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Spin chirality in antiferromagnets offers new opportunities for spintronics. The kagome antiferromagnet Mn3Sn is a paradigmatic material in which the antiferromagnetic order parameter can be detected and controlled by electrical means. However, direct investigation of the magnetic texture of Mn3Sn has been challenging because of the tiny moment hosted in its magnetic octupole, hindering further clarification of this unique material. Here, we address this issue by observing the stray magnetic field from Mn3Sn using a diamond quantum scanning magnetometer. The spatially-resolved intrinsic domains and domain walls in a high-quality single-crystalline Mn3Sn film quantitatively reveal the polarization angle of the magnetic octupole in the kagome plane, the domain's local magnetization, the domain wall's width and chirality, and the octupole order in domain walls. Our nanoscale investigation of Mn3Sn, a powerful complement to macroscopic measurements, paves the road for developing chiral antiferromagnetism and its potential for spintronic applications., Comment: 17 pages, 4 figures

We present a comprehensive study of the magnetoelastic properties of the Ising pyrochlore oxide Ho$_{2}$Ti$_{2}$O$_{7}$, known as spin ice, by means of high-field magnetostriction measurements and numerical calculations. When a magnetic field is applied along the crystallographic <111> axis, the longitudinal magnetostriction exhibits a broad maximum in the low-field regime around 30 T, followed by a dramatic lattice contraction due to crystal-field (CF) level crossing at $B_{\rm cf} \sim 65$ T. The transverse magnetostriction exhibits a contrasting behavior, highlighting the anisotropic nature of the CF striction. We identify distinct timescales of spin dynamics and CF-phonon dynamics by applying a magnetic field with different field-sweep rates. Our mean-field calculations, based on a point-charge model, successfully reproduce the overall magnetostriction behavior, revealing the competition between the exchange striction and CF striction. A signature of the CF level crossing is also observed through adiabatic magnetocaloric-effect measurements, consistent with our magnetostriction data., Comment: 10 pages, 8 figures

Two-dimensional (2D) van der Waals (vdW) materials have been an exciting area of research ever since scientists first isolated a single layer of graphene. Single layer magnetic materials can provide a pathway for vdW heterostructures with magnetic properties. While most of the magnetic vdW materials exhibit ordering transitions in the bulk, here we report a successful exfoliation of a triangular lattice S=1 antiferromagnet NiGa$_2$S$_4$, which already demonstrates exotic magnetism in the bulk material. We establish the number of layers of the material by atomic force microscopy (AFM) and detail a careful characterization using Raman and optical spectroscopy to demonstrate how the optical, electronic, and structural properties of NiGa$_2$S$_4$ change as a function of sample thickness. Optical measurements and electronic structure calculations of bulk versus monolayer NiGa$_2$S$_4$ confirm the material to be a Mott insulator with an electronic gap of about 1.5 eV, which slightly increases for layers below 10 L. We conclude with a theoretical analysis of the possibility of doping monolayer NiGa$_2$S$_4$ by proximity to a metal., Comment: 11 pages, 8 figures

The high-throughput calculation predicts that the Fe-based cubic ferromagnet Fe$_3$Si may exhibit a large anomalous Nernst effect (ANE). Here, we report our experimental observation of the large Nernst coefficient $S_{yx}\sim$2 $\mu$V/K and the transverse thermoelectric coefficient $-\alpha_{yx}$ $\sim$ 3 Am$^{-1}$K$^{-1}$ for Fe$_3$Si polycrystal at room temperature. The large $-\alpha_{yx}$ indicates that the large ANE originates from the intrinsic Berry curvature mechanism. The high Curie temperature of 840 K and the most abundant raw elements of Fe and Si make Fe$_3$Si a competitive candidate for Nernst thermoelectric generations., Comment: Accepted to Proceedings of the 15th Asia Pacific Physics Conference (APPC 15), Springer Nature

Kagome-lattice materials offer novel playgrounds of exploring topologically nontrivial states of electrons under influence of many-body interactions. A noncollinear kagome antiferromagnet Mn$_3$Sn has attracted particular interest for application in spintronics owing to the large anomalous Hall effect related to the Weyl dispersion near the Fermi energy. In addition, strong electronic correlation suggesting the Kondo physics has also been implied. However, the effect of correlation on the band topology and their interplay remains elusive. Here, we investigate nonequilibrium Hall transport in a photoexcited Mn$_3$Sn using time-resolved terahertz Faraday rotation spectroscopy. In equilibrium, Mn$_3$Sn is a bad metal close to the Mott-Ioffe-Regal limit with low carrier mobility, and thus only the anomalous Hall effect is discerned. By contrast, intense photoexcitation beyond an approximate threshold gives rise to a clear cyclotron resonance, namely the normal Hall effect, indicating the emergence of unusual carriers with 50 times lighter effective mass and 40 times less scattering. The lifetime of high-mobility carriers as long as a few tens of picoseconds and a threshold-like behavior for the pump fluence are hardly explained by contribution of photoexcited hot carriers. Instead, the emergence of unusual carriers may be accounted for by dielectric screening of the on-site Coulomb interaction by high-density delocalized photocarriers. A possible role of electronic correlation in equilibrium transport in Mn$_3$Sn beyond the single-particle picture is discussed., Comment: 28 pages, 6 figures

