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The superconducting order parameter of the noncentrosymmetric superconductor LaRhSn is investigated by means of low temperature measurements of the specific heat, muon-spin relaxation/rotation ($\mu$SR) and the tunnel-diode oscillator (TDO) based method. The specific heat and magnetic penetration depth [$\lambda(T)$] show an exponentially activated temperature dependence, demonstrating fully gapped superconductivity in LaRhSn. The temperature dependence of $\lambda^{-2}(T)$ deduced from the TDO based method and $\mu$SR show nearly identical behavior, which can be well described by a single-gap $s$-wave model, with a zero temperature gap value of $\Delta(0)=1.77(4)k_BT_c$. The zero-field $\mu$SR spectra do not show detectable changes upon cooling below $T_c$, and therefore there is no evidence for time-reversal-symmetry breaking in the superconducting state., Comment: 9 pages, 8 figures

We have synthesized YbPdAs with the hexagonal ZrNiAl-type structure, in which the Yb-atoms form a distorted kagome sublattice in the hexagonal basal plane. Magnetic, transport, and thermodynamic measurements indicate that YbPdAs is a low-carrier Kondo lattice compound with an antiferromagnetic transition at $T_\mathrm{N}$ = 6.6 K, which is slightly suppressed in applied magnetic fields up to 9 T. The magnetic entropy at $T_\mathrm{N}$ recovers only 33\% of $R\ln{2}$, the full entropy of the ground state doublet of the Yb-ions. The resistivity displays a $-\ln T$ dependence between 30 and 15 K, followed by a broad maximum at $T\rm_{coh}$ = 12 K upon cooling. Below $T\rm_{coh}$, the magnetoresistance changes from negative to positive, suggesting a crossover from single-ion Kondo scattering processes at intermediate temperatures to coherent Kondo lattice behaviors at low temperatures. Both the Hall resistivity measurements and band structure calculations indicate a relatively low carrier concentration in YbPdAs. Our results suggest that YbPdAs could provide an opportunity for examining the interplay of Kondo physics and magnetic frustration in low carrier systems., Comment: 9 pages, 9 figures

We present the results of muon spin relaxation ($\mu$SR) and neutron scattering on the Ce-based quasikagome lattice CeRh$_{1-x}$Pd$_{x}$Sn ($x=0.1$ to 0.75). Our ZF-$\mu$SR results reveal the absence of static long-range magnetic order down to 0.05~K in $x = 0.1$ single crystals. The weak temperature-dependent plateaus of the dynamic spin fluctuations below 0.2~K in ZF-$\mu$SR together with its longitudinal-field (LF) dependence between 0 and 3~kG indicate the presence of dynamic spin fluctuations persisting even at $T$ = 0.05~K without static magnetic order. On the other hand, $C_{\text{4f}}$/$T$ increases as --log $T$ on cooling below 0.9~K, passes through a broad maximum at 0.13~K and slightly decreases on further cooling. The ac-susceptibility also exhibits a frequency independent broad peak at 0.16~K, which is prominent with an applied field $H$ along $c$-direction. We, therefore, argue that such a behavior for $x=0.1$ (namely, a plateau in spin relaxation rate ($\lambda$) below 0.2~K and a linear $T$ dependence in $C_{\text{4f}}$ below 0.13~K) can be attributed to a metallic spin-liquid (SL) ground state near the quantum critical point in the frustrated Kondo lattice. The LF-$\mu$SR study suggests that the out of kagome plane spin fluctuations are responsible for the SL behavior. Low energy inelastic neutron scattering (INS) of $x$ = 0.1 reveals gapless magnetic excitations, which are also supported by the behavior of $C_{\text{4f}}$ proportional to $T^{1.1}$ down to 0.06~K., Comment: 19 pages and 9 figures

Polycrystalline La$_{7}$Ir$_{3}$ is reported to show superconductivity breaking time-reversal symmetry while also having an isotropic $s$-wave gap. Single crystals of this noncentrosymmetric superconductor are highly desirable to understand the nature of the electron pairing mechanism in this system. Here we report the growth of high-quality single crystals of La$_{7}$Ir$_{3}$ by the Czochralski method. The structural and superconducting properties of these large crystals have been investigated using x-rays, magnetization, resistivity and heat capacity measurements. We observe a clear anisotropy in the lower and upper critical fields for magnetic fields applied parallel and perpendicular to the hexagonal $c$ axis. We also report the presence of a robust electronic critical field, that diverges from the upper critical field derived from heat capacity, which is the hallmark of surface superconductivity., Comment: 20 + 5 pages, 6 + 4 figures, 1 + 1 tables. Accepted for publication into Physical Review Materials

We report the observation of multiple magnetic transitions in single crystals of EuPtAs using magnetization, transport, and thermodynamic measurements. EuPtAs crystallizes in the noncentrosymmetric tetragonal LaPtSi-type structure (space group I41md) and undergoes a second-order antiferromagnetic transition at 14.8 K, which is followed by a first-order transition at about 7.5 K. Both transitions are suppressed by magnetic fields applied parallel and perpendicular to the c axis, and multiple field-induced transitions are observed for both field directions, leading to complex temperature-field diagrams with a dome-like magnetic phase for fields parallel to the c axis. Moreover, the dependence of the low temperature resistivity on the application of a training field, but the lack of remanent magnetization, suggests the presence of multiple antiferromagnetic domains in zero-field., Comment: 8 pages, 8 figures

