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R. Kajimoto

Publications and source records attributed to R. Kajimoto.

At least 19 recordsLinked to original sources

Zr-based bulk metallic glass clamp cell for high-pressure inelastic neutron scattering

We report the fabrication and characterization of a Zr-based bulk metallic glass (Zr-BMG) clamp cell designed for high-pressure inelastic neutron scattering (INS) measurements. The INS spectra of the empty cell exhibit broad and featureless backgrounds, reflecting the amorphous structure of the Zr-BMG. Test measurements using a reference sample, CsFeCl$_{3}$, confirm that the neutron transmission of the Zr-BMG cell is significantly higher than that of a conventional monobloc CuBe clamp cell. These results demonstrate that the Zr-BMG clamp cell provides both enhanced neutron transparency and a clean background profile, thereby advancing high-pressure INS studies.

cond-mat.mtrl-sci

Phonon spectrum in the spin-Peierls phase of CuGeO$_3$

CuGeO$_3$ has long been studied as a prototypical example of the spin-Peierls transition in a $S = 1/2$ Heisenberg chain. Despite intensive investigation of this quasi-one-dimensional material, systematic measurements and calculations of the phonon excitations in the dimerized phase have not to date been possible, leaving certain aspects of the spin-Peierls phenomenon unresolved. We perform state-of-the-art density functional theory (DFT) calculations to compute the electronic structure and phonon dynamics in the low-temperature dimerized phase. We also perform high-resolution neutron spectroscopy to measure the full phonon spectrum over multiple Brillouin zones. We find excellent agreement between our numerical and experimental results that extend to all measurement temperatures. Notable features of our phonon spectra include a number of steeply dispersive modes, nonmonotonic dispersion features, and specific phonon anticrossings, which we relate to the mode eigenvectors. By calculating the magnetic interactions within DFT and studying the effects of different phonon modes on the superexchange paths, we discuss the possibility of observing spin-phonon hybridization effects in experiments performed both in and out of equilibrium.

cond-mat.str-el

Spin excitations coupled with lattice and charge dynamics in La$_{2-x}$Sr$_{x}$CuO$_4$

Spin excitations of layered copper oxide show various characteristic features, depending on the carrier concentration. In this study, we conducted inelastic neutron scattering (INS) measurements on La$_{2-x}$Sr$_{x}$CuO$_4$ (LSCO), with $x$ = 0, 0.075, 0.18, and 0.30 and La$_{2-x}$Sr$_{x}$NiO$_4$ (LSNO) with 1/3, to clarify the origin of the intensity enhancement in the excitation spectrum of LSCO at the energy ($ω$) of 16--19 meV [Phys. Rev. B {\bf 91}, 224404 (2015), {\it ibid}. {\bf 93}, 094416 (2016)]. We confirmed the presence of a peak-structure in the $ω$-dependence of the local spin susceptibility $χ''(ω)$ of superconducting (SC) LSCO with a peak energy of 16--19 meV, where the spin excitations intersect optical phonon branches. A comparable peak-structure is not observed in the insulating La$_2$CuO$_4$, LSNO, and heavily overdoped LSCO with $x$ = 0.30. A dome-shaped $x$-dependence of the integrated intensity around the peak energies is revealed for SC phase by summarizing the present and previously reported results. Furthermore, our phonon calculation on LCO shows the existence of two optical branches at $\sim$19 meV that could stabilize stripe-alignment of carriers due to out-of-plane vibrations of Cu or O of the CuO$_2$ planes. These results indicate the interplay among spin, charge, and lattice dynamics and suggest that the intensity enhancement is associated with their composite excitations.

cond-mat.supr-con

Spin gap and L modulated intensity at the low-energy incommensurate magnetic fluctuations in the superconducting state of Sr2RuO4

Low-energy incommensurate (IC) magnetic fluctuations in the multiband superconductor Sr$_2$RuO$_4$ is investigated by high-resolution inelastic neutron scattering measurements and random phase approximation (RPA) calculations. Below $T_\text{c}$, the substantial spin gap is observed at $\mathbf{Q}_\text{IC}=(0.3, 0.3, L)$ where the quasi-one-dimensional $α$ and $β$ sheets consisting of the Fermi surfaces are in good nesting conditions. $L$ modulated intensity of the low-energy IC magnetic fluctuations and our RPA calculations indicate that the superconducting gaps regarding the $α$ and $β$ sheets have the horizontal line nodes.

cond-mat.supr-con

Quantum magnetisms in uniform triangular lattices Li2AMo3O8 (A = In, Sc)

