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T. Takabatake

Publications and source records attributed to T. Takabatake.

At least 55 records · Page 3Linked to original sources

Crystal-field ground state of the orthorhombic Kondo insulator CeRu2Al10

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.

cond-mat.str-el↗

Electronic-Structure-Driven Magnetic Ordering in a Kondo Semiconductor CeOs2Al10

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 $T_0$.

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Direct evidence of long-range ordering of reduced magnetic moments in the spin-gap compound CeOs2Al10 through muon spin relaxation investigations

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.

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Low temperature line-width broadening in optical-conductivity spectra of the off-center rattling phonons in type-I clathrate Ba$_8$Ga$_{16}$Sn$_{30}$

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.

cond-mat.mtrl-sci↗

Long-range magnetic order in CeRu2Al10 evidenced by muSR and neutron diffraction

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.

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Structural Modification and Metamagnetic Anomaly in the Ordered State of CeOs2Al10

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 χ= M/B is highly anisotropic, χ_a>χ_c>χ_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.

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Different Evolution of Intrinsic Gap in Kondo Semiconductors SmB6 and YbB12

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.

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Optical conductivity of rattling phonons in type-I clathrate Ba$_8$Ga$_{16}$Ge$_{30}$

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.

cond-mat.mtrl-sci↗

Field dependence of the thermopower of CeNiSn

Previously measured thermopower data of CeNiSn exhibit a significant sample dependence and non-monotonous behavior in magnetic fields. In this paper we demonstrate that the measured thermopower S(T) may contain a contribution from the huge Nernst coefficient of the compound, even in moderate fields of 2 T. A correction for this effect allows to determine the intrinsic field dependence of S(T). The observed thermopower behavior can be understood from Zeeman splitting of a V-shaped pseudogap in magnetic fields.

cond-mat.str-el↗

A Kondo lattice antiferromagnet CePd5Al2

We report on the electrical resistivity, magnetic susceptibility and heat-capacity measurements on a new intermetallic compound CePd5Al2, crystallizing in the ZrNi2Al5-type tetragonal structure, with lattice parameters a = 4.156 A and c = 14.883 A. The compound presents Kondo lattice behavior and an easy-plane antiferromagnetic ground state with two magnetic transitions at 2.9 K and 3.9 K. The Sommerfeld coefficient is estimated as 60 mJ/mol K^2.

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Terahertz conductivity of localized photoinduced carriers in Mott insulator YTiO$_{3}$ at low excitation density, contrasted with metallic nature in band semiconductor Si

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 $μ$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.

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Easy-plane magnetocrystalline anisotropy in the multi-step metamagnet CeIr3Si2

Highly anisotropic properties of CeIr$_3$Si$_2$ have been observed by the magnetization $M$($B$), electrical resistivity $ρ$, and specific heat measurements on a single-crystalline sample. This compound with an orthorhombic structure having zigzag chains of Ce ions along the a-axis undergos magnetic transitions at 3.9 K and 3.1 K. At 0.3 K, metamagnetic transitions occur at 0.68 T and 1.3 T for $B$$//$$b$ and 0.75 T for $B$$//$$c$. Easy-plane magnetocrystalline anisotropy is manifested as $M$($B//b$) $\cong$ $M$($B//c$) $\cong$ 11$M$($B//a$) at $B$ = 5 T. Electrical resistivity is also anisotropic; $ρ_{b}$ $\cong$ $ρ_{c}$ $\ge$ 2$ρ_{a}$. The magnetic part of $ρ$ exhibits a double-peak structure with maxima at 15 K and 250 K. The magnetic entropy at $T$$\rm_{N1}$ = 3.9 K is a half of $R$ln2. These observations are ascribable to the combination of the Kondo effect with $T$$\rm_{K}$ $\sim$ 20 K and a strong crystal field effect. The analysis of $M$($B$) and paramagnetic susceptibility revealed unusually large energy splitting of 500 K and 1600 K for the two excited doublets, respectively.

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Universal scaling in the dynamical conductivity of heavy fermion Ce and Yb compounds

Dynamical conductivity spectra s(w) have been measured for a diverse range of heavy-fermion (HF) Ce and Yb compounds. A characteristic excitation peak has been observed in the mid-infrared region of s(w) for all the compounds, and has been analyzed in terms of a simple model based on conduction (c)-f electron hybridized band. A universal scaling is found between the observed peak energies and the estimated c-f hybridization strengths of these HF compounds. This scaling demonstrates that the model of c-f hybridized band can generally and quantitatively describe the charge excitation spectra of a wide range of HF compounds.

