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Hiroya Sakurai

Publications and source records attributed to Hiroya Sakurai.

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Superconducting Lanthanum Nickel Oxides with Bilayered and Trilayered Crystal Structures

In 2023, superconductivity in La$_3$Ni$_2$O$_7$ was discovered under high pressures above approximately 14 GPa. In addition to its high transition temperature ($T_{\mathrm{c}} \simeq 80$ K), the structural resemblance to high-$T_{\mathrm{c}}$ cuprates has strongly stimulated research, soon followed by the discovery of superconductivity in La$_4$Ni$_3$O$_{10}$. These compounds belong to the Ruddlesden--Popper phases, comprising double- and triple-layered NiO$_2$ square lattices separated by LaO rock-salt slabs. Research on these systems has rapidly developed along three major directions, as in other prominent families of superconductors such as the cuprates and iron arsenides: expanding the chemical variety of compounds, enhancing $T_{\mathrm{c}}$ through elemental substitution, and elucidating the superconducting mechanism. These challenges, being closely interconnected, continue to drive the field. The clarification of the pairing mechanism encounters a particular difficulty, since the key experiments must be performed under high pressures. This situation highlights the significance of developing nickel oxides that exhibit superconductivity at much lower pressures, ideally at ambient pressure, which would in turn broaden the scope of chemical tuning and detailed physical characterization. In this context, it is timely and meaningful to summarize the present state of knowledge. Here, we emphasize sample synthesis and characterization, which are already well established and often decisive for progress in unconventional superconductors, while providing a brief overview of the currently available electronic properties.

cond-mat.supr-con

Characterization of Nuclear and Magnetic Structures of Wolframite-Type MgReO4 and ZnReO4

We utilized high-pressure methods to synthesize the oxides AReO$4$ (A=Zn, Mg) and characterized their crystal structures as monoclinic wolframite-type. By combining muon spin spectroscopy ($\mu^+$SR) with DFT calculations for muon stopping sites, we identify two possible magnetic spin structures for both compounds: $\Gamma_3$ with the propagation vector $\mathbf{k} = (0,1/2,0)$ and $\Gamma_4$ with $\mathbf{k} = (0,0,0)$. In both cases, the magnetic moments are canted from the principal axes within the $ac$-plane. The ordered moment of the proposed structures is $\mathbf{0.29(5)~\mu\mathrm{B}}$ for $\Gamma_3$ and $\mathbf{0.25(8)~\mu_\mathrm{B}}$ for $\Gamma_4$. The low moment is consistent with the absence of a magnetic contribution to the neutron powder diffraction (NPD) spectra. Bond valence sum (BVS) analysis supports the oxidation state of Re being Re$^{6+}$ in the compounds, and we suggest that a combination of $t_\mathrm{2g}$ orbital splitting due to spin-orbit coupling (SOC) and $d$-$p$ orbital hybridization is responsible for the strongly suppressed ordered magnetic moment.

cond-mat.mtrl-sci

Microscopic evidence for spin-spinless stripe order with reduced Ni moments within $ab$ plane for bilayer nickelate La$_3$Ni$_2$O$_7$ probed by $^{139}$La-NQR

The intrinsic electronic properties of La$_3$Ni$_2$O$_{7}$ have been selectively investigated by nuclear quadrupole resonance (NQR) at the La(2) site outside the NiO$_2$ bilayers. The La(2)$_{\rm a}$ site of the ideal La$_3$Ni$_2$O$_{7}$ is clearly distinguished from the La(2)$_{\rm b}$ site close to the local defects. Below 150K, almost half of the intrinsic La(2)$_{\rm a}$ sites are dominated by a finite internal field within the $ab$ plane, while the other half are dominated by zero internal field. The result is fully consistent with the single spin-spinless stripe order of ($\cdots\uparrow\circ\downarrow\circ\uparrow\circ\cdots$), where the reduced Ni magnetic moments are parallel to the $ab$-plane. Even for the La(2)$_{\rm b}$ site, the result is also explained within the same model by considering the inhomogeneous internal magnetic fields enhanced around the nearby defects such as oxygen vacancies. These findings provide unambiguous microscopic evidence for the single spin-spinless stripe order below 150 K at ambient pressure.

cond-mat.str-el

High-pressure synthesis of bilayer nickelate Sr$_{3}$Ni$_{2}$O$_{5}$Cl$_{2}$ with tetragonal crystal structure