Molecular based spin-1/2 triangular lattice systems such as LiZn$_2$Mo$_3$O$_8$ have attracted research interest. Distortions, defects, and intersite disorder are suppressed in such molecular-based magnets, and intrinsic geometrical frustration gives rise to unconventional and unexpected ground states. Li$_2$$A$Mo$_3$O$_8$ ($A$ = In or Sc) is such a compound where spin-1/2 Mo$_3$O$_{13}$ clusters in place of Mo ions form the uniform triangular lattice. Their ground states are different according to the $A$ site. Li$_2$InMo$_3$O$_8$ undergoes conventional $120^\circ$ long-range magnetic order below $T_\text{N}=12$~K whereas isomorphic Li$_2$ScMo$_3$O$_8$ exhibits no long-range magnetic order down to 0.5~K. Here, we report exotic magnetisms in Li$_2$InMo$_3$O$_8$ and Li$_2$ScMo$_3$O$_8$ investigated by muon spin rotation ($μ$SR) and inelastic neutron scattering (INS) spectroscopies using polycrystalline samples. Li$_2$InMo$_3$O$_8$ and Li$_2$ScMo$_3$O$_8$ show completely different behaviors observed in both $μ$SR and INS measurements, representing their different ground states. Li$_2$InMo$_3$O$_8$ exhibits spin wave excitation which is quantitatively described by the nearest neighbor anisotropic Heisenberg model based on the $120^\circ$ spin structure. In contrast, Li$_2$ScMo$_3$O$_8$ undergoes short-range magnetic order below 4~K with quantum-spin-liquid-like magnetic fluctuations down to the base temperature. Origin of the different ground states is discussed in terms of anisotropies of crystal structures and magnetic interactions.

cond-mat.str-el

Time-of-flight elastic and inelastic neutron scattering studies on the localized $4d$ electron layered perovskite La$_5$Mo$_4$O$_{16}$

The magnetic structure and spin-wave excitations in the quasi-square-lattice layered perovskite compound La$_5$Mo$_4$O$_{16}$ were studied by a combination of neutron diffraction and inelastic neutron scattering techniques using polycrystalline sample. Neutron powder diffraction refinement revealed that the magnetic structure is ferrimagnetic in the $ab$ plane with antiferromagnetic stacking along the $c$ axis where the magnetic propagation vector is $\mathbf{k}=\left(0,0,\frac{1}{2}\right)$. The ordered magnetic moments are estimated to be $0.54(2)μ_\text{B}$ for Mo$^{5+}$ ($4d^1$) ions and $1.07(3)μ_\text{B}$ for Mo$^{4+}$ ($4d^2$) ions at 4 K, which are about half of the expected values. The inelastic neutron scattering results display strong easy-axis magnetic anisotropy along the $c$ axis due to the spin-orbit interaction in Mo ions evidenced by the spin gap at the magnetic zone center. The model Hamiltonian consisting of in-plane anisotropic exchange interactions, the interlayer exchange interaction, and easy-axis single-ion anisotropy can explain our inelastic neutron scattering data well. Strong Ising-like anisotropy and weak interlayer coupling compared with the intralayer exchange interaction can explain both the high-temperature magnetoresistance and long-time magnetization decay recently observed in La$_5$Mo$_4$O$_{16}$.

cond-mat.str-el

Spin nematic susceptibility studied by inelastic neutron scattering in FeSe

Mechanism of unconventional superconductivity in FeSe has been intensely scrutinized recently because of a variety of exotic properties unprecedented for other iron-based superconductors. A central unanswered question concerns the origin of the interaction that causes the nematic transition at $T_s=90\,K$ without accompanying magnetic order. Elucidating the nature of spin excitations in the normal state is a key to addressing this issue. Here we report, from inelastic neutron-scattering measurements in FeSe single crystals, that high-energy spin excitation spectra of FeSe exhibit characteristic energy dependence with missing intensity at around 70-80$\,$meV, which are very different from other iron-based superconductors. Despite of the strongest electron correlations among the iron-based superconductor family, the spectra are qualitatively at variance with the local moment model and can be essentially described by the itinerant electron picture. Moreover, the dynamical spin susceptibility above $T_s$ is only weakly temperature dependent, which is in stark contrast to the Curie-Weiss behavior of the electronic nematic susceptibility, suggesting that the nematic transition is not likely driven by spin but by orbital degrees of freedom.

cond-mat.supr-con

Spin excitations in hole-overdoped iron-based superconductors

Understanding the overall features of magnetic excitation is essential for clarifying the mechanism of Cooper pair formation in iron-based superconductors. In particular, clarifying the relationship between magnetism and superconductivity is a central challenge because magnetism may play a key role in their exotic superconductivity. BaFe2As2 is one of ideal systems for such investigation because its superconductivity can be induced in several ways, allowing a comparative examination. Here we report a study on the spin fluctuations of the hole-overdoped iron-based superconductors Ba1-xKxFe2As2 (x = 0.5 and 1.0; Tc = 36 K and 3.4 K, respectively) over the entire Brillouin zone using inelastic neutron scattering. We find that their spin spectra consist of spin wave and chimney-like dispersions. The chimney-like dispersion can be attributed to the itinerant character of magnetism. The band width of the spin wave-like dispersion is almost constant from the non-doped to optimum-doped region, which is followed by a large reduction in the overdoped region. This suggests that the superconductivity is suppressed by the reduction of magnetic exchange couplings, indicating a strong relationship between magnetism and superconductivity in iron-based superconductors.