We report a systematic study of the $5d$-electron-doped system Ce(Fe$_{1-x}$Ir$_x$)$_2$Al$_{10}$ ($0 \leq x \leq 0.15$). With increasing $x$, the orthorhombic $b$~axis decreases slightly while accompanying changes in $a$ and $c$ leave the unit cell volume almost unchanged. Inelastic neutron scattering, along with thermal and transport measurements, reveal that for the Kondo semiconductor CeFe$_2$Al$_{10}$, the low-temperature energy gap which is proposed to be a consequence of strong $c \mhyphen f$ hybridization, is suppressed by a small amount of Ir substitution for Fe, and that the system adopts a metallic ground state with an increase in the density of states at the Fermi level. The charge or transport gap collapses (at $x=$~0.04) faster than the spin gap with Ir substitution. Magnetic susceptibility, heat capacity, and muon spin relaxation measurements demonstrate that the system undergoes long-range antiferromagnetic order below a N\'eel temperature, $T_{\mathrm{N}}$, of 3.1(2)~K for $x = 0.15$. The ordered moment is estimated to be smaller than 0.07(1)~$\mu_\mathrm{B}$/Ce although the trivalent state of Ce is confirmed by Ce L$_3$-edge x-ray absorption near edge spectroscopy. It is suggested that the $c \mhyphen f$ hybridization gap, which plays an important role in the unusually high ordering temperatures observed in Ce$T_2$Al$_{10}$ ($T$ = Ru and Os), may not be necessary for the onset of magnetic order with a low $T_{\mathrm{N}}$ seen here in Ce(Fe$_{1-x}$Ir$_x$)$_2$Al$_{10}$., Comment: 12 pages, 11 figures

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.

CeIrSn with a quasikagome Ce lattice in the hexagonal basal plane is a strongly valence fluctuating compound, as we confirm by hard x-ray photoelectron spectroscopy and inelastic neutron scattering, with a high Kondo temperature of $T_{\mathrm{K}}\sim 480$\,K. We report a negative in-plane thermal expansion $\alpha/T$ below 2\,K, which passes through a broad minimum near 0.75\,K. Volume and $a$-axis magnetostriction for $B \parallel a$ are markedly negative at low fields and change sign before a sharp metamagnetic anomaly at 6\,T. These behaviors are unexpected for Ce-based intermediate valence systems, which should feature positive expansivity. Rather they point towards antiferromagnetic correlations at very low temperatures. This is supported by muon spin relaxation measurements down to 0.1\,K, which provide microscopic evidence for a broad distribution of internal magnetic fields. Comparison with isostructural CeRhSn suggests that these antiferromagnetic correlations emerging at $T\ll T_{\mathrm{K}}$ result from geometrical frustration., Comment: to be published in Phys. Rev. Lett

The dynamic magnetic properties of the Kondo-insulator state in CeFe2Al10 (spin gap, resonance mode) have been investigated using polarized neutrons on a single crystal of pure CeFe2Al10. The results indicate that the magnetic excitations are polarized mainly along the orthorhombic a axis and their dispersion along the orthorhombic c direction could be determined. Polycrystalline samples of Nd- and Rh-doped CeFe2Al0 were also studied by the time-of-flight technique, with the aim of finding out how the low-energy magnetic excitation spectra change upon isoelectronic substitution of the rare-earth (Nd) on the magnetic Ce site or electron doping (Rh) on the transition-element Fe sublattice. The introduction of magnetic Nd impurities strongly modifies the spin gap in the Ce dynamic magnetic response and causes the appearance of a quasielastic signal. The crystal-field excitations of Nd, studied in both LaFe2Al10 and CeFe2Al10, also reveal a significant influence of f-electron hybridization (largest in the case of Ce) on the crystal-field potential. As a function of the Rh concentration, a gradual change is observed from a Kondo-insulator to a metallic Kondo-lattice response, likely reflecting the decrease in the hybridization energy., Comment: 27 pages, 15 figures

A number of rare-earth monopnictides have topologically non-trivial band structures together with magnetism and strong electronic correlations. In order to examine whether the antiferromagnetic (AFM) semimetal YbAs ($T\rm_N$ = 0.5 K) exhibits such a scenario, we have grown high-quality single crystals using a flux method, and characterized the magnetic properties and electronic structure using specific heat, magnetotransport and angle-resolved photoemission spectroscopy (ARPES) measurements, together with density functional theory (DFT) calculations. Both ARPES and DFT calculations find no evidence for band inversions in YbAs, indicating a topologically trivial electronic structure. From low-temperature magnetotransport measurements, we map the field-temperature phase diagram, where we find the presence of a field stabilized phase distinct from the AFM phase at low temperatures. An extremely large magnetoresistance (XMR) for both YbAs and the nonmagnetic counterpart LuAs, is also observed, which can consistently be accounted for by the presence of electron-hole compensation. Moreover, an angle-dependent study of the Shubnikov-de Haas effect oscillations reveals very similar Fermi surfaces between YbAs and LuAs, with light effective masses down to at least 0.5 K, indicating that the Yb-$4f$ electrons are well localized, and do not contribute to the Fermi surface. However, the influence of the localized Yb-$4f$ electrons on the magnetotransport of YbAs can be discerned from the distinct temperature dependence of the XMR compared to that of LuAs, which we attribute to the influence of short-ranged spin correlations that appear well above $T\rm_N$., Comment: 12 pages, 10 figures

