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Quantum spin liquids (QSLs) represent an exotic quantum many-body state characterized by the suppression of long-range magnetic order due to strong quantum fluctuations. The kagome spin-1/2 antiferromagnet (AFM) is a prime candidate for realizing QSLs, but its ground state remains an unresolved conundrum. Here we investigate the recently discovered perfect kagome AFM YCu$_3$(OH)$_{6.5}$Br$_{2.5}$ to elucidate two central enigmas surrounding the kagome AFM. Ultra-sensitive torque magnetometry experiments reveal that the intrinsic magnetic susceptibility arising from the kagome layer remains nearly temperature-independent down to exceedingly low temperatures. This observation seemingly implies the emergence of gapless fermionic spin excitations akin to Pauli paramagnetism in metals. However, most strikingly, these results stand in stark contrast to the conspicuous absence of a temperature-linear contribution to the specific heat. These findings appear irreconcilable with the widely-discussed theoretical frameworks assuming fermionic quasiparticles (QPs), instead suggesting a transition of bosonic QPs into a superfluid state with a gapless Goldstone mode. Furthermore, magnetocaloric measurements evince an entropy anomaly, constituting thermodynamic evidence that magnetic fields instigate the opening of a spin gap, driving a quantum phase transition into a 1/9 magnetization plateau state. These results shed light on the nature of the low-energy excitations in zero and strong magnetic fields, providing crucial insights into the long-standing unresolved issues of the ground state of the kagome AFM., Comment: 23 pages, 9 figures

The spin-1/2 Heisenberg antiferromagnet on an anisotropic triangular lattice (ATL) is an archetypal spin system hosting exotic quantum magnetism and dimensional crossover. However, the progress in experimental research on this field has been limited due to the scarcity of ideal model materials. Here, we show that rhenium oxyhalides $A_{3}$ReO$_{5}X_{2}$, where spin-1/2 Re$^{6+}$ ions form a layered structure of ATLs, allow for flexible chemical substitution in both cation $A^{2+}$ ($A$ = Ca, Sr, Ba, Pb) and anion $X^{-}$ ($X$ = Cl, Br) sites, leading to seven synthesizable compounds. By combining magnetic susceptibility and high-field magnetization measurements with theoretical calculations using the orthogonalized finite-temperature Lanczos method, we find that the anisotropy $J'/J$ ranges from 0.25 to 0.45 depending on the chemical composition. Our findings demonstrate that $A_{3}$ReO$_{5}X_{2}$ is an excellent platform for realizing diverse effective spin Hamiltonians that differ in the strength of the anisotropy $J'/J$ as well as the relevance of perturbation terms such as the Dzyaloshinskii-Moriya interaction and interlayer exchange coupling., Comment: 11 pages, 5 figures, SM: 4 pages, 2 figures

We developed a resistance measurement using radio frequency reflection to investigate the electrical transport characteristics under destructive pulsed magnetic fields above 100 T. A homemade flexible printed circuit for a sample stage reduced the noise caused by the induced voltage from the pulsed magnetic fields, improving the accuracy of the measurements of the reflected waves. From the obtained reflectance data, the absolute value of the magnetoresistance was successfully determined by using a phase analysis with admittance charts. These developments enable more accurate and comprehensive measurements of electrical resistance in pulsed magnetic fields., Comment: 7 pages, 5 figures

We investigate the crystallographic and magnetic properties of a chromium-based thiospinel CuGaCr$_{4}$S$_{8}$. From a synchrotron x-ray diffraction experiment and structural refinement, Cu and Ga atoms are found to occupy the tetrahedral $A$-sites in an alternate way, yielding breathing pyrochlore Cr network. CuGaCr$_{4}$S$_{8}$ undergoes a magnetic transition associated with a structural distortion at 31 K in zero magnetic field, indicating that the spin-lattice coupling is responsible for relieving the geometrical frustration. When applying a pulsed high magnetic field, a sharp metamagnetic transition takes place at 40 T, followed by a 1/2-magnetization plateau up to 103 T. These phase transitions accompany dielectric anomalies, suggesting the presence of helical spin correlations in low-field phases. The density-functional-theory calculation reveals that CuGaCr$_{4}$S$_{8}$ is dominated by antiferromagnetic and ferromagnetic exchange couplings within small and large tetrahedra, respectively, in analogy with CuInCr$_{4}$S$_{8}$. We argue that $A$-site-ordered Cr thiospinels serve as an excellent platform to explore diverse magnetic phases along with pronounced magnetoelastic and magnetodielectric responses., Comment: 12 pages, 13 figures

