd}}$--neighbour exchange. The spin-wave spectrum is well described by a $J_3$-only model including a tiny symmetric exchange anisotropy.
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.
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