Electrical resistivity $\rho(T)$ and specific heat $C(T)$ measurements have been made on the diluted 4$f^2$ system Y(Pr)Ir$_2$Zn$_{20}$. Both data of $\rho$ and magnetic specific heat $C_{\rm m}$ per Pr ion are well scaled as a function of $T/T_{\rm 0}$, where $T_{\rm 0}$ is a characteristic temperature of non-Fermi liquid (NFL) behaviors. Furthermore, the temperature dependences of $\rho$ and $C_{\mathrm{m}}/T$ agree with the NFL behaviors predicted by the two-channel Kondo model for the strong coupling limit. Therefore, we infer that the observed NFL behaviors result from the single-site quadrupole Kondo effect due to the hybridization of the 4$f^2$ states with multi-channel conduction electrons., Comment: 13 pages, 5figures

We report thermal expansion and magnetostriction of the cubic non-Kramers system PrIr$_2$Zn$_{20}$ with a non-magnetic $\varGamma_{3}$ ground state doublet. In previous experiments, antiferroquadrupolar order at \hbox{$T_{\mathrm{Q}}=0.11$\,K} and a Fermi liquid state around $B_{\mathrm{c}}\approx5$\,T for \hbox{$\boldsymbol{B}\parallel[001]$}, indicative of possible ferrohastatic order, were discovered. For magnetic fields \hbox{$\boldsymbol{B}\parallel[001]$}, the low temperature longitudinal and transverse thermal expansion and magnetostriction are highly anisotropic. The resulting volume strain is very small, indicating that the Pr valence remains nearly constant as a function of magnetic field. We conclude that the Fermi liquid state around $B_{\mathrm{c}}$ forms through a very little change in c-f hybridization. This result is in sharp contrast to Ce- and Yb-based Kramers Kondo lattices which show significantly larger volume strains due to the high sensitivity of the Kondo temperature to hydrostatic pressure., Comment: 8 pages, 8 figures

Hexagonal CeRhSn with paramagnetic $4f$ moments on a distorted Kagome lattice displays zero-field quantum critical behavior related to geometrical frustration. We report high-resolution thermal expansion and magnetostriction measurements under multiextreme conditions such as uniaxial stress up to 200 MPa, temperatures down to 0.1 K and magnetic fields up to 10 T. Under uniaxial stress along the $a$-direction, quantum criticality disappears and a complex magnetic phase diagram arises with a sequence of phases below 1.2 K and fields between 0 and 3 T ($\parallel a$). Since the Kondo coupling increases with stress, which alone would stabilize paramagnetic behavior in CeRhSn, the observed order arises from the release of geometrical frustration by in-plane stress., Comment: Accepted in PRB Rapid Comm

The strange electronic state of a class of materials which violates the predictions of conventional Fermi-liquid theory of metals remains enigmatic. Proximity to a quantum critical point is a possible origin of this non-Fermi liquid (NFL) behavior, which is usually accomplished by tuning the ground state with non-thermal control parameters such as chemical composition, magnetic field or pressure. We present the spin dynamics study of a stoichiometric NFL system CeRhBi, using low-energy inelastic neutron scattering (INS) and muon spin relaxation (muSR) measurements. It shows evidence for an energy-temperature (E/T) scaling in the INS dynamic response and a time-field scaling of the muSR asymmetry function indicating a quantum critical behavior in this compound. The E/T scaling reveals a local character of quantum criticality consistent with the power-law divergence of the magnetic susceptibility, logarithmic divergence of the magnetic heat capacity and T-linear resistivity at low temperature. The NFL behavior and local criticality occur over a very wide dynamical range at zero field and ambient pressure without any tuning in this stoichiometric heavy fermion compound is striking, making CeRhBi an exemplary model system amenable to in-depth studies for quantum criticality., Comment: 8 pages, 3 figures

The recent discovery of topological Kondo insulating behaviour in strongly correlated electron systems has generated considerable interest in Kondo insulators both experimentally and theoretically. The Kondo semiconductors CeT2Al10 (T=Fe, Ru and Os) possessing a c-f hybridization gap have received considerable attention recently because of the unexpected high magnetic ordering temperature of CeRu2Al10 (TN=27 K) and CeOs2Al10 (TN=28.5 K) and the Kondo insulating behaviour observed in the valence fluctuating compound CeFe2Al10 with a paramagnetic ground state down to 50 mK. We are investigating this family of compounds, both in polycrystalline and single crystal form, using inelastic neutron scattering to understand the role of anisotropic c-f hybridization on the spin gap formation as well as on their magnetic properties. We have observed a clear sign of a spin gap in all three compounds from our polycrystalline study as well as the existence of a spin gap above the magnetic ordering temperature in T=Ru and Os. Our inelastic neutron scattering studies on single crystals of CeRu2Al10 and CeOs2Al10 revealed dispersive gapped spin wave excitations below TN. Analysis of the spin wave spectrum reveals the presence of strong anisotropic exchange, along the c-axis (or z-axis) stronger than in the ab-plane. These anisotropic exchange interactions force the magnetic moment to align along the c-axis, competing with the single ion crystal field anisotropy, which prefers moments along the a-axis. In the paramagnetic state (below 50 K) of the Kondo insulator CeFe2Al10, we have also observed dispersive gapped magnetic excitations which transform into quasi-elastic scattering on heating to 100 K. We will discuss the origin of the anisotropic hybridization gap in CeFe2Al10 based on theoretical models of heavy-fermion semiconductors., Comment: 17 pages, 7 figures, SCTE2016

