arXiv subjects

Y. Muro

Publications and source records attributed to Y. Muro.

17 recordsLinked to original sources

arXiv2023

Quantum Griffiths singularity in the stoichiometric heavy-fermion system CeRh$_4$Al$_{15}$

We present a detailed investigation of the stoichiometric CeRh$_4$Al$_{15}$ single crystal compound using the temperature dependence of the heat capacity [$C_{\text{P}}$($T$)], electrical resistivity [$\rho$($T$)], magnetic susceptibility [$\chi$($T$)], and magnetization [$M$($H$)] measurements for a magnetic field ($H$) applied in the basal plane and along the $c$-axis. The low temperature power-law behavior of $C$/$T$ $\propto$ $\chi$ $\propto$ $T^{-1+\alpha}$, the isotherm magnetization, $M \sim H^{\alpha}$ with the exponent $\alpha$ = 0.45 - 0.55, and the $T$-linear resistivity $\Delta \rho$ $\sim$ $T^\epsilon$ with $\epsilon \sim$ 1 are found to be consistent with the formation of quantum Griffiths singularities in the non-Fermi-liquid (NFL) regime. We further investigated the spin dynamics of a polycrystalline sample of CeRh$_4$Al$_{15}$, using zero-field (ZF) and longitudinal-field (LF) muon spin relaxation ($\mu$SR) measurements. ZF-$\mu$SR measurements do not reveal any sign of long-range magnetic ordering down to 70~mK. The electronic relaxation rate ($\lambda$) below 0.5~K increases rapidly and shows a thermal activation-like characteristic [$T$log($\lambda$)$\sim$ $T$] over the entire measured temperature range between 70~mK to 4~K, indicating the presence of low energy spin fluctuations in CeRh$_4$Al$_{15}$. LF-$\mu$SR measurements show a time-field ($t/H^{\eta}$) scaling of the $\mu$SR asymmetry indicating a quantum critical behavior of this compound. Furthermore, inelastic neutron scattering study on the polycrystalline sample reveals two crystal field excitations near 19 and 33~meV. These features collectively provide strong evidence of NFL behavior in CeRh$_4$Al$_{15}$ due to the formation of Griffiths phase close to a $T$ $\rightarrow$ 0~K quantum critical point.

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arXiv2021

A crossover from Kondo semiconductor to metallic antiferromagnet with $5d$-electron doping in CeFe$_2$Al$_{10}$

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 Néel 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)~$μ_\mathrm{B}$/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$_{10}$.

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arXiv2020

Effect of Nd and Rh substitution on the spin dynamics of Kondo insulator CeFe2Al10

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.

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arXiv2016

Inelastic neutron scattering investigations of an anisotropic hybridization gap in the Kondo insulators: CeT2Al10 (T=Fe, Ru and Os)

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.

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arXiv2016

Quantitative study of the f occupation in CeMIn5 and other cerium compounds with hard x-rays

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.

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arXiv2015

Contrasting chemical pressure effect on the moment direction in the Kondo semiconductor CeT$_2$Al$_{10}$ (T = Ru,Os)

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$-$0.34$μ_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 $μ_B$ 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 $μ_B$ 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 ($μ$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$_{10}$.

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arXiv2015

Quantitative study of valence and configuration interaction parameters of the Kondo semiconductors CeM2Al10 (M = Ru, Os and Fe) by means of bulk-sensitive hard x-ray photoelectron spectroscopy

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.

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arXiv2014

Suppression of antiferromagnetic order and hybridization gap by electron- and hole-doping in the Kondo semiconductor CeOs$_{2}$Al$_{10}$

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 $0.3$ $μ_\mathrm{B}/$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 $χ$, electrical resistivity $ρ$, 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 $μ_\mathrm{AF}$ 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 $μ_\mathrm{AF}$ is increased to $1$ $μ_\mathrm{B}/$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 $γ$ in $C(T)$. Furthermore, the simultaneous suppression of $T_\mathrm{N}$ and the semiconducting gap in $ρ(T)$ at $T > T_\mathrm{N}$ indicates that the presence of the hybridization gap is indispensable for the unusual AFM order in CeOs$_{2}$Al$_{10}$.

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arXiv2013

Competing 4f-electron dynamics in Ce(Ru1-xFex)2Al10 (x=0 to 1): magnetic ordering emerging from the Kondo semiconducting state

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.

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arXiv2013

Another dimension: investigations of molecular magnetism using muon-spin relaxation

We review examples of muon-spin relaxation measurements on molecule-based magnetic coordination polymers, classified by their magnetic dimensionality. These include the one-dimensional s=1/2 spin chain Cu(pyz)(NO3)2 and the two-dimensional s=1/2 layered material [Cu(HF2)(pyz)2]BF4. We also describe some of the more exotic ground states that may become accessible in the future given the ability to tune the interaction strengths of our materials through crystal engineering.

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arXiv2012

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.

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arXiv2012

Neutron scattering experiments and simulations near the magnetic percolation threshold of Fe_x Zn_{1-x} F_2

The low temperature excitations in the anisotropic antiferromagnetic Fe_{1-x} Zn_x F_2 for x=0.25 and 0.31, at and just above the magnetic percolation threshold concentration x_p=0.25, were measured using inelastic neutron scattering. The excitations were simulated for x=0.31 using a localized, classical excitation model, which accounts well for the energies and relative intensities of the excitations observed in the scattering experiments.

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arXiv2010

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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arXiv2010

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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arXiv2010

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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arXiv2010

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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arXiv2007

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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