Studying superconductivity in Dirac semimetals is an important step in understanding quantum matter with topologically non-trivial order parameters. We report on the properties of the superconducting phase in single crystals of the Dirac material LaCuSb2 prepared by the self-flux method. We find that chemical and hydrostatic pressure drastically suppress the superconducting transition. Furthermore, due to large Fermi surface anisotropy, magnetization and muon spin relaxation measurements reveal Type-II superconductivity for applied magnetic fields along the $a$-axis, and Type-I superconductivity for fields along the $c$-axis. Specific heat confirms the bulk nature of the transition, and its deviation from single-gap $s$-wave BCS theory suggests multigap superconductivity. Our tight-binding model points to an anisotropic gap function arising from the spin-orbital texture near the Dirac nodes, providing an explanation for the appearance of an anomaly in specific heat well below $T_c$. Given the existence of superconductivity in a material harboring Dirac fermions, LaCuSb2 proves an interesting material candidate in the search for topological superconductivity., Comment: 58 pages, 5 main figures, supplemental information attached

Resonant ultrasound spectroscopy (RUS) is a powerful technique for measuring the full elastic tensor of a given material in a single experiment. Previously, this technique was limited to regularly-shaped samples such as rectangular parallelepipeds, spheres, and cylinders. We demonstrate a new method for determining the elastic moduli of irregularly-shaped samples, extending the applicability of RUS to a much larger set of materials. We apply this new approach to the recently-discovered unconventional superconductor UTe$_2$ and provide its elastic tensor at both 300 and 4 kelvin., Comment: 18 pages, 3 figures, 12 tables

Using Raman scattering spectroscopy, we uncover a complex magnetic behavior of Nd$_2$Ir$_2$O$_7$ , which stands out among magnetic pyrochlores by the lowest temperature of the all-in-all-out (AIAO) Ir moments ordering ($T^\mathrm{N}_{\small\rm{Ir}}=33$~K) and the highest temperature at which AIAO order of rare-earth Nd ions is detected ($T^\mathrm{*}_{\small\rm{Nd}}$=15~K). Our findings suggest that in the temperature range between 15~K and 33~K, Nd magnetic moments exhibit strong fluctuations, possibly originating from spin ice behavior. This complex behavior emerges from the interplay of strong spin-orbit coupling, electronic correlations, and geometric frustration on two magnetic pyrochlore sublattices of Nd and Ir ions. The ordering of Ir magnetic moments is accompanied by an appearance of one-magnon Raman modes at 26.3 and 29.6 meV compatible with the AIAO order and of a broad mode at 14 meV, which could be associated with spinon continuum arising from Nd spin ice fluctuations. While two one-magnon excitations show minimal temperature evolution with decreasing temperature, the 14 meV mode shifts to higher frequencies as the temperature approaches a crossover to Nd AIAO order, broadens, and disappears below 15~K. An additional two-magnon excitation of the AIAO Nd order at around 33 meV appears in the spectra at low temperatures. These rather high energies of magnetic excitations of Nd moments make Nd$_2$Ir$_2$O$_7$ a particularly attractive playground to study the rare-earth magnetism on the pyrochlore lattice.

Multipolar Kondo systems offer unprecedented opportunities for designing astonishing quantum phases and functionalities beyond spin-only descriptions. A model material platform of this kind is the cubic heavy-fermion system Pr$Tr_{2}$Al$_{20}$ ($Tr=$ Ti, V), which hosts a nonmagnetic crystal-electric-field (CEF) ground state and substantial Kondo entanglement of the local quadrupolar and octopolar moments with the conduction electron sea. Here, we explore magnetoresistance (MR) and Hall effect of PrTi$_{2}$Al$_{20}$ that develops ferroquadrupolar (FQ) order below $T_{Q} \sim 2$ K and compare its behavior with that of the non-4$f$ analog, LaTi$_{2}$Al$_{20}$. In the FQ ordered phase, PrTi$_{2}$Al$_{20}$ displays extremely large magnetoresistance (XMR) of $\sim 10^{3}\%$. The unsaturated, quasi-linear field ($B$) dependence of the XMR violates the conventional Kohler's scaling and defies description based on carrier compensation alone. By comparing the MR and the Hall effect observed in PrTi$_{2}$Al$_{20}$ and LaTi$_{2}$Al$_{20}$, we conclude that the open-orbit topology on the electron-type Fermi surface (FS) sheet is key for the observed XMR. The low-temperature MR and the Hall resistivity in PrTi$_{2}$Al$_{20}$ display pronounced anisotropy in the [111] and [001] magnetic fields, which is absent in LaTi$_{2}$Al$_{20}$, suggesting that the transport anisotropy ties in with the anisotropic magnetic-field response of the quadrupolar order parameter.

We investigate ultrafast dynamics of the anomalous Hall effect (AHE) in the topological antiferromagnet Mn3Sn with sub-100 fs time resolution. Optical pulse excitations largely elevate the electron temperature up to 700 K, and terahertz probe pulses clearly resolves ultrafast suppression of the AHE before demagnetization. The result is well reproduced by microscopic calculation of the intrinsic Berry-curvature mechanism while the extrinsic contribution is clearly excluded. Our work opens a new avenue for the study of nonequilibrium AHE to identify the microscopic origin by drastic control of the electron temperature by light.