Orbital degrees of freedom in condensed matters could play important roles in forming a variety of exotic electronic states by interacting with conduction electrons. In 4f electron systems, because of strong intra-atomic spin-orbit coupling, an orbitally degenerate state inherently carries quadrupolar degrees of freedom. The present work has focussed on a purely quadrupole-active system PrIr2Zn20 showing superconductivity in the presence of an antiferroquadrupole order at TQ = 0.11 K. We observed non-Fermi liquid (NFL) behaviors emerging in the electrical resistivity and the 4f contribution to the specific heat, C_4f, in the paramagnetic state at T > TQ. Moreover, in magnetic fields below 6 T, all data set of the electrical resistivity and C_4f(T) are well scaled with characteristic temperatures T0's. This is the first observation of the NFL state in the nonmagnetic quadrupole-active system, whose origin is intrinsically different from that observed in the vicinity of the conventional quantum critical point. It implies possible formation of a quadrupole Kondo lattice resulting from hybridization between the quadrupoles and the conduction electrons. Below 0.13 K, the electrical resistivity and C_4f(T) exhibit anomalies as B approaches 5 T. This is the manifestation of a field-induced crossover toward a Fermi-liquid ground state in the quadrupole Kondo lattice., Comment: 8 pages, 6 figures

We present bulk-sensitive hard x-ray photoelectron spectroscopy (HAXPES) data of the Ce3d core levels and lifetime-reduced L edge x-ray absorption spectroscopy (XAS) in the partial fluorescence yield (PFY) mode of the CeMIn5 family with M = Co, Rh, and Ir. The HAXPES data are analyzed quantitatively with a combination of full multiplet and configuration interaction model which allows correcting for the strong plasmons in the CeMIn5 HAXPES data, and reliable weights wn of the different fn contributions in the ground state are determined. The CeMIn5 results are compared to HAXPES data of other heavy fermion compounds and a systematic decrease of the hybridization strength Veff from CePd3 to CeRh3B2 to CeRu2Si2 is observed, while it is smallest for the three CeMIn5 compounds. The f-occupation, however, increases in the same sequence and is close to one for the CeMIn5 family. The PFY-XAS data confirm an identical f-occupation in the three CeMIn5 compounds and a phenomenological fit to these PFY-XAS data combined with a configuration interaction model yields consistent results., Comment: 9 pages, 5 figures

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.

Geometrical frustration describes situations where interactions are incompatible with the lattice geometry and stabilizes exotic phases such as spin liquids. Whether geometrical frustration of magnetic interactions in metals can induce unconventional quantum critical points is an active area of research. We focus on the hexagonal heavy fermion metal CeRhSn where the Kondo ions are located on distorted kagome planes stacked along the c axis. Low-temperature specific heat, thermal expansion and magnetic Gr\"uneisen parameter measurements prove a zero-field quantum critical point. The linear thermal expansion, which measures the initial uniaxial pressure derivative of the entropy, displays a striking anisotropy. Critical and noncritical behaviors along and perpendicular to the kagome planes, respectively, prove that quantum criticality is driven by geometrical frustration. We also discovered a spin-flop-type metamagnetic crossover. This excludes an itinerant scenario and suggests that quantum criticality is related to local moments in a spin-liquid like state., Comment: 14 pages, 5 figures

The opening of a spin gap in the orthorhombic compounds CeT$_2$Al$_{10}$ (T = Ru and Os) is followed by antiferromagnetic ordering at $T_N$ = 27 K and 28.5 K, respectively, with a small ordered moment (0.29$-$0.34$\mu_B$) along the $c-$axis, which is not an easy axis of the crystal field (CEF). In order to investigate how the moment direction and the spin gap energy change with 10\% La doping in Ce$_{1-x}$La$_x$T$_2$Al$_{10}$ (T = Ru and Os) and also to understand the microscopic nature of the magnetic ground state, we here report on magnetic, transport, and thermal properties, neutron diffraction (ND) and inelastic neutron scattering (INS) investigations on these compounds. Our INS study reveals the persistence of spin gaps of 7 meV and 10 meV in the 10\% La-doped T = Ru and Os compounds, respectively. More interestingly our ND study shows a very small ordered moment of 0.18 $\mu_B$ along the $b-$axis (moment direction changed compared with the undoped compound), in Ce$_{0.9}$La$_{0.1}$Ru$_2$Al$_{10}$, however a moment of 0.23 $\mu_B$ still along the $c-$axis in Ce$_{0.9}$La$_{0.1}$Os$_2$Al$_{10}$. This contrasting behavior can be explained by a different degree of hybridization in CeRu$_2$Al$_{10}$ and CeOs$_2$Al$_{10}$, being stronger in the latter than in the former. Muon spin rotation ($\mu$SR) studies on Ce$_{1-x}$La$_x$Ru$_2$Al$_{10}$ ($x$ = 0, 0.3, 0.5 and 0.7), reveal the presence of coherent frequency oscillations indicating a long$-$range magnetically ordered ground state for $x$ = 0 to 0.5, but an almost temperature independent Kubo$-$Toyabe response between 45 mK and 4 K for $x$ = 0.7. We will compare the results of the present investigations with those reported on the electron and hole$-$doping in CeT$_2$Al$_{10}$., Comment: 11 pages, 7 figures