The mutual coupling of spin and lattice degrees of freedom is ubiquitous in magnetic materials and potentially creates exotic magnetic states in response to the external magnetic field. Particularly, geometrically frustrated magnets serve as a fertile playground for realizing magnetic superstructure phases. Here, we observe an unconventional two-step magnetostructural transition prior to a half-magnetization plateau in a breathing pyrochlore chromium spinel by means of state-of-the-art magnetization and magnetostriction measurements in ultrahigh magnetic fields available up to 600 T. Considering a microscopic magnetoelastic theory, the intermediate-field phase can be assigned to a magnetic superstructure with a three-dimensional periodic array of 3-up-1-down and canted 2-up-2-down spin molecules. We attribute the emergence of the magnetic superstructure to a unique combination of the strong spin-lattice coupling and large breathing anisotropy., Comment: 10 pages, 5 figures, SI: 15 pages, 14 figures

We have performed magnetic torque and resistivity measurements on a centrosymmetric skyrmion-host GdRu2Si2, in which the dominant magnetic interaction leading to skyrmion formation is under debate. We observe both the de Haas-van Alphen and Shubnikov-de Haas oscillations in the forced ferromagnetic phase. The angular dependence of the quantum oscillation frequencies can be reproduced by the ab-initio calculation. The de Haas-van Alphen oscillation is also observed in the double-Q phase with a different frequency to that in the forced ferromagnetic phase, indicating a Fermi surface reconstruction due to the coupling between localized spins and conduction electrons. Based on these experimental findings, the magnetic interactions in this system are discussed., Comment: 11 pages, 8 figures

The phonon magnetochiral effect (MChE) is the nonreciprocal acoustic and thermal transports of phonons caused by the simultaneous breaking of the mirror and time-reversal symmetries. So far, the phonon MChE has been observed only in a ferrimagnetic insulator Cu2OSeO3, where the nonreciprocal response disappears above the Curie temperature of 58 K. Here, we study the nonreciprocal acoustic properties of a room-temperature ferromagnet Co9Zn9Mn2 for unveiling the phonon MChE close to the room temperature. Surprisingly, the nonreciprocity in this metallic compound is enhanced at higher temperatures and observed up to 250 K. This clear contrast between insulating Cu2OSeO3 and metallic Co9Zn9Mn2 suggests that metallic magnets have a mechanism to enhance the nonreciprocity at higher temperatures. From the ultrasound and microwave-spectroscopy experiments, we conclude that the magnitude of the phonon MChE of Co9Zn9Mn2 mostly depends on the magnon bandwidth, which increases at low temperatures and hinders the magnon-phonon hybridization. Our results suggest that the phonon nonreciprocity could be further enhanced by engineering the magnon band of materials., Comment: 6 pages, 4 figures, 1 table

The observation of spinon excitations in the $S=\frac{1}{2}$ triangular antiferromagnet Ca$_3$ReO$_5$Cl$_2$ reveals a quasi-one-dimensional (1D) nature of magnetic correlations, in spite of the nominally 2D magnetic structure. This phenomenon is known as frustration-induced dimensional reduction. Here, we present high-field electron spin resonance spectroscopy and magnetization studies of Ca$_3$ReO$_5$Cl$_2$, allowing us not only to refine spin-Hamiltonian parameters, but also to investigate peculiarities of its low-energy spin dynamics. We argue that the presence of the uniform Dzyaloshinskii-Moriya interaction (DMI) shifts the spinon continuum in momentum space and, as a result, opens a zero-field gap at the $\Gamma$ point. We observed this gap directly. The shift is found to be consistent with the structural modulation in the ordered state, suggesting this material as a perfect model triangular-lattice system, where a pure DMI-spiral ground state can be realized.

Under magnetic fields, quantum magnets often undergo exotic phase transitions with various kinds of order. The discovery of a sequence of fractional magnetization plateaus in the Shastry-Sutherland compound SrCu2(BO3)2 has played a central role in the high-field research on quantum materials, but so far this system could only be probed up to half the saturation value of the magnetization. Here, we report the first experimental and theoretical investigation of this compound up to the saturation magnetic field of 140 T and beyond. Using ultrasound and magnetostriction techniques combined with extensive tensor-network calculations (iPEPS), several spin-supersolid phases are revealed between the 1/2 plateau and saturation (1/1 plateau). Quite remarkably, the sound velocity of the 1/2 plateau exhibits a drastic decrease of -50%, related to the tetragonal-to-orthorhombic instability of the checkerboard-type magnon crystal. The unveiled nature of this paradigmatic quantum system is a new milestone for exploring exotic quantum states of matter emerging in extreme conditions., Comment: 8 pages, 4 figures, 2 tables