A novel oxychloride, Sr$_{3}$Ni$_{2}$O$_{5}$Cl$_{2}$, was synthesized for the first time under high pressure of 10 GPa at 1400 ${}^\circ$C, motivated by a theoretical prediction of its potential superconductivity under ambient pressure. Small single crystals were used to determine the crystal structure and measure the temperature dependence of electrical resistance. The crystal is isostructural with the recently discovered superconductor, La$_{3}$Ni$_{2}$O$_{7}$, in line with the theoretical expectation.

cond-mat.supr-con

Phase diagram of pressure-induced high temperature superconductor La$_{3}$Ni$_{2}$O$_{7+\delta}$

We successfully synthesized samples of La$_{3}$Ni$_{2}$O$_{7+\delta}$ ($\delta = -0.50$, $-0.16$, $0.00$, $+0.01$, and $+0.12$) and measured the resistance under extremely high pressures using a diamond anvil cell to establish the electronic phase diagram. A Mott insulating state appears at $\delta = -0.50$, where all Ni ions are divalent. With increasing oxygen content, superconductivity appears at $\delta = 0.00$ and higher, above approximately 25 GPa, passing through Anderson localization at $\delta = -0.16$. The superconducting transition temperature $T_{\mathrm{c}}$ decreases with increasing pressures for both $\delta = 0.00$ and $+0.12$, with the pressure dependence of $T_{\mathrm{c}}$ being much stronger in the latter than in the former.

cond-mat.supr-con

Pressure-induced superconductivity in La$_{4}$Ni$_{3}$O$_{10+\delta}$ ($\delta$ = 0.04 and -0.01)

The superconducting transition temperatures, $T_{\mathrm{c}}$, of La$_{4}$Ni$_{3}$O$_{10+\delta}$($\delta$ = 0.04 and -0.01) were determined under various pressures up to 124.9 GPa by electrical resistance measurements with a diamond anvil cell. $T_{\mathrm{c}}$ exhibits a strong dependence on oxygen content within the pressure range of approximately 20 GPa and 80 GPa. At 48.0 GPa, $T_{\mathrm{c}}$ of La$_{4}$Ni$_{3}$O$_{10.04}$ peaks at 36 K, marking the highest $T_{\mathrm{c}}$ reported thus far.

cond-mat.supr-con

Theoretical analysis on the possibility of superconductivity in a trilayer Ruddlesden-Popper nickelate La$_4$Ni$_3$O$_{10}$ under pressure and its experimental examination: comparison with La$_3$Ni$_2$O$_7$

We study the possibility of superconductivity in a trilayer Ruddlesden-Popper nickelate La$_4$Ni$_3$O$_{10}$ under pressure both theoretically and experimentally, making comparison with the recently discovered high $T_c$ superconductor La$_3$Ni$_2$O$_7$, a bilayer nickelate. Through DFT calculations, we find that a structural phase transition from monoclinic to tetragonal takes place around 10 - 15 GPa. Using the tetragonal crystal structure, we theoretically investigate the possibility of superconductivity, where a combination of fluctuation exchange approximation and linearized Eliashberg equation is applied to a six-orbital model constructed from first principles band calculation. The obtained results suggests that La$_4$Ni$_3$O$_{10}$ may also become superconducting under high pressure with $T_c$ comparable to some cuprates, although it is not as high as La$_3$Ni$_2$O$_7$. We also perform experimental studies using our polycrystalline samples of La$_3$Ni$_2$O$_{7.01}$ and La$_4$Ni$_3$O$_{9.99}$. The superconducting transition of La$_3$Ni$_2$O$_{7.01}$, with a maximum onset $T_c$ of 67.0 K at a pressure of 26.5 GPa, is confirmed by a drop in the electrical resistance, as well as the magnetic field dependence of the resistance. Quite interestingly, similar temperature and magnetic field dependencies of the resistance are observed also for La$_4$Ni$_3$O$_{9.99}$, where a drop in the resistance is observed at lower temperatures compared to La$_3$Ni$_2$O$_{7.01}$, under pressures of 32.8 GPa and above. Given the theoretical expectation, the reduction in the resistance can most likely be attributed to the occurrence of superconductivity in La$_4$Ni$_3$O$_{9.99}$. The temperature at which the resistance deviates from a linear behavior, considered as the onset $T_c$, monotonically increases up to 23 K at 79.2 GPa, which is opposite to the pressure dependence of $T_c$ in La3Ni2O7.01.

cond-mat.supr-con

Revised Magnetic Structure and Tricritical Behavior of the CMR Compound NaCr$_2$O$_4$ Investigated with High Resolution Neutron Diffraction and $μ^+$SR

