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We present a single-crystal neutron diffraction study on the Shastry-Sutherland lattice system TbB$_4$ at zero magnetic field and under pulsed high magnetic fields up to 35 T applied along the crystallographic $c$ axis. While our results confirm the magnetic structures at zero-field as well as those at the half- and full-magnetization plateaus, they offer new insight into the $\frac{2}{9}$- and $\frac{1}{3}$-magnetization plateaus observed in this system. A stripe model of polarized 4-spin-plaquettes whose stripe density proportionally increases with the macroscopic magnetization is in full agreement with the neutron diffraction data. Equally well suited alternative models exist which explain the observed Bragg peaks which are inherently limited in a pulsed high magnetic field experiment. We discuss the different intensity distribution in $Q$ space which can be used to distinguish these models in future experiments.

Kondo insulators have recently aroused great interest because they are promising materials that host a topological insulator state caused by the strong electron interactions. Moreover, recent observations of the quantum oscillations in the insulating state of Kondo insulators have come as a great surprise. Here, to investigate the surface electronic state of a prototype Kondo insulator YbB$_{12}$, we measured transport properties of single crystals and microstructures. In all samples, the temperature dependence of the electrical resistivity is insulating at high temperatures and the resistivity exhibits a plateau at low temperatures. The magnitude of the plateau value decreases with reducing sample thickness, which is quantitatively consistent with the surface electronic conduction in the bulk insulating YbB$_{12}$. Moreover, the magnetoresistance of the microstructures exhibits a weak-antilocalization effect at low field. These results are consistent with the presence of topologically protected surface state, suggesting that YbB$_{12}$ is a candidate material of the topological Kondo insulator. The high field resistivity measurements up to $\mu_0H$ = 50 T of the microstructures provide supporting evidence that the quantum oscillations of the resistivity in YbB$_{12}$ occurs in the insulating bulk., Comment: This is the version of the article before peer review or editing, as submitted by an author to Journal of Physics D: Applied Physics. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at 10.1088/1361-6463/ac10d9

In heavy fermions the relaxation dynamics of photoexcited carriers has been found to be governed by the low energy indirect gap, E$_{g}$, resulting from hybridization between localized moments and conduction band electrons. Here, carrier relaxation dynamics in a prototype Kondo insulator YbB${}_{12}$ is studied over large range of temperatures and over three orders of magnitude. We utilize the intrinsic non-linearity of dynamics to quantitatively determine microscopic parameters, such as electron-hole recombination rate. The extracted value reveals that hybridization is accompanied by a strong charge transfer from localized 4f-levels. The results imply the presence of a hybridization gap up to temperatures of the order of E$_{g}$/k$_{B}\approx200$ K, which is extremely robust against electronic excitation. Finally, below 20 K the data reveal changes in the low energy electronic structure, attributed to short-range antiferromagnetic correlations between the localized levels.

We performed high-magnetic-field ultrasonic experiments on YbB$_{12}$ up to 59 T to investigate the valence fluctuations in Yb ions. In zero field, the longitudinal elastic constant $C_{11}$, the transverse elastic constants $C_{44}$ and $\left( C_{11} - C_{12} \right)/2$, and the bulk modulus $C_\mathrm{B}$ show a hardening with a change of curvature at around 35 K indicating a small contribution of valence fluctuations to the elastic constants. When high magnetic fields are applied at low temperatures, $C_\mathrm{B}$ exhibits a softening above a field-induced insulator-metal transition signaling field-induced valence fluctuations. Furthermore, at elevated temperatures, the field-induced softening of $C_\mathrm{B}$ takes place at even lower fields and $C_\mathrm{B}$ decreases continuously with field. Our analysis using the multipole susceptibility based on a two-band model reveals that the softening of $C_\mathrm{B}$ originates from the enhancement of multipole-strain interaction in addition to the decrease of the insulator energy gap. This analysis indicates that field-induced valence fluctuations of Yb cause the instability of the bulk modulus $C_\mathrm{B}$., Comment: 15 pages, 11 figures