Pyrochlore iridates are thought to be a fertile ground for the realization of topologically non-trivial and strongly correlated states of matter. Here we provide a compelling evidence of interacting Weyl electrons in Nd$_2$Ir$_2$O$_7$ and quadratic band touching in Pr$_2$Ir$_2$O$_7$ by Raman scattering. We observe a magnetically-driven phase transition between the topological Weyl semimetal and a Luttinger semimetal with quadratic band touching in Nd$_2$Ir$_2$O$_7$. Our theoretical analysis of the Raman scattering from Weyl and Luttinger quasiparticles agrees with experimental observations, and enables a characterization of the material parameters while revealing interaction and disorder effects through a relatively short quasiparticle lifetime., Comment: 8 pages, 3 figures; improved fitting of theory to experiment

The quest for topological states in strongly correlated materials is challenging but essential from fundamental research and application perspectives. The magnetic Weyl semimetal (WSM) state in the chiral antiferromagnet Mn$_3$Sn emerges with strong electronic correlations, offering an intriguing arena for exploring the interplay between Weyl fermions and correlation physics. One prominent characteristic of the WSM state is the chiral anomaly, yet the potential effects of electronic correlations on the chiral anomaly remain unexplored. Here, we report a comprehensive study of the in-plane magnetotransport properties of single-crystal Mn$_{3+x}$Sn$_{1-x}$ with three different Mn doping levels ($x=0.053$, 0.070, and 0.090). The excess Mn leads to glassy ferromagnetic behavior and the Kondo effect, aside from shifting the chemical potential relative to the Weyl nodes. Thus, systematic tuning of the Mn doping level enables us to study the interplay between the spin-fluctuation scatterings, the correlation effect, and the chiral anomaly. We identify negative longitudinal magnetoresistance and planar Hall effect specific to the chiral anomaly for all three doping levels, indicating that the chiral anomaly persists in the presence of strong correlations., Comment: 7 pages, 5 figures

We measure the full elastic tensors of Mn$_3$Ge and Mn$_3$Sn as a function of temperature through their respective antiferromagnetic phase transitions. Large discontinuities in the bulk moduli at the N\'eel transitions indicate strong magnetoelastic coupling in both compounds. Strikingly, the discontinuities are nearly a factor of 10 larger in Mn$_3$Ge than in Mn$_3$Sn. We use the magnitudes of the discontinuities to calculate the pressure derivatives of the N\'eel temperature, which are 39 K/GPa 14.3 K/GPa for Mn$_3$Ge and Mn$_3$Sn, respectively. We measured in-plane shear modulus $c_{66}$, which couples strongly to the magnetic order, in magnetic fields up to 18 T and found quantitatively similar behavior in both compounds. Recent measurements have demonstrated strong piezomagnetism in Mn$_3$Sn: our results suggest that Mn$_3$Ge may be an even better candidate for this effect., Comment: 17 pages, 8 figures

The frustrated magnet Nd$_2$Ir$_2$O$_7$, where strong correlations together with spin-orbit coupling play a crucial role, is predicted to be a Weyl semimetal and to host topological pairs of bulk Dirac-like valleys. Here we use an external magnetic field to manipulate the localized rare earth 4f moments coupled to the 5d electronic bands. Low energy optical spectroscopy reveals that a field of only a few teslas suffices to create charge compensating pockets of holes and electrons in different regions of momentum space, thus introducing a valley population shift that can be tuned with the field., Comment: 8 pages, 6 figures

Quantum electronic matter has long been understood in terms of two limiting behaviors of electrons: one of delocalized metallic states, and the other of localized magnetic states. Understanding the strange metallic behavior which develops at the brink of localization demands new probes of the underlying electronic charge dynamics. Using a state-of-the-art technique, synchrotron-radiation-based Mossbauer spectroscopy, we have studied the longitudinal charge fluctuations of the strange metal phase of beta-YbAlB4 as a function of temperature and pressure. We find that the usual single absorption peak in the Fermi-liquid regime splits into two peaks upon entering the critical regime. This spectrum is naturally interpreted as a single nuclear transition, modulated by nearby electronic valence fluctuations whose long time-scales are further enhanced, due to the formation of charged polarons. Our results represent a direct observation of critical charge fluctuations as a new signature of strange metals.

It has become common knowledge that phonons can generate thermal Hall effect in a wide variety of materials, although the underlying mechanism is still controversial. We study longitudinal $\kappa_{xx}$ and transverse $\kappa_{xy}$ thermal conductivity in Pr$_2$Ir$_2$O$_7$, which is a metallic analogue of spin ice. Despite the presence of mobile charge carriers, we find that both $\kappa_{xx}$ and $\kappa_{xy}$ are dominated by phonons. A $T/H$ scaling of $\kappa_{xx}$ unambiguously reveals that longitudinal heat current is substantially impeded by resonant scattering of phonons on paramagnetic spins. Upon cooling, the resonant scattering is strongly affected by a development of spin ice correlation and $\kappa_{xx}$ deviates from the scaling in an anisotropic way with respect to field directions. Strikingly, a set of the $\kappa_{xx}$ and $\kappa_{xy}$ data clearly shows that $\kappa_{xy}$ correlates with $\kappa_{xx}$ in its response to magnetic field including a success of the $T/H$ scaling and its failure at low temperature. This remarkable correlation provides solid evidence that an indispensable role is played by spin-phonon scattering not only for hindering the longitudinal heat conduction, but also for generating the transverse response., Comment: 18 pages, 4 figures

X-ray magnetic circular dichroism (XMCD) signals are usually absent in antiferromagnets. In this letter, we report the observation of spontaneous XMCD spectra originating from the inverse triangular spin structure, or the polarization of the cluster magnetic octupole, in the chiral antiferromagnet Mn$_{3}$Sn thin film. The result is consistent with the recent theoretical predictions that the inverse triangular spin structure can give rise to finite XMCD signals in the absence of net magnetization [J. Phys. Soc. Jpn. 89, 083703 (2020) and Phys. Rev. Lett. 126, 157402 (2021)].