The caged compound LaRu2Zn20 exhibits a structural transition at TS =150 K, whose driving mechanism remains elusive. We have investigated atomic dynamics by the measurements of specific heat C and inelastic X-ray scattering (IXS). The lattice part of the specific heat Clat divided by T3, Clat/T3, shows a broad peak at around 15 K, which is reproduced by two Einstein modes with characteristic temperatures of 35 K and 82 K, respectively. IXS measurements along the [111] and [110] directions reveal optical phonon modes at 3 meV (35 K) and 7 meV (80 K), respectively, whose values agree with the values of Einstein temperatures. The first principles calculation has assigned the phonon modes at 3 meV as the optical modes of Zn atoms located at the middle of two La atoms. The low-energy vibration of the Zn atom perpendicular to the there-fold axis is thought to lead the structural instability of LaRu2Zn20., Comment: 11pages, 4 figures

We have found that Ce3Pd20As6 crystallizes into a cubic C6Cr23-type structure. Combination of electron probe microanalysis of the chemical composition and Rietveld analysis of the powder X-ray diffraction pattern has revealed an inhomogeneous atomic composition of variable stoichiometry. The physical properties of Ce3Pd20As6 were investigated by measuring the magnetization, electrical resistivity and specific heat. The 4f electrons of Ce3+ ions are well localized but do not show phase transition down to 0.5 K. The metallic electrical resistivity shows a weak Kondo screening. The residual resistivity ratio is rather low probably due to the variable stoichiometry. The magnetization curve and magnetic entropy suggest the Gamma_8 quartet crystalline-electric-field ground state at least one of two Ce sites., Comment: 19 pages, 6 figures, to be published in J. Alloys Comp

The occupancy of the 4f^n contributions in the Kondo semiconductors CeM2Al10(M = Ru, Os and Fe) has been quantitatively determined by means of bulk-sensitive hard x-ray photoelectron spectroscopy (HAXPES) on the Ce 3d core levels. Combining a configuration interaction scheme with full multiplet calculations allowed to accurately describe the HAXPES data despite the presence of strong plasmon excitations in the spectra. The configuration interaction parameters obtained from this analysis -- in particular the hybridization strength V_eff and the effective f binding energy Delta_f -- indicate a slightly stronger exchange interaction in CeOs2Al10 compared to CeRu2Al10, and a significant increase in CeFe2Al10. This verifies the coexistence of a substantial amount of Kondo screening with magnetic order and places the entire CeM2Al10 family in the region of strong exchange interactions., Comment: 9 pages, 4 figures, submitted to Physical Review B

We present a detailed investigation of the hole (3\% Re) doping effect on the polycrystalline CeRu$_{2}$Al$_{10}$ sample by magnetization, heat capacity, resistivity, muon spin rotation ($\mu$SR), and neutron scattering (both elastic and inelastic) measurements. CeRu$_2$Al$_{10}$ is an exceptional cerium compound with an unusually high Neel temperature of 27 K. Here we study the stability of the unusual magnetic order by means of controlled doping, and we uncover further surprising attributes of this phase transition. The heat capacity, resistivity and $\mu$SR measurements reveal an onset of magnetic ordering below 23 K, while a broad peak at 31 K (i.e. above $T_N$), has been observed in the temperature dependent susceptibility, indicating an opening of a spin gap above $T_N$. Our important finding, from the neutron diffraction, is that the compound orders antiferromagnetically with a propagation vector $\bf k$ = (1 0 0) and the ordered state moment is 0.20(1)$\mu_B$ along the $b-$axis. This is in sharp contrast to the undoped compound, which shows AFM ordering at 27 K with the ordered moment of 0.39(3)$\mu_B$ along the $c-$axis. Similar to CeRu$_2$Al$_{10}$ our inelastic neutron scattering study on the Re doped shows a sharp spin gap-type excitation near 8 meV at 5 K, but with slightly reduced intensity compared to the undoped compound. Further the excitation broadens and shifts to lower energy ($\le$ 4 meV) near 35 K. These results suggest that the low temperature magnetic properties of the hole doped sample is governed by the competition between the anisotropic hybridization effect and crystal field anisotropy as observed in hole-doped CeOs$_2$Al$_{10}$., Comment: 10 pages, 10 figures, Submitted to Phys. Rev. B

The effects of electron (Ir) and hole (Re) doping on the hybridization gap and antiferromagnetic order have been studied by magnetization, muon spin relaxation ($\mu^+$SR), and inelastic neutron scattering on the polycrystalline samples of Ce(Os$_{1-x}$Ir$_x$)$_2$Al$_{10}$ ($x$ = 0.08 and 0.15) and CeOs$_{1.94}$Re$_{0.06}$Al$_{10}$. $\mu^+$SR spectra clearly reveals magnetic ordering below 20 and 10 K for $x$ = 0.08 and 0.15 samples respectively with a very weak signature of oscillations of the muon initial asymmetry at very short time scale. Our important findings are that small amount of electron doping (i) completely suppress the inelastic magnetic excitations near 11 meV down to 2K, which were observed in the undoped compound, and the response transforms into a broad quasielastic response and (ii) the internal field at the corresponding muon site is remarkably enhanced by about ten times compared with the parent compound. On the other hand with small amount of hole (3\% Re) doping the intensity of the inelastic magnetic excitations near 11 meV is reduced significantly. The main origin of the observed doping effect is an extra 5$d$ electrons being carried by Ir and a hole carried by Re compared with that the Os atom. The obtained results demonstrate a great sensitivity of the carrier doping and provides additional ways to study their anomalous magnetic properties., Comment: 9 pages, 13 figures