Quantum oscillations (QOs) in transport and thermodynamic parameters at high magnetic fields are an unambiguous signature of the Fermi surface, the defining characteristic of a metal. Therefore, recent observations of QOs in insulating SmB$_6$ and YbB$_{12}$, in particular the QOs of the resistivity $\rho_{xx}$ in YbB$_{12}$, have been a big surprise, pointing to the formation of a novel state of quantum matter. Despite the large charge gap inferred from the insulating behaviour of $\rho_{xx}$, these compounds seemingly host a Fermi surface at high magnetic fields. However, the nature of the ground state in zero field has been little explored. Here we report the use of low-temperature heat-transport measurements to discover gapless, itinerant, charge-neutral excitations in the ground state of YbB$_{12}$. At zero field, despite $\rho_{xx}$ being far larger than that of conventional metals, a sizable linear temperature dependent term in the thermal conductivity is clearly resolved in the zero-temperature limit ($\kappa_{xx}/T(T\rightarrow0)=\kappa_{xx}^0/T\neq0$). Such a residual $\kappa_{xx}^0/T$ term at zero field, which is absent in SmB$_6$, leads to a spectacular violation of the Wiedemann-Franz law: the Lorenz ratio $L=\kappa_{xx}\rho_{xx}/T$ is $10^{4}$-$10^{5}$ times larger than that expected in conventional metals. These data indicate that YbB$_{12}$ is a charge insulator but a thermal metal, suggesting the presence of itinerant neutral fermions. Remarkably, more insulating crystals with larger activation energies exhibit a larger amplitude of the resistive QOs as well as a larger $\kappa_{xx}^0/T$, in stark contrast to conventional metals. Moreover, we find that these fermions couple to magnetic field, despite their charge neutrality. Our findings expose novel gapless and highly itinerant, charge-neutral quasiparticles in this unconventional quantum state., Comment: 7 pages, 4 figures. This is the original submitted version. Final version is accepted for publication in Nature Physics

In metals, orbital motions of conduction electrons on the Fermi surface are quantized in magnetic fields, which is manifested by quantum oscillations in electrical resistivity. This Landau quantization is generally absent in insulators. Here we report a notable exception in an insulator, ytterbium dodecaboride (YbB12). Despite much larger than that of metals, the resistivity of YbB12 exhibits profound quantum oscillations. This unconventional oscillation is shown to arise from the insulating bulk, yet the temperature dependence of their amplitude follows the conventional Fermi liquid theory of metals. The large effective masses indicate the presence of Fermi surface consisting of strongly correlated electrons. Our result reveals a mysterious bipartite ground state of YbB12: it is both a charge insulator and a strongly correlated metal., Comment: This is the original submitted version

The peculiar metallic electronic states observed in the Kondo insulator, samarium hexaboride (SmB$_6$), has stimulated considerable attention among those studying non-trivial electronic phenomena. However, experimental studies of these states have led to controversial conclusions mainly to the difficulty and inhomogeneity of the SmB$_6$ crystal surface. Here, we show the detailed electronic structure of SmB$_6$ with angle-resolved photoelectron spectroscopy measurements of the three-fold (111) surface where only two inequivalent time-reversal-invariant momenta (TRIM) exist. We observe the metallic two-dimensional state was dispersed across the bulk Kondo gap. Its helical in-plane spin polarisation around the surface TRIM suggests that SmB$_6$ is topologically non-trivial, according to the topological classification theory for weakly correlated systems. Based on these results, we propose a simple picture of the controversial topological classification of SmB$_6$., Comment: 34 pages, 4 figures for main text; 9 figures for supplementary material

We report a systematic study of Sm valence in the prototypical intermediate valence compound SmB$_6$. Sm mean valence, $v_{\rm Sm}$, was measured by X-ray absorption spectroscopy as functions of pressure ($1

DyB4 has a two-dimensional Shastry-Sutherland (Sh-S) lattice with strong Ising character of the Dy ions. Despite the intrinsic frustrations, surprisingly, it undergoes two successive transitions: a magnetic ordering at TN = 20K, and a quadrupole ordering at TQ=12.5 K. From high-resolution neutron and synchrotron X-ray powder diffraction studies, we have obtained full structural information on this material in all phases, and demonstrate that structural modifications occurring at quadrupolar transition lead to the lifting of frustrations inherent in the Sh-S model. Our study thus provides a complete experimental picture of how the intrinsic frustration of the Sh-S lattice can be lifted by the coupling to quadrupole moments. We show that two other factors, i.e. strong spin-orbit coupling and long-range RKKY interaction in metallic DyB4, play an important role in this behavior., Comment: 12 pages, 3 figures Physical Review B, accepted

Recent studies suggest that an exemplary Kondo insulator SmB6 belongs to a new class of topological insulators (TIs), in which non-trivial spin-polarized metallic states emerge on surface upon the formation of Kondo hybridization gap in the bulk. Remarkably, the bulk resistivity reaches more than 20 Ohm cm at 4 K, making SmB6 a candidate for a so-called bulk-insulating TI. We here investigate optical-pulse responses of SmB6 by pump-and-probe photoemission spectroscopy. Surface photovoltage effect is observed below ~90 K. This indicates that an optically-active band bending region develops beneath the novel metallic surface upon the bulk-gap evolution. The photovoltaic effect persists for >200 microsec, which is long enough to be detected by electronics devices, and could be utilized for optical gating of the novel metallic surface.