Frustrated magnets with a strong spin-lattice coupling can show rich magnetic phases and the associated fascinating phenomena. A promising platform is the breathing pyrochlore magnet CuInCr$_{4}$S$_{8}$ with localized $S=3/2$ Cr$^{3+}$ ions, which is proposed to be effectively viewed as an $S=6$ Heisenberg antiferromagnet on the face-centered-cubic lattice. Here, we unveil that CuInCr$_{4}$S$_{8}$ exhibits a complex magnetic phase diagram with a small phase pocket ($A$ phase) by means of magnetization, magnetostriction, magnetocapacitance, and magnetocaloric-effect measurements in pulsed high magnetic fields of up to 60 T. Remarkably, the appearance of $A$ phase is accompanied by anomalous magnetostrictive and magnetocapacitive responses, suggesting the emergence of helimagnetism in contrast to the neighboring commensurate magnetic phases. Besides, the high-entropy nature is confirmed in the high-temperature side of $A$ phase. These features are potentially related to a thermal fluctuation-driven multiple-$q$ state caused by the magnetic frustration, which has been theoretically predicted but yet experimentally undiscovered., Comment: 13 pages, 12 figures. Published in Phys. Rev. Research

We studied the acoustic properties of liquid oxygen up to 90 T by means of ultrasound measurements. We observed a monotonic decrease of the sound velocity and an asymptotic increase of the sound attenuation when applying magnetic fields. The unusual attenuation, twenty times as large as the zero-field value, suggests strong fluctuations of the local molecular arrangement. We point out that the observed fluctuations are related to a liquid-liquid transition or crossover, from a small-magnetization to a large-magnetization liquid, which is characterized by a local-structure rearrangement. To investigate higher-field properties of liquid oxygen, we performed single-turn-coil experiments up to 180 T by means of the acoustic, dilatometric, magnetic, and optical techniques. We observed only monotonic changes of these properties, reflecting the absence of the proposed liquid-liquid transition in our experimental conditions., Comment: 10 pages, 10 figures. arXiv admin note: text overlap with arXiv:1906.01207

Single-turn coil (STC) technique is a convenient way to generate ultrahigh magnetic fields of more than 100 T. During the field generation, the STC explosively destructs outward due to the Maxwell stress and Joule heating. Unfortunately, the STC does not work at its full potential because it has already expanded when the maximum magnetic field is reached. Here, we propose an easy way to delay the expansion and increase the maximum field by using a mass-loaded STC. By loading clay on the STC, the field profile drastically changes, and the maximum field increases by 4 %. This method offers an access to higher magnetic fields for physical property measurements., Comment: 6 pages, 5 figures, Accepted in Review of Scientific Instruments

The specific heat $C$ of the cuprate superconductors La$_{2-x}$Sr$_x$CuO$_4$ and Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+\delta}$ was measured at low temperature (down to $0.5~{\rm K}$), for dopings $p$ close to $p^\star$, the critical doping for the onset of the pseudogap phase. A magnetic field up to $35~{\rm T}$ was applied to suppress superconductivity, giving direct access to the normal state at low temperature, and enabling a determination of $C_e$, the electronic contribution to the normal-state specific heat, at $T \to 0$. In La$_{2-x}$Sr$_x$CuO$_4$ at $x=p = 0.22$, $0.24$ and $0.25$, $C_e / T = 15-16~{\rm mJmol}^{-1}{\rm K}^{-2}$ at $T = 2~{\rm K}$, values that are twice as large as those measured at higher doping ($p > 0.3$) and lower doping ($p < 0.15$). This confirms the presence of a broad peak in the doping dependence of $C_e$ at $p^\star\simeq 0.19$, as previously reported for samples in which superconductivity was destroyed by Zn impurities. Moreover, at those three dopings, we find a logarithmic growth as $T \to 0$, such that $C_e / T \sim {\rm B}\ln(T_0/T)$. The peak vs $p$ and the logarithmic dependence vs $T$ are the two typical thermodynamic signatures of quantum criticality. In the very different cuprate Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+\delta}$, we again find that $C_e / T \sim {\rm B}\ln(T_0/T$) at $p \simeq p^\star$, strong evidence that this $\ln(1/T)$ dependence - first discovered in the cuprates La$_{1.8-x}$Eu$_{0.2}$Sr$_x$CuO$_4$ and La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ - is a universal property of the pseudogap critical point. All four materials display similar values of the $\rm B$ coefficient, indicating that they all belong to the same universality class., Comment: 8 pages, 6 figures

