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Register a new userMagnetization Plateau Observed by Ultra-High Field Faraday Rotation in a Kagome Antiferromagnet Herbertsmithite
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To capture the high-field magnetization process of herbertsmithite (ZnCu3(OH)6Cl2), Faraday rotation (FR) measurements were carried out on a single crystal in magnetic fields of up to 190 T. The magnetization data evaluated from the FR angle exhibited a saturation behavior above 150 T at low temperatures, which was attributed to the 1/3 magnetization plateau. The overall behavior of the magnetization process was reproduced by theoretical models based on the nearest-neighbor Heisenberg model. This suggests that herbertsmithite is a proximate kagome antiferromagnet hosting an ideal quantum spin liquid in the ground state. A distinguishing feature is the superlinear magnetization increase, which is in contrast to the Brillouin function-type increase observed by conventional magnetization measurements and indicates a reduced contribution from free spins located at the Zn sites to the FR signal.
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Measuring the specific heat of herbertsmithite single crystals in high magnetic fields (up to $34$ T) allows us to isolate the low-temperature kagome contribution while shifting away extrinsic Schottky-like contributions. The kagome contribution follows an original power law $C_{p}(Trightarrow0)propto T^{alpha}$ with $alphasim1.5$ and is found field-independent between $28$ and $34$ T for temperatures $1leq Tleq4$ K. These are serious constrains when it comes to replication using low-temperature extrapolations of high-temperature series expansions. We manage to reproduce the experimental observations if about $10$ % of the kagome sites do not contribute. Between $0$ and $34$ T, the computed specific heat has a minute field dependence then supporting an algebraic temperature dependence in zero field, typical of a critical spin liquid ground state. The need for an effective dilution of the kagome planes is discussed and is likely linked to the presence of copper ions on the interplane zinc sites. At very low temperatures and moderate fields, we also report some small field-induced anomalies in the total specific heat and start to elaborate a phase diagram.
Employing complementary torque magnetometry and electron spin resonance on single crystals of herbertsmithite, the closest realization to date of a quantum kagome antiferromagnet featuring a spin-liquid ground state, we provide novel insight into different contributions to its magnetism. At low temperatures, two distinct types of defects with different magnetic couplings to the kagome spins are found. Surprisingly, their magnetic response contradicts the three-fold symmetry of the ideal kagome lattice, suggesting the presence of a global structural distortion that may be related to the establishment of the spin-liquid ground state.
Despite tremendous investigations, a quantum spin liquid state realized in spin-1/2 kagome Heisenberg antiferromagnet remains largely elusive. In herbertsmithite ZnCu$_3$(OH)$_6$Cl$_2$, a quantum spin liquid candidate on the perfect kagome lattice, precisely characterizing the intrinsic physics of the kagome layers is extremely challenging due to the presence of interlayer Cu/Zn antisite disorder within its crystal structure. Here we measured the specific heat and thermal conductivity of single crystal herbertsmithite in magnetic fields with high resolution. Our results are highlighted by the excellent scaling collapse of the intrinsic magnetic specific heat contribution arising from the kagome layers as a function of $T/H$ (temperature/magnetic field). In addition, no residual linear term in the thermal conductivity $kappa/T(Trightarrow 0)$ is observed in zero and applied magnetic fields, indicating the absence of itinerant gapless excitations. These results suggest a new picture for a quantum spin liquid state of the kagome layers of herbertsmithite, wherein localized orphan spins arise and interact with random exchanges in conjunction with a non-itinerant quantum spin liquid.
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 have investigated spin-wave excitations in a magnetic-field-induced 1/5-magnetization plateau phase in a triangular lattice antiferromagnet CuFeO2 (CFO), by means of inelastic neutron scattering measurements under applied magnetic fields of up to 13.4 T. Comparing the observed spectra with the calculations in which spin-lattice coupling effects for the nearest neighbor exchange interactions are taken into account, we have determined the Hamiltonian parameters in the field-induced 1/5- plateau phase, which directly show that CFO exhibits a bond order associated with the magnetic structure in this phase.
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