A detailed low-energy electronic structure of a Kondo insulator YbB$_{12}$ was revealed by a synergetic combination of ultrahigh-resolution laser photoemission spectroscopy (PES) and time-resolved PES. The former confirmed a 25-meV pseudogap corresponding to the Kondo temperature of this material, and more importantly, it revealed that a 15-meV gap and a Kondo-peak feature developed below a crossover temperature $T^\ast \sim 110$ K. In harmony with this, the latter discovered a very long recombination time exceeding 100 ps below $\sim$$T^\ast$. This is a clear manifestation of photoexcited carriers due to the bottleneck in the recovery dynamics, which is interpreted as a developing hybridization gap of a hard gap., Comment: 6 pages, 4 figures, revised version accepted for publication in PRB Rapid Communications

We investigate the pressure effect of the electrical resistivity and magnetization of Ce$_{0.8}$La$_{0.2}$B$_{6}$. The situation in which phase IV stably exists inside phase II at H=0 T could be realized by applying a pressure above $P\sim 1.1$ GPa. This originates from the fact that the stability of phase II under pressure is larger than those of phases IV and III. The results seem to be difficult to reproduce by taking the four interactions of $\Gamma_{\mathrm{5u}}$-type AFO, $O_{xy}$-type AFQ, $T_{xyz}$-type AFO, and AF exchange into account within a mean-field calculation framework., Comment: 4 pages, 5 figures, to appear in J. Phys. Soc. Jpn. 79 (2010) No.7

Dependence of the spectral functions on temperature and rare-earth substitution was examined in detail for Kondo semiconductor alloys Sm1-xEuxB6 and Yb1-xLuxB12 by bulk-sensitive photoemission. It is found that the 4f lattice coherence and intrinsic (small) energy gap are robust for SmB6 against the Eu substitution up to x = 0.15 while both collapse by Lu substitution already at x = 0.125 for YbB12. Our results suggest that the mechanism of the intrinsic gap formation is different between SmB6 and YbB12 although they were so far categorized in the same kind of Kondo semiconductors., Comment: 5 pages, 3 figures

We performed optical-pump terahertz-probe measurements of a Mott insulator YTiO$_{3}$ and a band semiconductor Si using a laser diode (1.47 eV) and a femtosecond pulse laser (1.55 eV). Both samples possess long energy-relaxation times (1.5 ms for YTiO$_{3}$ and 15 $\mu$s for Si); therefore, it is possible to extract terahertz complex conductivities of photoinduced carriers under equilibrium. We observed highly contrasting behavior - Drude conductivity in Si and localized conductivity possibly obeying the Jonscher law in YTiO$_{3}$. The carrier number at the highest carrier-concentration layer in YTiO$_{3}$ is estimated to be 0.015 per Ti site. Anisotropic conductivity of YTiO$_{3}$ is determined. Our study indicates that localized carriers might play an important role in the incipient formation of photoinduced metallic phases in Mott insulators. In addition, this study shows that the transfer-matrix method is effective for extracting an optical constant of a sample with a spatially inhomogeneous carrier distribution., Comment: 16 pages,7 figures, to appear in J. Phys.: Condens. Matter

We have performed a single crystal neutron scattering experiment on Ce0.7La0.3B6 to investigate the order parameter of phase IV microscopically. Below the phase transition temperature 1.5 K of phase IV, weak but distinct superlattice reflections at the scattering vector (h/2,h/2,l/2) (h, l = odd number) have been observed by neutron scattering for the first time. The intensity of the superlattice reflections is stronger for high scattering vectors, which is quite different from the usual magnetic form factor of magnetic dipoles. This result directly evidences that the order parameter of phase IV has a complex magnetization density, consistent with the recent experimental and theoretical prediction in which the order parameter is the magnetic octupoles Tbeta with Gamma5 symmetry of point group Oh. Neutron scattering experiments using short wavelength neutrons, as done in this study, could become a general method to study the high-rank multipoles in f electron systems., Comment: 4 pages, 4 figures