cond-mat.supr-con

Phonon and Magnetic Excitations in Superconducting Ca$_{10}$Pt$_4$As$_8$(Fe$_{1-x}$Pt$_x$As)$_{10}$

Inelastic neutron scattering studies have been carried out on selected phonons and magnetic excitations of a crystal of superconducting (SC) Ca$_{10}$Pt$_4$As$_8$(Fe$_{1-x}$Pt$_x$As)$_{10}$ with the onset transition temperature $T_{\rm c}^{\rm onset} \sim$ 33 K to investigate the role that orbital fluctuations play in the Cooper pairing. The spectral weight of the magnetic excitations, $χ''({\bm Q}, ω)$ at ${\bm Q} = {\bm Q}_{\rm M}$ (magnetic $Γ$ points) is suppressed (enhanced) in the relatively low (high) $ω$ region. The maximum of the enhancement is located at $ω= ω_{\rm p} \sim$ 18 meV at temperature $T = 3$ K corresponding to the $ω_{\rm p}/k_{\rm B}T_{\rm c}^{\rm onset} \sim$ 6.3. This large value is rather favorable to the orbital-fluctuation mechanism of the superconductivity with the so-called $S_{++}$ symmetry. In the phonon measurements, we observed slight softening of the in-plane transverse acoustic mode corresponding to the elastic constant $C_{66}$. This softening starts at $T$ well above the superconducting $T_{\rm c}$, as $T$ decreases. An anomalously large increase in the phonon spectral weight of in-plane optical modes was observed in the range of $35 < ω< 40$ meV with decreasing $T$ from far above $T_{\rm c}$. Because this $ω$ region mainly corresponds to the in-plane vibrations of Fe atoms, the finding presents information on the coupling between the orbital fluctuation of the Fe 3$d$ electrons and lattice system, useful for studying possible roles of the orbital fluctuation in the pairing mechanism and appearance of the so-called nematic phase.

cond-mat.supr-con

Development of spin correlations in the geometrically frustrated triangular-lattice Heisenberg antiferromagnet CuCrO2

Magnetic excitations in the triangular-lattice Heisenberg antiferromagnet (TLHA) CuCrO2 were studied using single-crystal inelastic neutron scattering. A diffusive quasielastic component that persisted without developing a correlation length over a wide temperature range both below and above the ordering temperature was observed. Furthermore, characteristic momentum dependence was observed that was reproduced using minimum spin clusters. The robust spin clusters contrast with conventional magnetic ordering and may be universal in TLHAs.

cond-mat.str-el

High-energy spin and charge excitations in electron-doped copper oxide superconductors

The evolution of electronic (spin and charge) excitations upon carrier doping is an extremely important issue in superconducting layered cuprates and the knowledge of its asymmetry between electron- and hole-dopings is still fragmentary. Here we combine x-ray and neutron inelastic scattering measurements to track the doping dependence of both spin and charge excitations in electron-doped materials. Copper L3 resonant inelastic x-ray scattering spectra show that magnetic excitations shift to higher energy upon doping. Their dispersion becomes steeper near the magnetic zone center and deeply mix with charge excitations, indicating that electrons acquire a highly itinerant character in the doped metallic state. Moreover, above the magnetic excitations, an additional dispersing feature is observed near the Γ-point, and we ascribe it to particle-hole charge excitations. These properties are in stark contrast with the more localized spin-excitations (paramagnons) recently observed in hole-doped compounds even at high doping-levels.

cond-mat.supr-con

Inelastic neutron scattering study of phonon anomalies in La1.5Sr0.5NiO4

The high-energy phonons in La1.5Sr0.5NiO4, in which the checkerboard charge ordering is formed, was investigated by the inelastic neutron scattering. We found that the longitudinal modes show strong anomalies compared with La2NiO4. We argue the similarity and difference in the phonon anomalies between the present sample and the preceding works of different compositions.

cond-mat.str-el

Influence of Mg, Ag and Al substitutions on the magnetic excitations in the triangular-lattice antiferromagnet CuCrO2

