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Register a new userMagnetic ordering of the distorted kagome antiferromagnet Y$_3$Cu$_9$(OH)$_{18}$[Cl$_8$(OH)] prepared via optimal synthesis
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Experimental studies of high-purity kagome-lattice antiferromagnets (KAFM) are of great importance in attempting to better understand the predicted enigmatic quantum spin-liquid ground state of the KAFM model. However, realizations of this model can rarely evade magnetic ordering at low temperatures due to various perturbations to its dominant isotropic exchange interactions. Such a situation is for example encountered due to sizable Dzyaloshinskii-Moriya magnetic anisotropy in YCu$_3$(OH)$_6$Cl$_3$, which stands out from other KAFM materials by its perfect crystal structure. We find evidence of magnetic ordering also in the distorted sibling compound Y$_3$Cu$_9$(OH)$_{18}$[Cl$_8$(OH)], which has recently been proposed to feature a spin-liquid ground state arising from a spatially anisotropic kagome lattice. Our findings are based on a combination of bulk susceptibility, specific heat, and magnetic torque measurements that disclose a Neel transition temperature of $T_N=11$~K in this material, which might feature a coexistence of magnetic order and persistent spin dynamics as previously found in YCu$_3$(OH)$_6$Cl$_3$. Contrary to previous studies of single crystals and powders containing impurity inclusions, we use high-purity single crystals of Y$_3$Cu$_9$(OH)$_{18}$[Cl$_8$(OH)] grown via an optimized hydrothermal synthesis route that minimizes such inclusions. This study thus demonstrates that the lack of magnetic ordering in less pure samples of the investigated compound does not originate from the reduced symmetry of spin lattice but is instead of extrinsic origin.
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We present the crystal structure and magnetic properties of Y$_{3}$Cu$_{9}$(OH)$_{19}$Cl$_{8}$, a stoichiometric frustrated quantum spin system with slightly distorted kagome layers. Single crystals of Y$_{3}$Cu$_{9}$(OH)$_{19}$Cl$_{8}$ were grown under hydrothermal conditions. The structure was determined from single crystal X-ray diffraction and confirmed by neutron powder diffraction. The observed structure reveals two different Cu-positions leading to a slightly distored kagome layer in contrast to the closely related YCu$_{3}$(OH)$_{6}$Cl$_{3}$. Curie-Weiss behavior at high-temperatures with a Weiss-temperature $theta_{W}$ of the order of $-100$ K, shows a large dominant antiferromagnetic coupling within the kagome planes. Specific-heat and magnetization measurements on single crystals reveal an antiferromagnetic transition at T$_{N}=2.2$ K indicating a pronounced frustration parameter of $theta_{W}/T_{N}approx50$. Optical transmission experiments on powder samples and single crystals confirm the structural findings. Specific-heat measurements on YCu$_{3}$(OH)$_{6}$Cl$_{3}$ down to 0.4 K confirm the proposed quantum spin-liquid state of that system. Therefore, the two Y-Cu-OH-Cl compounds present a unique setting to investigate closely related structures with a spin-liquid state and a strongly frustrated AFM ordered state, by slightly releasing the frustration in a kagome lattice.
Spin liquids are exotic phases of quantum matter challenging Landaus paradigm of symmetry-breaking phase transitions. Despite strong exchange interactions, spins do not order or freeze down to zero temperature. While well-established for 1D quantum antiferromagnets, in higher dimension where quantum fluctuations are less acute, realizing and understanding such states represent major issues, both theoretical and experimental. In this respect the simplest nearest-neighbor Heisenberg antiferromagnet Hamiltonian on the highly frustrated kagome lattice has proven to be a fascinating and inspiring model. The exact nature of its ground state remains elusive and the existence of a spin-gap is the first key-issue to be addressed to discriminate between the various classes of proposed spin liquids. Here, through low-temperature Nuclear Magnetic Resonance (NMR) contrast experiments on high quality single crystals, we single out the kagome susceptibility and the corresponding dynamics in the kagome archetype, the mineral herbertsmithite, ZnCu$_3$(OH)$_6$Cl$_2$. We firmly conclude that this material does not harbor any spin-gap, which restores a convergence with recent numerical results promoting a gapless Dirac spin liquid as the ground state of the Heisenberg kagome antiferromagnet.
The magnetic ground state of the ideal quantum kagome antiferromagnet (QKA) has been a long-standing puzzle, mainly because perturbations to the nearest-neighbor isotropic Heisenberg Hamiltonian can lead to various fundamentally different ground states. Here we investigate a recently synthesized QKA representative YCu$_3$(OH)$_6$Cl$_3$, where perturbations commonly present in real materials, like lattice distortion and intersite ion mixing, are absent. Nevertheless, this compound enters a long-range magnetically ordered state below $T_N=15$ K. Our powder neutron diffraction experiment reveals that its magnetic structure corresponds to a coplanar $120^circ$ state with negative vector spin chirality. The ordered magnetic moments are suppressed to $0.42(2)mu_B$, which is consistent with the previously detected spin dynamics persisting to the lowest experimentally accessible temperatures. This indicates either a coexistence of magnetic order and disorder or the presence of strong quantum fluctuations in the ground state of YCu$_3$(OH)$_6$Cl$_3$. The origin of the magnetic order is sought in terms of Dzyaloshinskii-Moriya magnetic anisotropy and further-neighbor isotropic exchange interactions.
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.
We studied the magnetic properties of YCu$_3$(OH)$_6$Br$_2$[Br$_{1-x}$(OH)$_{x}$] ($x$ = 0.33 and 0.45), where Cu$^{2+}$ ions form two-dimensional kagome layers. There is no magnetic order down to 50 mK while the Curie-Weiss temperature is in the order of -100 K. At zero magnetic field, the low-temperature specific heat shows a $T^2$ dependence. Above 2 T, a linear-temperature dependence term in specific heat emerges, and the value of $gamma = C/T$ increases linearly with the field. Furthermore, the magnetic susceptibility tends to a constant value at $T = 0$. Our results suggest that the magnetic ground state of YCu$_3$(OH)$_6$Br$_2$[Br$_{1-x}$(OH)$_{x}$] is consistent with a Dirac quantum-spin-liquid state with linearly dispersing spinon strongly coupled with emergent gauge field, which has long been theoretically proposed as a candidate ground state in the two-dimensional kagome Heisenberg antiferromagnetic system.
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