The mixed valence Cr compound NaCr$_2$O$_4$, synthesized using a high-pressure technique, offers a unique playground for investigating unconventional physical properties in condensed matter. In the present study, muon spin rotation/relaxation ($μ^+$SR) and high-resolution neutron powder diffraction (NPD) measurements were carried out to clarify the true magnetic ground state of this interesting compound. Our detailed study brings new insight, allowing us to confirm the existence of a commensurate antiferromagnetic order (C-AFM) and to extract its ordered Cr moment $μ^{\rm C}_{\rm Cr}=(4.30\pm0.01)μ_B$. Such a value of the ordered moment is in fact compatible with the existence of high-spin Cr sites. Further, the value of the canting angle of the Cr spin axial vector is refined as $θ_{\rm c}=(8.8\pm0.5)^{\circ}$. Employing high-quality samples in combination with time-of-flight NPD, a novel magnetic supercell was also revealed. Such supercell display an incommensurate (IC)-AFM propagation vector (0~0~${\textstyle \frac{1}{2}-}δ$), having an ordered moment $μ^{\rm IC}_{\rm Cr}=(2.20\pm0.03)μ_B$. It is suggested that the C-AFM and IC-AFM modulations are due to itinerant and localized contributions to the magnetic moment, respectively. Finally, the direct measurement of the magnetic order parameter provided a value of the critical exponent $β= 0.245 \approx \frac{1}{4}$, suggesting a non conventional critical behavior for the magnetic phase transition in NaCr$_2$O$_4$.

cond-mat.str-el

Na-ion Dynamics in the Solid Solution Na$_{\rm x}$Ca$_{1- \rm x}$Cr$_2$O$_4$ Studied by Muon Spin Rotation and Neutron Diffraction

In this work we present systematic set of measurements carried out by muon spin rotation/relaxation ($μ^+$SR) and neutron powder diffraction (NPD) on the solid solution Na$_{\rm x}$Ca$_{1- \rm x}$Cr$_2$O$_4$. This study investigates Na-ion dynamics in the quasi-1D (Q1D) diffusion channels created by the honeycomb-like arrangement of CrO$_6$ octahedra, in the presence of defects introduced by Ca doping. With increasing Ca content, the size of the diffusion channels is enlarged, however, this effect does not enhance the Na ion mobility. Instead the overall diffusivity is hampered by the local defects and the Na hopping probability is lowered. The diffusion mechanism in Na$_{\rm x}$Ca$_{1- \rm x}$Cr$_2$O$_4$ was found to be interstitial and the activation energy as well as diffusion coefficient were determined for all the members of the solid solution.

cond-mat.mtrl-sci

Magnetic nature of wolframite MgReO$_4$

Rhenium oxides belonging to the family $A$ReO$_4$ where $A$ is a metal cation, exhibit interesting electronic and magnetic properties. In this study we have utilized the muon spin rotation/relaxation ($μ^+$SR) technique to study the magnetic properties of the MgReO$_4$ compound. To the best of our knowledge, this is the first investigation reported on this interesting material, that is stabilized in a wolframite crystal structure using a special high-pressure synthesis technique. Bulk magnetic studies show the onset of an antiferromagnetic (AF) long range order, or a possible singlet spin state at $T_{\rm C1}\approx90$~K, with a subtle second high-temperature transition at $T_{\rm C2}\approx280$~K. Both transitions are also confirmed by heat capacity ($C_p$) measurements. From our $μ^+$SR measurements, it is clear that the sample enters an AF order below $T_{\rm C1}=T_{\rm N}\approx85$~K. We find no evidence of magnetic signal above $T_{\rm N}$, which indicates that $T_{\rm C2}$ is likely linked to a structural transition. Further, via sensitive zero field (ZF) $μ^+$SR measurements we find evidence of a spin reorientation at $T_{\rm Cant}\approx65$~K. This points towards a transition from a collinear AF into a canted AF order at low temperature, which is proposed to be driven by competing magnetic interactions.

cond-mat.str-el

Pressure-Induced Restoration of the Reversed Crystal-Field Splitting in $α$-Sr$_2$CrO$_4$

Motivated by an experimental finding that the successive phase transitions in $α$-Sr$_2$CrO$_4$ observed at ambient pressure ceases to exist under high pressures, we carry out the density-functional-theory-based electronic structure calculations and demonstrate that the reversal of the crystal-field splitting reported previously is restored under high pressures, so that the orbital degrees of freedom disappears, resulting in the single phase transition that divides the system into high-temperature Mott insulating and low-temperature antiferromagnetic insulating phases.

