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Register a new userSpecific Heat of the Kagome Antiferromagnet Herbertsmithite in High Magnetic Fields
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Added by
Quentin Barth\\'elemy
Publication date
2021
fields
Physics
and research's language is
English
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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.
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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.
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.
We have measured the specific heat of the coupled spin-dimer antiferromagnet Ba$_3$Mn$_2$O$_8$ to 50 mK in temperature and to 29 T in the magnetic field. The experiment extends to the midpoint of the field region (25.9 T $leq H leq$ 32.3 T) of the magnetization plateau at 1/2 of the saturation magnetization, and reveals the presence of three ordered phases in the field region between that of the magnetization plateau and the low-field spin-liquid region. The exponent of the phase boundary with the thermally disordered region is smaller than the theoretical value based on the Bose-Einstein condensation of spin triplets. At zero field and 29 T, the specific-heat data show gapped behaviors characteristic of spin liquids. The zero-field data indicate that the gapped triplet excitations form two levels whose energies differ by nearly a factor of two. At least the lower level is well localized. The data at 29 T reveal that the low-lying excitations at the magnetization plateau are weakly delocalized.
CeRhIn$_5$ is a prototypical antiferromagnetic heavy-fermion compound, whose behavior in a magnetic field is unique. A magnetic field applied in the basal plane of the tetragonal crystal structure induces two additional phase transitions. When the magnetic field is applied along, or close to, the $c$ axis, a new phase characterized by a pronounced in-plane electronic anisotropy emerges at $B^* approx$ 30 T, well below the critical field, $B_c simeq$ 50 T, to suppress the antiferromagnetic order. The exact origin of this new phase, originally suggested to be an electronic-nematic state, remains elusive. Here we report low-temperature specific-heat measurements in CeRhIn$_5$ in high static magnetic fields up to 36 T applied along both the $a$ and $c$ axes. For fields applied along the $a$ axis, we confirmed the previously suggested phase diagram, and extended it to higher fields. This allowed us to observe a triple point at $sim$ 30 T, where the first-order transition from an incommensurate to commensurate magnetic structure merges into the onset of the second-order antiferromagnetic transition. For fields applied along the $c$ axis, we observed a small but distinct anomaly at $B^*$, which we discuss in terms of a possible field-induced transition, probably weakly first-order. We further suggest that the transition corresponds to a change of magnetic structure. We revise magnetic phase diagrams of CeRhIn$_5$ for both principal orientations of the magnetic field based entirely on thermodynamic anomalies.
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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