The thermopower, S, of CexR1-xB6 (R=La, Pr, Nd) was investigated. S with a positive sign shows a typical behavior observed in the Ce Kondo system, an increase with decreasing temperature at high temperatures and a maximum at low temperatures. The S values of all the systems at high temperatures are roughly linearly dependent on the Ce concentration, indicating the conservation of the single-impurity character of the Kondo effect in a wide x range. However, the maximum value of S, S_max, and the temperature, T_max, at which S_max is observed exhibit different x dependences between CexLa1-xB6 and CexR1-xB6 (R=Pr, Nd). In CexLa1-xB6, T_max, which is ~8 K in CeB6, decreases with decreasing x and converges to ~1 K in a very dilute alloy and S_max shows an increase below x ~ 0.1 after decreasing with decreasing x. In CexR1-xB6 (R=Pr, Nd), T_max shows a weak x dependence but S_max shows a roughly linear decrease in x. These results are discussed from the standpoint of the chemical pressure effect and the Ce-Ce interaction. S in the long-range ordered phase shows very different behavior between CexPr1-xB6 and CexNd1-xB6., Comment: PDF file, 7 pages with 9 figures, accepted for publication

Optical conductivity [$\sigma(\omega)$] of the Kondo semiconductor YbB$_{12}$ has been measured over wide ranges of temperature ($T$=8$-$690 K) and photon energy ($\hbar \omega \geq$ 1.3 meV). The $\sigma(\omega)$ data reveal the entire crossover of YbB$_{12}$ from a metallic electronic structure at high $T$ into a semiconducting one at low $T$. Associated with the gap development in $\sigma(\omega)$, a clear onset is newly found at $\hbar\omega$=15 meV for $T \leq$ 20 K. The onset energy is identified as the gap width of YbB$_{12}$ appearing in $\sigma(\omega)$. This gap in \sigma(\omega)$ is interpreted as the indirect gap, which has been predicted in the band model of Kondo semiconductor. On the other hand, the strong mid-infrared (mIR) peak observed in $\sigma(\omega)$ is interpreted as arising from the direct gap. The absorption coefficient around the onset and the mIR peak indeed show characteristic energy dependences expected for indirect and direct optical transitions in conventional semiconductors., Comment: 4 pages, 3 figures, submitted to J. Phys. Soc. Jpn

The spin dynamics of mixed-valence YbB12 has been studied by inelastic neutron scattering on a high-quality single crystal. In the Kondo-insulating regime realized at low temperature, the spectra exhibit a spin-gap structure with two sharp, dispersive, in-gap excitations at E = 14.5 and approximately 20 meV. The lower mode is shown to be associated with short-range correlations near the antiferromagnetic wave vector q0 = (1/2, 1/2, 1/2). Its properties are in overall agreement with those expected for a "spin exciton'' branch in an indirect hybridization gap semiconductor., Comment: 4 pages, 4 figures ; submitted to Physical Review Letters

We have performed the bulk-sensitive high-resolution soft x-ray photoemission study of a Kondo semiconductor CeRhAs and related compounds CeNiSn and CePdSn. The comparison of the spectra of polycrystalline CePdSn on the fractured and scraped surfaces shows that the fracturing of the samples is much better than the scraping in order to obtain intrinsic photoemission spectra. The Ce 4d core-level spectra show clear differences in the electronic states among the materials., Comment: 4 pages including 3 figures, to appear in Journal of Electron Spectroscopy and Related Phenomena

We report the electrical resistivity, Hall coefficient, thermoelectric power, specific heat, and thermal conductivity on single crystals of the type-VIII clathrate Ba8Ga16Sn30 grown from Sn-flux. Negative S and R_H over a wide temperature range indicate that electrons dominate electrical transport properties. Both rho(T) and S(T) show typical behavior of a heavily doped semiconductor. The absolute value of S increases monotonically to 243 uV/K with increasing temperature up to 550 K. The large S may originate from the low carrier concentration n=3.7x10^19 cm^(-3). Hall mobility u_H shows a maximum of 62 cm^2/Vs around 70 K. The analysis of temperature dependence of u_H suggests a crossover of dominant scattering mechanism from ionized impurity to acoustic phonon scattering with increasing temperature. The existence of local vibration modes of Ba atoms in cages composed of Ga and Sn atoms is evidenced by analysis of experimental data of structural refinement and specific heat, which give an Einstein temperature of 50 K and a Debye temperature of 200 K. This local vibration of Ba atoms should be responsible for the low thermal conductivity (1.1 W/m K at 150 K). The potential of type-VIII clathrate compounds for thermoelectric application is discussed., Comment: 6 pages, 6 figures, submitted to Phys. Rev. B