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

The Kondo semiconductor CeOs$_{2}$Al$_{10}$ exhibits an antiferromagnetic (AFM) order at $T_\mathrm{N}= 28.5$ K, whose temperature is unexpectedly high for the small ordered moment of $0.3$ $\mu_\mathrm{B}/$Ce. We have studied the effects of electron- and hole-doping on the hybridization gap and AFM order by measuring the magnetization $M$, magnetic susceptibility $\chi$, electrical resistivity $\rho$, and specific heat $C$ on single crystals of Ce(Os$_{1-x}$Ir$_{x}$)$_{2}$Al$_{10}$($x \le 0.15$) and Ce(Os$_{1-y}$Re$_{y}$)$_{2}$Al$_{10}$($y \le 0.1$). The results of $M (B)$ indicates that the AFM ordered moment $\mu_\mathrm{AF}$ changes the direction from the $c$-axis for $x = 0$ to the $a$-axis for $x = 0.03$. With increasing $x$ up to 0.15, $T_\mathrm{N}$ gradually decreases although the $4f$ electron state becomes localized and the magnitude of $\mu_\mathrm{AF}$ is increased to $1$ $\mu_\mathrm{B}/$Ce. With increasing $y$, the $4f$ electron state is more delocalized and the AFM order disappears at a small doping level $y = 0.05$. In both electron- and hole-doped systems, the suppression of $T_\mathrm{N}$ is well correlated with the increase of the Sommerfeld coefficient $\gamma$ in $C(T)$. Furthermore, the simultaneous suppression of $T_\mathrm{N}$ and the semiconducting gap in $\rho (T)$ at $T > T_\mathrm{N}$ indicates that the presence of the hybridization gap is indispensable for the unusual AFM order in CeOs$_{2}$Al$_{10}$., Comment: 16 pages, 7 figures, submitted to Phys. Rev. B

Recently the Ce-based caged-type compounds having general formula CeT2Al10 (T=Fe, Ru and Os) have generated considerable interest due to the Kondo semiconducting paramagnetic ground state (down to 40 mK) observed in CeFe2Al10 and anomalously high magnetic ordering temperature with a spin gap formation at low temperatures in Kondo semimetals CeRu2Al10 and CeOs2Al10. The formation of long-range magnetic ordering out of the Kondo semiconducting/semimetallic state itself is extraordinary and these are the first examples of this enigmatic coexistence of electronic ground states. These compounds also exhibit strong anisotropy in the magnetic and transport properties, which has been explained on the basis of single ion crystal electric field (CEF) anisotropy in the presence of strongly anisotropic hybridization between localised 4f-electron and conduction electrons. Further they also exhibit a remarkable modification of magnetic and transport properties with doping on Ce, or T or Al sites. In this review we briefly discuss the bulk properties of these compounds, giving a detailed discussion on our muon-spin-relaxation (muSR) investigations and inelastic neutron scattering (INS) results., Comment: 36 pages, 21 figures, 2 tables. Physica Scripta (2013)

The lightly hole-doped system CeOs1.94Re0.06Al10 has been studied by muon spin relaxation and neutron diffraction measurements. A long-range antiferromagnetic ordering of the Ce-sublattice with substantially reduced value of the magnetic moment 0.18(1) \mu_B has been found below T_N = 21 K. Similar to the undoped parent compound, the magnetic ground state of CeOs1.94Re0.06Al10 preserves the anomalous direction of the ordered moments along the c-axis. The obtained result reveals the crucial difference between electron- and hole-doping effects on the magnetic ordering in CeOs2Al10. The former suppresses the anisotropic c-f hybridization and promotes localized Ce moments. On the contrary, the latter increases the hybridization and shifts the system towards delocalized non-magnetic state.

We have investigated optical conductivity spectra of $n$- and $p$-type Ba$_8$Ga $_{16}$Sn$_{30}$ ($\alpha$-BGS) with type-VIII clathrate structure, at temperatures from 296\,K down to 6\,K with a terahertz time-domain spectrometer (0.2\,-\,2.5\,THz). The continuous spectra contributed from charge carriers are dispersive in this frequency range and also temperature- and carrier type-dependent. The Drude-Smith model taking multiple-scatterings of charge carriers into account well reproduces those data. The relaxation rate of the $n$-type carriers decreases more sharply than that in the $p$-type material, suggesting that a stronger electron-phonon interaction may exist in the $n$-type than in the $p$-type. On the other hand, the localized infrared-active modes observed at 1.3\,THz and 1.7\,THz, identified as the rattling phonons of the Ba$^{2+}$ ion's quasi-on-center vibrations, become soft and broad significantly with decreasing temperature as well as observed in type-I BGS and BGG (Ba$_8$Ga$_{16}$Ge$_{30}$) clathrates. The softening in the $n$-type is smaller by about 30% than in the $p$-type, whereas the linewidth brodening is almost the same independently on the carrier type. The difference in the softening is discussed with a scenario where the interaction of rattling phonons with carriers can modify the anharmonic potential of the guest ions. The anomalous broadening at low temepratures is also discussed by the impurity-scattering model presented for a rattling-phonon system strongly hybridized with acoustic cage phonons.