Magnetic excitations in CuCrO$_{2}$, CuCr$_{0.97}$Mg$_{0.03}$O$_{2}$, Cu$_{0.85}$Ag$_{0.15}$CrO$_{2}$, and CuCr$_{0.85}$Al$_{0.15}$O$_{2}$ have been studied by powder inelastic neutron scattering to elucidate the element substitution effects on the spin dynamics in the Heisenberg triangular-lattice antiferromagnet CuCrO$_{2}$. The magnetic excitations in CuCr$_{0.97}$Mg$_{0.03}$O$_{2}$ consist of a dispersive component and a flat component. Though this feature is apparently similar to CuCrO$_{2}$, the energy structure of the excitation spectrum shows some difference from that in CuCrO$_{2}$. On the other hand, in Cu$_{0.85}$Ag$_{0.15}$CrO$_{2}$ and CuCr$_{0.85}$Al$_{0.15}$O$_{2}$ the flat components are much reduced, the low-energy parts of the excitation spectra become intense, and additional low-energy diffusive spin fluctuations are induced. We argued the origins of these changes in the magnetic excitations are ascribed to effects of the doped holes or change of the dimensionality in the magnetic correlations.

cond-mat.str-el

Inelastic neutron scattering study of the magnetic fluctuations in Sr$_2$RuO$_4$

By performing time-of-flight neutron scattering measurements on a large amount of single crystals of Sr$_2$RuO$_4$, we studied detailed structure of the imaginary part of the dynamic spin susceptibility over a wide range of phase space. In the normal state at T=5 K, strong incommensurate (IC) peaks were clearly observed at around $\mathbf{Q}_\text{c}=(0.3,0.3)$ up to at least $\hbarω=80$ meV. In addition, our data also show strong magnetic fluctuations that exist on the ridges connecting the IC peaks around the $(π,π)$ point rather than around the $Γ$ point. Our results are consistent with the semi-mean-field random phase approximation calculation for a two dimensional Fermi liquid with a characteristic energy of 5.0 meV. Furthermore, the IC fluctuations were observed even at room temperature.

cond-mat.str-el

Strong spin resonance on BaFe2(As0.65P0.35)2 with Tc = 30 K

We performed inelastic neutron scattering on powder sample of the P-doped iron-based superconductor BaFe2(As0.65P0.35)2 with Tc = 30K, whose superconducting (SC) order parameter is expected to have line nodes. We have observed spin resonance at Q $\sim$ 1.2Å^{-1} and E=12 meV in the SC state. The resonance enhancement, which can be a measure of the area of sign reversal between the hole and electron Fermi surfaces (FSs), is comparable to those of other iron-based superconductors without line nodes. This fact indicates that the sign reversal between the FSs is still dominant in this system, and the line nodes should create only limited area of sign-reversal on a single FS. Hence the system can hold relatively high-Tc. Comparison with theoretical calculation indicates horizontal line nodes may be a candidate to reproduce the observation.

cond-mat.supr-con

Degradation of superconductivity and spin fluctuations by electron over-doping in LaFeAsO$_{1-x}$F$_{x}$

Low energy spin fluctuations are studied for the electron-doped Fe-based superconductor LaFeAsO(1-x)F(x) by inelastic neutron scattering up to the energy transfer of w = 15 meV using polycrystalline samples. Superconducting samples (x=0.057, Tc=25 K and x=0.082, Tc=29 K) show dynamical spin susceptibility chi"(w) almost comparable with the parent sample's. However chi"(w) is almost vanished in the x=0.158 sample where the superconductivity is highly suppressed. These results are compatible with the theoretical suggestions that the spin fluctuation plays an important role for the superconductivity.

cond-mat.supr-con

Neutron diffraction study of TbMnO3: Magnetic structure revisited

Magnetic ordering in TbMnO3 was revisited by a neutron diffraction study. In addition to the previously reported A-type and G-type modulated structures with a propagation vector (0,q_Mn,0), we found C-type and F-type orderings of the Mn moments. All the components appear below T_N^Mn = 46 K, and the G, C,and F-type components are enhanced below T_lock = 28 K, where q_Mn ordering locks at its low temperature value. The locking of the propagation vector also yields the squaring up of the spin arrangement. The magnetic moments of Tb ions show a quasi long-range ordering below T_N^Tb = 7 K. It drastically promotes the development of the G, C, and F-type components while suppressing the A-type components.

cond-mat.str-el

Ferromagnetic insulating phase in Pr{1-x}Ca{x}MnO3

A ferromagnetic insulating (FM-I) state in Pr0.75Ca0.25MnO3 has been studied by neutron scattering experiment and theoretical calculation. The insulating behavior is robust against an external magnetic field, and is ascribed to neither the phase separation between a ferromagnetic metallic (FM-M) phase and a non-ferromagnetic insulating one, nor the charge ordering. We found that the Jahn-Teller type lattice distortion is much weaker than PrMnO3 and the magnetic interaction is almost isotropic. These features resembles the ferromagnetic metallic state of manganites, but the spin exchange interaction J is much reduced compared to the FM-M state. The theoretical calculation based on the staggered type orbital order well reproduces several features of the spin and orbital state in the FM-I phase.

cond-mat.str-el