The paramagnetic Meissner effect (PME) in the field cooled susceptibility has been observed in superconducting single crystals of Ba_{1-x}K_xBiO_3 using magnetometers of Quantum-Design Co.. The PME is similar to that observed in cuprates and Nb superconductors. For the Ba_{0.63}K_{0.37}BiO_3 crystal, the PME is observed in cooling process under the field up to 750 Oe. The PME was not found in the virgin-charged superconducting magnet. The PME is found in a superconductor with trapped flux and may arise from a remnant field, a temperature inhomogeneity near T_c, and a potassium-concentration inhomogeneity., Comment: 4 pages, 4 figures

In order to explore the origin of the Metal-Insulator (M-I) transition, the precise crystal structures of the hole-doped Mott insulator system, Y1-XCaXTiO3 (x=0.37, 0.39 and 0.41), are studied for the temperature range between 20K and 300K by the synchrotron radiation (SR) X-ray powder diffraction. For both Y0.63Ca0.37TiO3 and Y0.61Ca0.39TiO3 compositions, the orthorhombic (Pbnm) - monoclinic (P21/n) structural phase transition occurs at around 230K, which is much higher than their own M-I transition temperatures, i.e. 60K and 130K, respectively. For these compositions, the significant phase separation (low-temperature orthorhombic + monoclinic) is also found in the vicinity of the M-I transition temperature. On the other hand, Y0.59Ca0.41TiO3, which dose not exhibit M-I transition and preserve a metallic behavior down to 1.5K, is in two phases state from 20K to 300K. It is concluded that the existence of the phase separation causes the M-I transition in Y1-xCaxTiO3, and the low-temperature orthorhombic phase contributes to the metallic property of this system.

We report on results from high-energy spectroscopic measurements on CeFe2, a system of particular interest due to its anomalous ferromagnetism with an unusually low Curie temperature and small magnetization compared to the other rare earth-iron Laves phase compounds. Our experimental results indicate very strong hybridization of the Ce 4f states with the delocalized band states, mainly the Fe 3d states. In the interpretation and analysis of our measured spectra, we have made use of two different theoretical approaches: The first one is based on the Anderson impurity model, with surface contributions explicitly taken into account. The second method consists of band-structure calculations for bulk CeFe2. The analysis based on the Anderson impurity model gives calculated spectra in good agreement with the whole range of measured spectra, and reveals that the Ce 4f -- Fe 3d hybridization is considerably reduced at the surface, resulting in even stronger hybridization in the bulk than previously thought. The band-structure calculations are ab initio full-potential linear muffin-tin orbital calculations within the local-spin-density approximation of the density functional. The Ce 4f electrons were treated as itinerant band electrons. Interestingly, the Ce 4f partial density of states obtained from the band-structure calculations also agree well with the experimental spectra concerning both the 4f peak position and the 4f bandwidth, if the surface effects are properly taken into account. In addition, results, notably the partial spin magnetic moments, from the band-structure calculations are discussed in some detail and compared to experimental findings and earlier calculations., Comment: 10 pages, 8 figures, to appear in Phys. Rev. B in December 2000

Optical reflectivity experiments have been conducted on single crystals of the Kondo insulator YbB_12 in order to obtain its optical conductivity, \sigma(\omega). Upon cooling below 70 K, a strong supression of \sigma(\omega) is seen in the far-infrared region, indicating the opening of an energy gap of ~ 25 meV. This gap development is coincident with a rapid decrease in the magnetic susceptibility, which shows that the gap opening has significant influence on magnetic properties. A narrow, asymmetric peak is observed at ~40 meV in \sigma(\omega), which is attributed to optical transitions between the Yb 4f-derived states across the gap. In addition, a broad peak is observed at ~0.25 eV. This peak is attributed to transitions between Yb 4f-derived states and p-d band, and is reminiscent of similar peaks previously observed for rare-earth hexaborides., Comment: 4 pages, 4 figures

We study the photoemission and optical conductivity response of the strongly correlated metallic system $Ca_xSr_{1-x}VO_3$. We find that the basic features of the transfer of spectral weight in photoemission experiments and the unusual lineshape of the optical response can be understood by modeling the system with a one band Hubbard model close to the Mott-Hubbard transition. We present a detailed comparison between the low frequency experimental data and the corresponding theoretical predictions obtained within the LISA method that is exact in the limit of large lattice connectivity., Comment: 4 pages + 2 figures, revtex