A magnetic Weyl semimetal is a recent focus of extensive research as it may exhibit large and robust transport phenomena associated with topologically protected Weyl points in momentum space. Since a magnetic texture provides a handle for the configuration of the Weyl points and its transport response, understanding of magnetic dynamics should form a basis of future control of a topological magnet. Mn3Sn is an example of an antiferromagnetic Weyl semimetal that exhibits a large response comparable to the one observed in ferromagnets despite a vanishingly small magnetization. The non-collinear spin order in Mn3Sn can be viewed as a ferroic order of cluster magnetic octupole and breaks the time-reversal symmetry, stabilizing Weyl points and the significantly enhanced Berry curvature near the Fermi energy. Here we report our first observation of time-resolved octupole oscillation in Mn3Sn. In particular, we find the giant effective damping of the octupole dynamics, and it is feasible to conduct an ultrafast switching at < 10 ps, a hundred times faster than the case of spin-magnetization in a ferromagnet. Moreover, high domain wall velocity over 10 km/s is theoretically predicted. Our work paves the path towards realizing ultrafast electronic devices using the topological antiferromagnet.

Magnetic materials with pyrochlore crystal structure form exotic magnetic states due to the high lattice frustration. In this work we follow the effects of coupling of the lattice and electronic and magnetic degrees of freedom in two Praseodymium-based pyrochlores Pr$_2$Zr$_2$O$_7$ and Pr$_2$Ir$_2$O$_7$. In both materials the presence of magnetic interactions does not lead to magnetically ordered low temperature states, however their electronic properties are different. A comparison of Raman phonon spectra of Pr$_2$Zr$_2$O$_7$ and Pr$_2$Ir$_2$O$_7$ allows us to identify magneto-elastic coupling in Pr$_2$Zr$_2$O$_7$ that elucidates its magnetic properties at intermediate temperatures, and allows us to characterize phonon-electron coupling in the semimetallic Pr$_2$Ir$_2$O$_7$. We also show that the effects of random disorder on the Raman phonon spectra is small., Comment: 6 pages, 5 figures

The Hall effect, in which current flows perpendicular to an applied electrical bias, has played a prominent role in modern condensed matter physics over much of the subject's history. Appearing variously in classical, relativistic and quantum guises, it has among other roles contributed to establishing the band theory of solids, to research on new phases of strongly interacting electrons, and to the phenomenology of topological condensed matter. The dissipationless Hall current requires time-reversal symmetry breaking. For over a century it has either been ascribed to externally applied magnetic field and referred to as the ordinary Hall effect, or ascribed to spontaneous non-zero total internal magnetization (ferromagnetism) and referred to as the anomalous Hall effect. It has not commonly been associated with antiferromagnetic order. More recently, however, theoretical predictions and experimental observations have identified large Hall effects in some compensated magnetic crystals, governed by neither of the global magnetic-dipole symmetry breaking mechanisms mentioned above. The goals of this article are to systematically organize the present understanding of anomalous antiferromagnetic materials that generate a non-zero Hall effect, which we will call anomalous Hall antiferromagnets, and to discuss this class of materials in a broader fundamental and applied research context. Our motivation in drawing attention to anomalous Hall antiferromagnets is two-fold. First, since Hall effects that are not governed by magnetic dipole symmetry breaking are at odds with the traditional understanding of the phenomenon, the topic deserves attention on its own. Second, this new reincarnation has again placed the Hall effect in the middle of an emerging field of physics at the intersection of multipole magnetism, topological condensed matter, and spintronics., Comment: 21 pages, 6 figures, 1 table

We report the results of our experimental studies on the magnetic, transport and thermoelectric properties of the ferromagnetic metal CoMnSb. Sizable anomalous Hall conductivity $\sigma_{yx}$ and transverse thermoelectric conductivity $\alpha_{yx}$ are found experimentally and comparable in size to the values estimated from density-functional theory. Our experiment further reveals that CoMnSb exhibits $-T\ln T$ critical behavior in $\alpha_{yx}(T)$, deviating from Fermi liquid behavior $\alpha_{yx}\sim T$ over a decade of temperature between 10 K to 400 K, similar to ferromagnetic Weyl and nodal-line semimetals. Our theoretical calculation for CoMnSb also predicts the $-T\ln T$ behavior when the Fermi energy locates near the Weyl nodes in momentum space., Comment: 6 pages, 4 figures