Combined experimental and modeling studies of the magnetocaloric effect, ultrasound, and magnetostriction were performed on single-crystal samples of the spin-dimer system Sr$_3$Cr$_2$O$_8$ in large magnetic fields, to probe the spin-correlated regime in the proximity of the field-induced XY-type antiferromagnetic order also referred to as a Bose-Einstein condensate of magnons. The magnetocaloric effect, measured under adiabatic conditions, reveals details of the field-temperature ($H,T$) phase diagram, a dome characterized by critical magnetic fields $H_{c1}$ = 30.4 T, $H_{c2}$ = 62 T, and a single maximum ordering temperature $T_{{\rm max}}(45~$T$)\simeq$8 K. The sample temperature was observed to drop significantly as the magnetic field is increased, even for initial temperatures above $T_{{\rm max}}$, indicating a significant magnetic entropy associated to the field-induced closure of the spin gap. The ultrasound and magnetostriction experiments probe the coupling between the lattice degrees of freedom and the magnetism in Sr$_3$Cr$_2$O$_8$. Our experimental results are qualitatively reproduced by a minimalistic phenomenological model of the exchange-striction by which sound waves renormalize the effective exchange couplings., Comment: 9 pages, 14 figures

Viscosity measurements in combination with pulsed magnetic fields are developed by use of a quartz-crystal microbalance (QCM). When the QCM is immersed in liquid, the resonant frequency, $f_0$, and the quality factor, $Q$, of the QCM change depending on $(\rho\eta)^{0.5}$, where $\rho$ is the mass density and $\eta$ the viscosity. During the magnetic-field pulse, $f_0$ and $Q$ of the QCM are simultaneously measured by a ringdown technique. The typical resolution of $(\rho\eta)^{0.5}$ is 0.5 %. As a benchmark, the viscosity of liquid oxygen is measured up to 55 T., Comment: 5 pages, 5 figures

We report a high-resolution terahertz spectroscopic study of quantum spin dynamics in the antiferromagnetic Heisenberg-Ising spin-chain compound BaCo$_2$V$_2$O$_8$ as a function of temperature and longitudinal magnetic field. Confined spinon excitations are observed in an antiferromagnetic phase below $T_N\simeq 5.5$ K. In a field-induced gapless phase above $B_c=3.8$ T, we identify many-body string excitations as well as low-energy fractional psinon/antipsinon excitations by comparing to Bethe-Ansatz calculations. In the vicinity of $B_c$, the high-energy string excitations are found to be dynamically dominant over the fractional excitations., Comment: 6 pages, 4 figures

We investigate the low-temperature magnetic properties of the molecule-based chiral spin chain [Cu(pym)(H$_2$O)$_4$]SiF$_6\cdot$H$_2$O (pym = pyrimidine). Electron-spin resonance, magnetometry and heat capacity measurements reveal the presence of staggered $g$ tensors, a rich low-temperature excitation spectrum, a staggered susceptibility and a spin gap that opens on the application of a magnetic field. These phenomena are reminiscent of those previously observed in non-chiral staggered chains, which are explicable within the sine-Gordon quantum-field theory. In the present case, however, although the sine-Gordon model accounts well for the form of the temperature-dependence of the heat capacity, the size of the gap and its measured linear field dependence do not fit with the sine-Gordon theory as it stands. We propose that the differences arise due to additional terms in the Hamiltonian resulting from the chiral structure of [Cu(pym)(H$_2$O)$_4$]SiF$_6\cdot$H$_2$O, particularly a uniform Dzyaloshinskii-Moriya coupling and a four-fold periodic staggered field., Comment: 6 pages, 3 figures and supplemental information

We report on magnetization, sound velocity, and magnetocaloric-effect measurements of the Ising-like spin-1/2 antiferromagnetic chain system BaCo$_2$V$_2$O$_8$ as a function of temperature down to 1.3 K and applied transverse magnetic field up to 60 T. While across the N\'{e}el temperature of $T_N\sim5$ K anomalies in magnetization and sound velocity confirm the antiferromagnetic ordering transition, at the lowest temperature the field-dependent measurements reveal a sharp softening of sound velocity $v(B)$ and a clear minimum of temperature $T(B)$ at $B^{c,3D}_\perp=21.4$ T, indicating the suppression of the antiferromagnetic order. At higher fields, the $T(B)$ curve shows a broad minimum at $B^c_\perp = 40$ T, accompanied by a broad minimum in the sound velocity and a saturation-like magnetization. These features signal a quantum phase transition which is further characterized by the divergent behavior of the Gr\"{u}neisen parameter $\Gamma_B \propto (B-B^{c}_\perp)^{-1}$. By contrast, around the critical field, the Gr\"{u}neisen parameter converges as temperature decreases, pointing to a quantum critical point of the one-dimensional transverse-field Ising model., Comment: Phys. Rev. Lett., to appear