The effect of Ir substitution for Os in CeOs2Al10, with an unusually high Neel temperature of T~28.5K, has been studied by high-resolution neutron diffraction and magnetization measurements. A small amount of Ir (~ 8%) results in a pronounced change of the magnetic structure of the Ce-sublattice. The new magnetic ground state is controlled by the single ion anisotropy and implies antiferromagnetic arrangement of the Ce-moments along the a-axis, as expected from the anisotropy of the paramagnetic susceptibility. The value of the ordered moments, 0.92(1) mu_B, is substantially bigger than in the undoped compound, whereas the transition temperature is reduced down to 21K. A comparison of the observed phenomena with the recently studied CeRu1.9Rh0.1Al10 system, exhibiting similar behaviour [A. Kondo et al., J. Phys. Soc. Jpn. 82, 054709 (2013)], strongly suggests the electron doping as the main origin of the ground state changes. This provides a new way of exploring the anomalous magnetic properties of the Ce(Ru/Os)2Al10 compounds.

We have carried out muon spin relaxation (muSR), neutron diffraction and inelastic neutron scattering (INS) investigations on polycrystalline samples of Ce(Ru1-xFex)2Al10 (x=0, 0.3, 0.5, 0.8 and 1) to investigate the nature of the ground state (magnetic ordered versus paramagnetic) and the origin of the spin gap formation as evident from the bulk measurements in the end members. Our zero-field muSR spectra clearly reveal coherent two-frequency oscillations at low temperature in x=0, 0.3 and 0.5 samples, which confirms the long-range magnetic ordering of the Ce-moment with TN=27, 26 and 21 K respectively. On the other hand the muSR spectra of x=0.8 and x=1 down to 1.4 K and 0.045 K, respectively exhibit a temperature independent Kubo-Toyabe term confirming a paramagnetic ground state. The long-range magnetic ordering in x=0.5 below 21 K has been confirmed through the neutron diffraction study. INS measurements of x=0 clearly reveal the presence of a sharp inelastic excitation near 8 meV between 5 K and 26 K, due to an opening of a gap in the spin excitation spectrum, which transforms into a broad response at and above 30 K. Interestingly, at 4.5 K the spin gap excitation broadens in x=0.3 and exhibits two clear peaks at 8.4(3) and 12.0(5) meV in x=0.5. In the x=0.8 sample, which remains paramagnetic down to 1.2 K, there is a clear signature of a spin gap of 10-12 meV at 7 K, with a strong Q-dependent intensity. Evidence of a spin gap of 12.5(5) meV has also been found in x=1. The observation of a spin gap in the paramagnetic samples (x=0.8 and 1) is an interesting finding in this study and it challenges our understanding of the origin of the semiconducting gap in CeT2Al10 (T=Ru and Os) compounds in terms of hybridization gap opening only a small part of the Fermi surface, gapped spin waves, or a spin-dimer gap., Comment: 40 pages, 18 figures, Phys. Rev. B accepted for publication (2013)

Superconducting and antiferroquadrupolar (AFQ) transitions in a Pr-based compound PrRh2Zn20 have been found to occur simultaneously at Tc=TQ=0.06 K. The superconducting transition manifests itself by zero resistance and large diamagnetic susceptibility. The specific heat exhibits a Schottky anomaly peaking at 14 K and magnetization curves measured at 2 K show anisotropic behaviors. The analysis of these data indicates that the crystalline electric field (CEF) ground state of the trivalent Pr ion is the non-Kramers Gamma3 doublet with the quadrupolar degrees of freedom. A sharp peak in the specific heat at 0.06 K has been attributed not to the superconducting transition but to the AFQ transition because the ordering temperature TQ decreases in B || [100] but increases in B || [110] and B || [111] with increasing B up to 6 T. This anisotropic behavior of TQ(B) can be well explained by a two-sublattice mean-field calculation, which corroborates the AFQ ordered state below TQ. The entropy release at TQ is only 10% of Rln2 expected for the Gamma3 doublet, suggesting possible interplay between the quadrupolar degrees of freedom and the superconductivity., Comment: 18 page, 6 figures, accepted for publication in Phys. Rev. B

We have succeeded in establishing the crystal-field ground state of CeRu2Al10, an orthorhombic intermetallic compound recently identified as a Kondo insulator. Using polarization dependent soft x-ray absorption spectroscopy at the Ce M4,5 edges, together with input from inelastic neutron and magnetic susceptibility experiments, we were able to determine unambiguously the orbital occupation of the 4f shell and to explain quantitatively both the measured magnetic moment along the easy a axis and the small ordered moment along the c-axis. The results provide not only a platform for a realistic modeling of the spin and charge gap of CeRu2Al10, but demonstrate also the potential of soft x-ray absorption spectroscopy to obtain information not easily accessible by neutron techniques for the study of Kondo insulators in general., Comment: submitted to Physical Review B Rapid Communications

The optical conductivity spectra of the rattling phonons in the clathrate Ba$_8$Ga$_{16}$Ge$_{30}$ are investigated in detail by use of the terahertz time-domain spectroscopy. The experiment has revealed that the lowest-lying vibrational mode of a Ba(2)$^{2+}$ ion consists of a sharp Lorentzian peak at 1.2 THz superimposed on a broad tail weighted in the lower frequency regime around 1.0 THz. With decreasing temperature, an unexpected linewidth broadening of the phonon peak is observed, together with monotonic softening of the phonon peak and the enhancement of the tail structure. These observed anomalies are discussed in terms of impurity scattering effects on the hybridized phonon system of rattling and acoustic phonons., Comment: Submitted to JPSJ