Pr$_2$Zr$_2$O$_7$ is a pyrochlore quantum spin-ice candidate. Using Raman scattering spectroscopy we probe crystal electric field excitations of Pr$^{3+}$, and demonstrate the importance of their interactions with the lattice. We identify a vibronic interaction with a phonon that leads to a splitting of a doublet crystal field excitation at around 55~meV. We also probe a splitting of the non-Kramers ground state doublet of Pr$^{3+}$ by observing a double line of the excitations to the first excited singlet state $E^0_g \rightarrow A_{1g}$. We show that the splitting has a strong temperature dependence, with the doublet structure most prominent between 50~K and 100~K, and the weight of one of the components strongly decreases on cooling. We suggest a static or dynamic deviation of Pr$^{3+}$ from the position in the ideal crystal structure can be the origin of the effect, with the deviation strongly decreasing at low temperatures., Comment: 6 pages, 3 figures

The recent discoveries of strikingly large zero-field Hall and Nernst effects in antiferromagnets Mn$_3$$X$, ($X$ = Sn, Ge) have brought the study of magnetic topological states to the forefront of condensed matter research and technological innovation. These effects are considered fingerprints of Weyl nodes residing near the Fermi energy, promoting Mn$_3$$X$, ($X$ = Sn, Ge) as a fascinating platform to explore the elusive magnetic Weyl fermions. In this review, we provide recent updates on the insights drawn from experimental and theoretical studies of Mn$_3$$X$, ($X$ = Sn, Ge) by combining previous reports with our new, comprehensive set of transport measurements of high-quality Mn$_3$Sn and Mn$_3$Ge single crystals. In particular, we report magnetotransport signatures specific to chiral anomalies in Mn$_3$Ge and planar Hall effect in Mn$_3$Sn, which have not yet been found in earlier studies. The results summarized here indicate the essential role of magnetic Weyl fermions in producing the large transverse responses in the absence of magnetization., Comment: 40 pages, 6 figures

We present a method for measuring thermal expansion under tunable uniaxial stresses, and show measurements of the thermal expansion of Mn$_3$Sn, a room temperature antiferromagnet that exhibits a spontaneous Hall effect, under uniaxial stresses of up to 1.51 GPa compression. Measurement of thermal expansion provides thermodynamic data about the nature of phase transitions, and uniaxial stress provides a powerful tuning method that does not introduce disorder. Mn$_3$Sn exhibits an anomaly in its thermal expansion near $\sim$270 K, associated with a first-order change in its magnetic structure. We show this transition temperature is suppressed by 54.6 K by 1.51 GPa compression along [0001]. We find the associated entropy change at the transition to be $\sim$ 0.1 J mol$^{-1}$ K$^{-1}$ and to vary only weakly with applied stress.

We use scanning tunneling microscopy/spectroscopy (STM/S) to elucidate the atomically resolved electronic structure in strongly correlated topological kagome magnet Mn$_3$Sn. In stark contrast to its broad single-particle electronic structure, we observe a pronounced resonance with a Fano line shape at the Fermi level resembling the many-body Kondo resonance. We find that this resonance does not arise from the step edges or atomic impurities, but the intrinsic kagome lattice. Moreover, the resonance is robust against the perturbation of a vector magnetic field, but broadens substantially with increasing temperature, signaling strongly interacting physics. We show that this resonance can be understood as the result of geometrical frustration and strong correlation based on the kagome lattice Hubbard model. Our results point to the emergent many-body resonance behavior in a topological kagome magnet., Comment: Includes Supplementary Materials. To appear in Phys. Rev. Lett (2020)

Electrical manipulation of emergent phenomena due to nontrivial band topology is a key to realize next-generation technology using topological protection. A Weyl semimetal is a three-dimensional gapless system that hosts Weyl fermions as low-energy quasiparticles. It exhibits various exotic phenomena such as large anomalous Hall effect (AHE) and chiral anomaly, which have robust properties due to the topologically protected Weyl nodes. To manipulate such phenomena, the magnetic version of Weyl semimetals would be useful as a magnetic texture may provide a handle for controlling the locations of Weyl nodes in the Brillouin zone. Moreover, given the prospects of antiferromagnetic (AF) spintronics for realizing high-density devices with ultrafast operation, it would be ideal if one could electrically manipulate an AF Weyl metal. However, no report has appeared on the electrical manipulation of a Weyl metal. Here we demonstrate the electrical switching of a topological AF state and its detection by AHE at room temperature. In particular, we employ a polycrystalline thin film of the AF Weyl metal Mn$_3$Sn, which exhibits zero-field AHE. Using the bilayer device of Mn$_3$Sn and nonmagnetic metals (NMs), we find that an electrical current density of $\sim 10^{10}$-$10^{11}$ A/m$^2$ in NMs induces the magnetic switching with a large change in Hall voltage, and besides, the current polarity along a bias field and the sign of the spin Hall angle $\theta_{\rm SH}$ of NMs [Pt ($\theta_{\rm SH} > 0$), Cu($\theta_{\rm SH} \sim 0$), W ($\theta_{\rm SH} < 0$)] determines the sign of the Hall voltage. Notably, the electrical switching in the antiferromagnet is made using the same protocol as the one used for ferromagnetic metals. Our observation may well lead to another leap in science and technology for topological magnetism and AF spintronics., Comment: 49 pages, 14 figures