The Kondo-lattice compound CeRhIn$_5$ displays a field-induced Fermi surface reconstruction at $B^*\approx30$ T, which occurs within the antiferromagnetic state, prior to the quantum critical point at $B_{c0}\approx50$ T. Here, in order to investigate the nature of the Fermi surface change, we measured the magnetostriction, specific heat, and magnetic torque of CeRhIn$_5$ across a wide range of magnetic fields. Our observations uncover the field-induced itineracy of the $4f$ electrons, where above $B_{\rm onset}\approx17$ T there is a significant enhancement of the Sommerfeld coefficient, and spin-dependent effective cyclotron masses determined from quantum oscillations. Upon crossing $B_{\rm onset}$, the temperature dependence of the specific heat also shows distinctly different behavior from that at low fields. Our results indicate that the Kondo coupling is remarkably robust upon increasing the magnetic field. This is ascribed to the delocalization of the $4f$ electrons at the Fermi surface reconstruction at $B^*$., Comment: 7 pages, 4 figures

Conventional, thermally-driven continuous phase transitions are described by universal critical behaviour that is independent of the specific microscopic details of a material. However, many current studies focus on materials that exhibit quantum-driven continuous phase transitions (quantum critical points, or QCPs) at absolute zero temperature. The classification of such QCPs and the question of whether they show universal behaviour remain open issues. Here we report measurements of heat capacity and de Haas-van Alphen (dHvA) oscillations at low temperatures across a field-induced antiferromagnetic QCP (B$_{c0}\simeq$ 50 T) in the heavy-fermion metal CeRhIn$_5$. A sharp, magnetic-field-induced change in Fermi surface is detected both in the dHvA effect and Hall resistivity at B$_0^*\simeq$ 30 T, well inside the antiferromagnetic phase. Comparisons with band-structure calculations and properties of isostructural CeCoIn$_5$ suggest that the Fermi-surface change at B$_0^*$ is associated with a localized to itinerant transition of the Ce-4f electrons in CeRhIn$_5$. Taken in conjunction with pressure data, our results demonstrate that at least two distinct classes of QCP are observable in CeRhIn$_5$, a significant step towards the derivation of a universal phase diagram for QCPs., Comment: 30 pages, including Supporting Information. appears in PNAS, Early Edition published on January 5, 2015

The crystal structures of Ni$X_2$(pyz)$_2$ ($X$ = Cl (\textbf{1}), Br (\textbf{2}), I (\textbf{3}) and NCS (\textbf{4})) were determined at 298~K by synchrotron X-ray powder diffraction. All four compounds consist of two-dimensional (2D) square arrays self-assembled from octahedral NiN$_4$$X_2$ units that are bridged by pyz ligands. The 2D layered motifs displayed by \textbf{1}-\textbf{4} are relevant to bifluoride-bridged [Ni(HF$_2$)(pyz)$_2$]$Z$F$_6$ ($Z$ = P, Sb) which also possess the same 2D layers. In contrast, terminal $X$ ligands occupy axial positions in \textbf{1}-\textbf{4} and cause a staggering of adjacent layers. Long-range antiferromagnetic order occurs below 1.5 (Cl), 1.9 (Br and NCS) and 2.5~K (I) as determined by heat capacity and muon-spin relaxation. The single-ion anisotropy and $g$ factor of \textbf{2}, \textbf{3} and \textbf{4} are measured by electron spin resonance where no zero--field splitting was found. The magnetism of \textbf{1}-\textbf{4} crosses a spectrum from quasi-two-dimensional to three-dimensional antiferromagnetism. An excellent agreement was found between the pulsed-field magnetization, magnetic susceptibility and $T_\textrm{N}$ of \textbf{2} and \textbf{4}. Magnetization curves for \textbf{2} and \textbf{4} calculated by quantum Monte Carlo simulation also show excellent agreement with the pulsed-field data. \textbf{3} is characterized as a three-dimensional antiferromagnet with the interlayer interaction ($J_\perp$) slightly stronger than the interaction within the two-dimensional [Ni(pyz)$_2$]$^{2+}$ square planes ($J_\textrm{pyz}$)., Comment: 17 pages, 12 figures