We have carried out neutron diffraction, muon spin relaxation (muSR) and inelastic neutron scattering investigations on a polycrystalline sample of CeOs2Al10 to investigate the nature of the phase transition observed near 29 K in the resistivity and heat capacity. Our muSR data clearly reveal coherent frequency oscillations below 28 K, indicating the presence of an internal field at the muon site, which confirms the long-range magnetic ordering of the Ce-moment below 28 K. Upon cooling the sample below 15 K, unusual behaviour of the temperature dependent muSR frequencies may indicate either a change of the muon site, consistent with the observation of superstructure reflections in electron diffraction or a change of the ordered magnetic structure. Neutron diffraction data do not reveal any clear sign of either magnetic Bragg peaks or superlattice reflections. Furthermore, inelastic neutron scattering (INS) measurements clearly reveal the presence of a sharp inelastic excitation near 11 meV between 5 K and 26 K, due to opening of a gap in the spin excitation spectrum, which transforms into a broad response at and above 30 K. The magnitude of the spin-gap (11 meV) as derived from the INS peak position agrees very well with the gap value as estimated from the bulk properties., Comment: 37 pages

With a terahertz time-domain spectrometer (0.3 - 3.0 THz) we have measured the optical conductivity of the type-I clathrate Ba$_8$Ga$_{16}$Sn$_{30}$ at temperatures from 300 K down to 7 K. Independent six spectra superimposed on the Drude conductivity are identified to infrared active vibrational modes of guest Ba ions and the cages. While the spectra of five higher-frequency modes depend hardly on temperature, the lowest-lying spectrum with a peak at 0.72 THz due to the Ba(2) ion's off-centering vibration in the oversized cage changes with temperature characteristically. With lowering temperature, the spectral shape of this so-called rattling phonon continues to become so broad that the line-width amounts to be comparable to the peak frequency. Furthermore, below about 100 K, the single broad peak tends to split into two subpeaks. While this splitting can be explained by assuming a multi-well anharmonic potential, the strong enhancement of the line-width broadening toward low temperature, cannot be understood, since the Boltzmann factor generally sharpens the low-temperature spectra., Comment: 5 pages, 4 figures

The low temperature state of CeRu2Al10 has been studied by neutron powder diffraction and muon spin relaxation (muSR). By combining both techniques, we prove that the transition occurring below T*~27K, which has been the subject of considerable debate, is unambiguously magnetic due to the ordering of the Ce sublattice. The magnetic structure with propagation vector k=(1,0,0) involves collinear antiferromagnetic alignment of the Ce moments along the c-axis of the Cmcm space group with a reduced moment of 0.34(2)mu_B. No structural changes within the resolution limit have been detected below the transition temperature. However, the temperature dependence of the magnetic Bragg peaks and the muon precession frequency show an anomaly around T2~12 K indicating a possible second transition.

We report the anisotropic changes in the electronic structure of a Kondo semiconductor CeOs$_2$Al$_{10}$ across an anomalous antiferromagnetic ordering temperature ($T_0$) of 29 K, using optical conductivity spectra. The spectra along the $a$- and $c$-axes indicate that a $c$-$f$ hybridization gap emerges from a higher temperature continuously across $T_0$. Along the b-axis, on the other hand, a different energy gap with a peak at 20 meV appears below 39 K, which is higher temperature than $T_0$, because of structural distortion. The onset of the energy gap becomes visible below $T_0$. Our observation reveals that the electronic structure as well as the energy gap opening along the b-axis due to the structural distortion induces antiferromagnetic ordering below $T_0$., Comment: 4 pages, 4 figures

A caged compound CeOs2Al10, crystallizing in the orthorhombic YbFe2Al10-type structure, undergoes a mysterious phase transition at T_0=29 K. We report the results of electron diffraction, magnetization, and magnetoresistance for single crystals. Superlattice reflections characterized by a wave vector q = (0, -2/3, 2/3) observed at 15 K indicate a structural modification in the ordered state. Activation-type behavior of the electrical resistivity along the three principal axes below 50 K suggests gap opening in the conduction band. The magnetic susceptibility \chi = M/B is highly anisotropic, \chi_a>\chi_c>\chi_b, all of which sharply decrease on cooling below T_0. Furthermore, a metamagnetic anomaly in the magnetization and a step in the magnetoresistance occur at B=6-8 T only when the magnetic field is applied parallel to the orthorhombic c axis. However, T_0 hardly changes under magnetic fields up to 14 T, irrespective of the field direction. By using these data, we present a B-T phase diagram and discuss several scenarios for the mysterious transition., Comment: 6 pages, 7 figures, accepted for publication in Phys. Rev. B

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

A series of infrared-active optical phonons have been detected in type-I clathrate Ba$_8$Ga$_{16}$Ge$_{30}$ by terahertz time-domain spectroscopy. The conductivity spectra with the lowest-lying peaks at 1.15 and 1.80 THz are identified with so-called rattling phonons, i.e., optical modes of the guest ion Ba$^{2+}(2)$ with $T_{1u}$ symmetry in the oversized tetrakaidecahedral cage. The temperature dependence of the spectra from these modes are totally consistent with calculations based on a one-dimensional anharmonic potential model that, with decreasing temperature, the shape becomes asymmetrically sharp associated with a softening for the weight to shift to lower frequency. These temperature dependences are determined, without any interaction effects, by the Bose-factor for optical excitations of anharmonic phonons with the nonequally spaced energy levels., Comment: 4 pages, 4 figures