Magnetic fluctuations induced by geometric frustration of local Ir-spins disturb the formation of long range magnetic order in the family of pyrochlore iridates, R$_{2}$Ir$_{2}$O$_{7}$ (R = lanthanide)$^{1}$. As a consequence, Pr$_{2}$Ir$_{2}$O$_{7}$ lies at a tuning-free antiferromagnetic-to-paramagnetic quantum critical point and exhibits a diverse array of complex phenomena including Kondo effect, biquadratic band structure, metallic spin-liquid (MSL), and anomalous Hall effect$^{2-5}$. Using spectroscopic imaging with the scanning tunneling microscope, complemented with machine learning K-means clustering analysis, density functional theory, and theoretical modeling, we probe the local electronic states in single crystal of Pr$_{2}$Ir$_{2}$O$_{7}$ and discover an electronic phase separation. Nanoscale regions with a well-defined Kondo resonance are interweaved with a non-magnetic metallic phase with Kondo-destruction. Remarkably, the spatial nanoscale patterns display a correlation-driven fractal geometry with power-law behavior extended over two and a half decades, consistent with being in proximity to a critical point. Our discovery reveals a new nanoscale tuning route, viz. using a spatial variation of the electronic potential as a means of adjusting the balance between Kondo entanglement and geometric frustration., Comment: Nature Communications (in press)

Both the Jahn-Teller distortion of Cu$^{2+}$O$_6$ octahedra and magnetic ordering are absent in hexagonal Ba$_3$CuSb$_2$O$_9$ suggesting a Cu 3$d$ spin-orbital liquid state. Here, by means of resonant x-ray scattering and absorption experiment, we show that oxygen 2$p$ holes play crucial role in stabilizing this spin-orbital liquid state. These oxygen holes appear due to the "reaction" Sb$^{5+}$$\rightarrow$Sb$^{3+}$ $+$ two oxygen holes, with these holes being able to attach to Cu ions. The hexagonal phase with oxygen 2$p$ holes exhibits also a novel charge-orbital dynamics which is absent in the orthorhombic phase of Ba$_3$CuSb$_2$O$_9$ with Jahn-Teller distortion and Cu 3$d$ orbital order. The present work opens up a new avenue towards spin-charge-orbital entangled liquid state in transition-metal oxides with small or negative charge transfer energy., Comment: 21 pages, 6 figures

NiGa$_2$S$_4$ is a triangular lattice S=1 system with strong two-dimensionality of the lattice, actively discussed as a candidate to host spin-nematic order brought about by strong quadrupole coupling. Using Raman scattering spectroscopy we identify a phonon of E$_g$ symmetry which can modulate magnetic exchange $J_1$ and produce quadrupole coupling. Additionally, our Raman scattering results demonstrate a loss of local inversion symmetry on cooling, which we associate with sulfur vacancies. This will lead to disordered Dzyaloshinskii-Moriya interactions, which can prevent long range magnetic order. Using magnetic Raman scattering response we identify 160~K as a temperature of an upturn of magnetic correlations. The temperature below 160~K, but above 50~K where antiferromagnetic magnetic start to increase, is a candidate for spin-nematic regime.

The origin of intrinsic quantum criticality in the heavy-fermion superconductor $\beta$-YbAlB$_4$ has been attributed to strong Yb valence fluctuations and its peculiar crystal structure. Here, we assess these contributions individually by studying the isostructural but fixed-valence compound $\beta$-LuAlB$_4$. Quantum oscillation measurements and DFT calculations reveal a Fermi surface markedly different from that of $\beta$-YbAlB$_4$, consistent with a `large' Fermi surface there. We also find an unexpected in-plane anisotropy of the electronic structure, in contrast to the isotropic Kondo hybridization in $\beta$-YbAlB$_4$., Comment: 6 pages, 4 figures

The off-diagonal (electric, thermal and thermoelectric) transport coefficients of a solid can acquire an anomalous component due to the non-trivial topology of the Bloch waves. We present a study of the anomalous Hall (AHE), Nernst (ANE) and thermal Hall effects (ATHE) in the Heusler Weyl ferromagnet Co$_2$MnGa. The Anomalous Wiedemann-Franz law, linking electric and thermal responses, was found to be valid over the whole temperature window. This indicates that the AHE has an intrinsic origin and the Berry spectrum is smooth in the immediate vicinity of the Fermi level. From the ANE data, we extract the magnitude and temperature dependence of $\alpha^A_{ij}$ and put under scrutiny the $\alpha^A_{ij}/\sigma^A_{ij}$ ratio, which approaches k$_B$/e at room temperature. We show that in various topological magnets the room-temperature magnitude of this ratio is a sizeable fraction of k$_B$/e and argue that the two anomalous transverse coefficients depend on universal constants, the Berry curvature averaged over a window set by either the Fermi wavelength (for Hall) or the de Broglie thermal length (for Nernst). Since the ratio of the latter two is close to unity at room temperature, such a universal scaling finds a natural explanation in the intrinsic picture of anomalous transverse coefficients., Comment: 5 pages, 4 figures, supplemental material included