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Energy gap formation in a valence fluctuating compound CeIrSb probed by Sb NMR and NQR

Sb-NMR/NQR study has revealed a formation of a pseudogap at the Fermi level in the density of states in a valence fluctuating compound CeIrSb. The nuclear spin-lattice relaxation rate divided by temperature, 1/T_1T has a maximum around 300 K and decreases significantly as 1/T_1T ~ T^2, followed by a 1/T_1T = const. relation at low temperature. This temperature dependence of 1/T_1T is well reproduced by assuming a V-shaped energy gap with a residual density of states at the Fermi level. The size of energy gap for CeIrSb is estimated to be about 350 K, which is by one order of magnitude larger than those for the isostructural Kondo semiconductors CeRhSb and CeNiSn. Despite the large difference in the size of energy gap, CeIrSb, CeRhSb and CeNiSn are indicated to be classified into the same group revealing a V-shaped gap due to c-f hybridization. The temperature dependence of the Knight shift measured in a high magnetic field agrees with the formation of this pseudogap.

cond-mat.str-el↗

Cage-size control of guest vibration and thermal conductivity in Sr8Ga16Si30-xGex

We present a systematic study of thermal conductivity, specific heat, electrical resistivity, thermopower and x-ray diffraction measurements performed on single-crystalline samples of the pseudoquaternary type-I clathrate system Sr8Ga16Si30-xGex, in the full range of 0 < x < 30. All the samples show metallic behavior with n-type majority carriers. However, the thermal conductivity and specific heat strongly depend on x. Upon increasing x from 0 to 30, the lattice parameter increases by 3%, from 10.446 to 10.726 A, and the localized vibrational energies of the Sr guest ions in the tetrakaidekahedron (dodecahedron) cages decrease from 59 (120) K to 35 (90) K. Furthermore, the lattice thermal conductivity at low temperatures is largely suppressed. In fact, a crystalline peak found at 15 K for x = 0 gradually decreases and disappears for x > 20, evolving into the anomalous glass-like behavior observed for x = 30. It is found that the increase of the free space for the Sr guest motion directly correlates with a continuous transition from on-center harmonic vibration to off-center anharmonic vibration, with consequent increase in the coupling strength between the guest's low-energy modes and the cage's acoustic phonon modes.

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Glasslike vs. crystalline thermal conductivity in carrier-tuned Ba8Ga16X30 clathrates (X = Ge, Sn)

The present controversy over the origin of glasslike thermal conductivity observed in certain crystalline materials is addressed by studies on single-crystal x-ray diffraction, thermal conductivity k(T) and specific heat Cp(T) of carrier-tuned Ba8Ga16X30 (X = Ge, Sn) clathrates. These crystals show radically different low-temperature k(T) behaviors depending on whether their charge carriers are electrons or holes, displaying the usual crystalline peak in the former case and an anomalous glasslike plateau in the latter. In contrast, Cp(T) above 4 K and the general structural properties are essentially insensitive to carrier tuning. We analyze these combined results within the framework of a Tunneling/Resonant/Rayleigh scatterings model, and conclude that the evolution from crystalline to glasslike k(T) is accompanied by an increase both in the effective density of tunnelling states and in the resonant scattering level, while neither one of these contributions can solely account for the observed changes in the full temperature range. This suggests that the most relevant factor which determines crystalline or glasslike behavior is the coupling strength between the guest vibrational modes and the frameworks with different charge carriers.

cond-mat.str-el↗

Thermopower of CexR1-xB6 (R=La, Pr and Nd)

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.

cond-mat.str-el↗

Tunable charge carriers and thermoelectricity of single-crystal Ba8Ga16Sn30

We have grown single crystals of the type-VIII intermetallic clathrate Ba8Ga16Sn30 from both Sn and Ga flux, evaluated their compositions through electron microprobe analysis and studied their transport properties through measurements on temperature dependent resistivity, thermopower and Hall coefficient. Crystals grown in Sn flux show n-type carriers and those from Ga flux show p-type carriers, whereas all measured compositions remain very close to the stoichiometric 8:16:30 proportion of Ba:Ga:Sn, expected from charge-balance principles. Our results indicate a very high sensitivity of the charge carrier nature and density with respect to the growth conditions, leading to relevant differences in transport properties which point to the importance of tuning this material for optimal thermoelectric performance.

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