Antiferromagnetic spin motion at terahertz (THz) frequencies attracts growing interests for fast spintronics, however their smaller responses to external field inhibit device application. Recently the noncollinear antiferromagnet Mn$_3$Sn, a Weyl semimetal candidate, was reported to show large anomalous Hall effect (AHE) at room temperature comparable to ferromagnets. Dynamical aspect of such large responses is an important issue to be clarified for future THz data processing. Here the THz anomalous Hall conductivity in Mn$_3$Sn thin films is investigated by polarization-resolved spectroscopy. Large anomalous Hall conductivity Re $\sigma_{xy} (\omega) \sim$ 20 $\rm{\Omega^{-1} cm^{-1}}$ at THz frequencies is clearly observed as polarization rotation. In contrast, Im $\sigma_{xy} (\omega)$ is small up to a few THz, showing that the AHE remains dissipationless over a large frequency range. A peculiar temperature dependence corresponding to the breaking/recovery of symmetry in the spin texture is also discussed. Observation of the THz AHE at room temperature demonstrates the ultrafast readout for the antiferromagnetic spintronics using Mn$_3$Sn and will also open new avenue for studying nonequilibrium dynamics in Weyl antiferromagnets.

Ferro-quadrupole (FQ) order in the non-Kramers $\Gamma_3$ doublet system PrTi$_2$Al$_{20}$ has been investigated via angle-resolved measurements of the specific heat, rotational magnetocaloric effect, and entropy, under a rotating magnetic field within the $(1\bar{1}0)$ plane. The FQ transition occurring at 2 K is robust when the magnetic field $B$ is applied precisely along the $[111]$ direction. By contrast, the magnetic field of larger than 1 T tilted away from the $[111]$ direction sensitively changes the FQ transition to a crossover. The energy gap between the ground and first-excited states in the FQ order increases remarkably with the magnetic field in $B \parallel [001]$, but hardly depends on the magnetic-field strength, at least up to 5 T, in the field orientation between the $[111]$ and $[110]$ axes. These features can be reproduced by using a phenomenological model for FQ order assuming an anisotropic field-dependent interaction between quadrupoles, which has been recently proposed to explain the field-induced first-order phase transition in PrTi$_2$Al$_{20}$. The present study demonstrates the great potential of the field-angle-resolved measurements for evaluating possible scenarios for multipole orders., Comment: 5 pages, 5 figures (main text) + 4 pages, 2 figures (supplemental material), accepted for publication in J. Phys. Soc. Jpn

Heavy fermion metals hosting multipolar local moments set a new stage for exploring exotic spin-orbital entangled quantum phases. In such systems, the quadrupolar Kondo effect serves as the key ingredient in the orbital-driven non-Fermi liquid (NFL) behavior and quantum critical phenomena. The cubic heavy fermion superconductor Pr$Tr_2$Al$_{20}$ ($Tr$: Ti, V) is a prime candidate for realizing the quadrupolar Kondo lattice. Here, we present a systematic study of the NFL phenomena in PrV$_2$Al$_{20}$ based on magnetoresistance (MR), magnetic susceptibility and specific heat measurements. Upon entering the NFL regime, we observe a universal scaling behavior expected for the quadrupolar Kondo lattice in PrV$_2$Al$_{20}$, which indicates a prominent role of the quadrupolar Kondo effect in driving the NFL behavior. Deviations from this scaling relation occur below $\sim 8$ K, accompanied by a sign change in the MR and a power-law divergence in the specific heat. This anomalous low-temperature state points to the presence of other mechanisms which are not included in the theory, such as heavy fermion coherence or multipolar quantum critical fluctuations., Comment: 14 pages, 4 figures

We report magnetic-field-induced first-order phase transitions in the ferro-quadrupole (FQ) ordered state of PrTi2Al20, in which non-Kramers Pr3+ ions with two 4f electrons have a non-magnetic Gamma3 doublet ground state in the cubic Td crystalline electric field. For magnetic fields along [111], 27Al-NMR and magnetization experiments reveal Qz \propto 3z2-r2 type FQ order below 2 K independent of field strength. Magnetic fields along [001] or [110], however, induce discontinuous switching of order parameters within the two dimensional space spanned by Qz and Qx \propto x2-y2 at small field values less than a few tesla. A symmetry-based theoretical analysis shows that the transitions can be caused by competition between the magnetic Zeeman interaction and anisotropy in the quadrupole-quadrupole interactions, if the latter dominates over the former in low fields and vice versa in high fields. Furthermore, striking violation of proportionality between NMR Knight shift and magnetic susceptibility is observed in the symmetry-broken FQ phases, indicating significant influence of FQ order on the hybridization between conduction and f electrons, which in turn mediates the RKKY-type quadrupole interaction causing the FQ order. This feedback effect may be a specific feature of quadrupole orders not commonly observed in magnetic phase transitions and play a key role for inducing the discontinuous transitions., Comment: 20 pages, 21 figures

Intermetallic compounds containing $f$-electron elements have been prototypical materials for investigating strong electron correlations and quantum criticality (QC). Their heavy fermion ground state evoked by the magnetic $f$-electrons is susceptible to the onset of quantum phases, such as magnetism or superconductivity, due to the enhanced effective mass ($m^{*}$) and a corresponding decrease of the Fermi temperature. However, the presence of $f$-electron valence fluctuations to a non-magnetic state is regarded an anathema to QC, as it usually generates a paramagnetic Fermi-liquid state with quasiparticles of moderate $m^{*}$. Such systems are typically isotropic, with a characteristic energy scale $T_0$ of the order of hundreds of kelvins that require large magnetic fields or pressures to promote a valence or magnetic instability. Here we show that the intermediate valence compound $\alpha$-YbAlB$_4$ surprisingly exhibits both quantum critical behaviour and a Lifshitz transition under low magnetic field, which is attributed to the anisotropy of the hybridization between the conduction and localized $f$-electrons. These findings suggest a new route to bypass the large valence energy scale in developing the QC., Comment: 18 pages, 15 figures (3 panels)

The anomalous Hall effect (AHE), a Hall signal occurring without an external magnetic field, is one of the most significant phenomena. However, understanding the AHE mechanism has been challenging and largely restricted to ferromagnetic metals. Here, we investigate the recently discovered AHE in the chiral antiferromagnet Mn3Sn by measuring a thermal analog of the AHE, known as an anomalous thermal Hall effect (ATHE). The amplitude of the ATHE scales with the anomalous Hall conductivity of Mn3Sn over a wide temperature range, demonstrating that the AHE of Mn3Sn arises from a dissipationless intrinsic mechanism associated with the Berry curvature. Moreover, we find that the dissipationless AHE is significantly stabilized by shifting the Fermi level toward the magnetic Weyl points. Thus, in Mn3Sn, the Berry curvature emerging from the proposed magnetic Weyl fermion state is a key factor for the observed AHE and ATHE., Comment: 28 pages, 8 figures

Broken symmetries in solids involving higher order multipolar degrees of freedom are historically referred to as "hidden orders" due to the formidable task of detecting them with conventional probes. Examples of such hidden orders include spin-nematic order in quantum magnets, and quadrupolar or higher multipolar orders in various correlated quantum materials. In this work, we theoretically propose that the study of magnetostriction provides a powerful and novel tool to directly detect higher-order multipolar symmetry breaking $-$ such as the elusive octupolar order $-$ by examining its scaling behaviour with respect to an applied magnetic field $h$. As an illustrative example, we examine such key scaling signatures in the context of Pr-based cage compounds with strongly correlated $f$-electrons, Pr(Ti,V,Ir)$_2$(Al,Zn)$_{20}$, whose low energy degrees of freedom are composed of purely higher-order multipoles: quadrupoles $\mathcal{O}_{20,22}$ and octupole $\mathcal{T}_{xyz}$. Employing a symmetry-based Landau theory of multipolar moments coupled to lattice strain fields, we demonstrate that a magnetic field applied along the [111] direction results in a length change with a distinct linear-in-$h$ scaling behaviour, accompanied by hysteresis, below the octupolar ordering temperature. We show that the resulting "magnetostriction coefficient" is directly proportional to the octupolar order parameter, providing the first clear access to this subtle order parameter. Along other field directions, we show that the field dependence of the magnetostriction provides a window into quadrupolar orders. Our work provides a springboard for future experimental and theoretical investigations of multipolar orders and their quantum phase transitions in a wide variety of systems., Comment: 10 pages (including References), 5 figures, 3 pages Supplementary Information

We have probed the crystalline electric-field ground states of pure $|J = 7/2, J_z = \pm 5/2\rangle$ as well as the anisotropic $c$-$f$ hybridization in both valence fluctuating systems $\alpha$- and $\beta$-YbAlB$_4$ by linear polarization dependence of angle-resolved core level photoemission spectroscopy. Interestingly, the small but distinct difference between \abyb was found in the polar angle dependence of linear dichroism, indicating the difference in the anisotropy of $c$-$f$ hybridization which may be essential to a heavy Fermi liquid state in $\alpha$-YbAlB$_4$ and a quantum critical state in $\beta$-YbAlB$_4$.

The Weyl antiferromagnet Mn$_3$Sn has recently attracted significant attention as it exhibits various useful functions such as large anomalous Hall effect that are normally absent in antiferromagnets. Here we report the thin film fabrication of the single phase of Mn$_3$Sn and the observation of the large anomalous Hall effect at room temperature despite its vanishingly small magnetization. Our work on the high-quality thin film growth of the Weyl antiferromagnet paves the path for developing the antiferromagnetic spintronics., Comment: 13 pages, 4 figures, to appear in Applied Physics Letters

Structure with orbital degeneracy is unstable toward spontaneous distortion. Such orbital correlation usually has a much higher energy scale than spins, and therefore, magnetic transition takes place at a much lower temperature, almost independently from orbital ordering. However, when the energy scales of orbitals and spins meet, there is a possibility of spin-orbital entanglement that would stabilize novel ground state such as spin-orbital liquid and random singlet state. Here we review on such a novel spin-orbital magnetism found in the hexagonal perovskite oxide Ba$_3$CuSb$_2$O$_9$, which hosts a self-organized honeycomblike short-range order of a strong Jahn-Teller ion Cu$^{2+}$. Comprehensive structural and magnetic measurements have revealed that the system has neither magnetic nor Jahn-Teller transition down to the lowest temperatures, and Cu spins and orbitals retain the hexagonal symmetry and paramagnetic state. Various macroscopic and microscopic measurements all indicate that spins and orbitals remain fluctuating down to low temperatures without freezing, forming a spin-orbital entangled liquid state., Comment: 33 pages, 17 figures, 1 table, to appear in Journal of Physics: Condensed Matter (topical review)