cond-mat.str-el

Na-ion dynamics in Quasi-1D compound NaV2O4

We have used the pulsed muon source at ISIS to study high-temperature Na-ion dynamics in the quasi-one-dimensional (Q1D) metallic antiferromagnet NaV2O4. By performing systematic zero-field and longitudinal-field measurements as a function of temperature we clearly distinguish that the hopping rate increases exponentially above Tdiff=250 K. The data is well fitted to an Arrhenius type equation typical for a diffusion process, showing that the Na-ions starts to be mobile above Tdiff . Such results makes this compound very interesting for the tuning of Q1D magnetism using atomic-scale ion-texturing through the periodic potential from ordered Na-vacancies. Further, it also opens the door to possible use of NaV2O4 and related compounds in energy related applications.

cond-mat.mtrl-sci

Spontaneous magnetization and magnetic susceptibility of LaVO3

Five characteristic temperatures of TM = 148 K, TN = 142 K, Tt = 138 K, Tf ~ 125 K and Tg ~ 50 K were found by the measurements of the magnetization curves at various temperature. The spontaneous magnetization appears below TM. It increases up to M_{S} simeq 2 times 10^{-4} mu_{B} at Tt and then decreases steeply below Tt, which qualitatively agrees with the temperature dependence of magnetization obtained under field-cooling (FC) condition. On the other hand, the slope of the magnetization curve, namely the magnetic susceptibility, drops below TN, which coincides with the temperature dependence of magnetization obtained under zero-FC condition, although the magnetization curves were obtained under FC condition. The temperature dependence of the spontaneous magnetization shows a minimum at Tf and a drop at Tg although there is no anomaly in the temperature dependence of FC or ZFC magnetization.

cond-mat.str-el

The magnetic structure of the $zigzag$ chain family Na$_{x}$Ca$_{1-x}$V$_2$O$_4$ determined by muon-spin rotation

We present muon-spin rotation measurements on polycrystalline samples of the complete family of the antiferromagnetic (AF) $zigzag$ chain compounds, Na$_x$Ca$_{1-x}$V$_2$O$_4$. In this family, we explore the magnetic properties from the metallic NaV$_2$O$_4$ to the insulating CaV$_2$O$_4$. We find a critical $x_c(\sim0.833)$ which separates the low and high Na-concentration dependent transition temperature and its magnetic ground state. In the $x x_c$ compounds, multiple sub-phases appear with temperature and $x$. Based on the muon data obtained in zero external magnetic field, a careful dipolar field simulation was able to reproduce the muon behavior and indicates a modulated helical incommensurate spin structure of the metallic AF phase. The incommensurate modulation period obtained by the simulation agrees with that determined by neutron diffraction.

cond-mat.str-el

$^{17}$O NMR Measurements on Superconducting Na$_{0.35}$CoO$_{2} \cdot y$H$_{2}$O

An $^{17}$O NMR measurement was performed on nonoriented polycrystalline Na$_{0.35}$CoO$_2 \cdot y$H$_2$O with superconducting (SC) transition temperature $T_\text{c} = 4.6$ K. A weak temperature dependence was observed in the Knight shift at the O site ($^{17}K$). The spin part of $^{17}K$ ($^{17}K_{\rm spin}$) is estimated from the plot of $^{17}K$ against bulk susceptibility $χ$. The $^{17}K_{\rm spin}$ decreases in the SC state, indicative of the decrease in the in-plane component of the spin susceptibility. The nuclear spin-lattice relaxation rate $1/T_1$ at the O site $^{17}(1/T_1)$ shows a good scaling with $1/T_1$ at the Co site $^{59}(1/T_1)$. This indicates that the spin fluctuations at the O site originate from the Co spin dynamics. The relationships between $^{17}(1/T_1T)$ and $^{17}K_{\rm spin}$ and between $^{17}(1/T_1T)$ and $^{59}(1/T_1T)$ show the development of incommensurate fluctuations at {\bf q $\sim$ 0} other than {\bf q $=$ 0} below 30 K. A clear indication of ferromagnetic correlations at {\bf q $=$ 0} was not observed from the present $^{17}$O-NMR studies.

cond-mat.supr-con

Possible unconventional superconductivity in Na$_x$CoO$_2$yH$_2$O probed by $μ$SR

The superconducting property of recently discovered sodium cobalt oxyhydrate, Na$_{0.35}$CoO$_2$1.3H$_2$O ($T_c=4.5$ K), has been studied by means of muon spin rotation/relaxation ($μ$SR) down to 2 K. It was found that the zero-field muon spin relaxation rate is independent of the temperature, indicating that no static magnetism appears in this compound, at least above 2 K. The result also provides evidence against the breakdown of time-reversal symmetry for the superconducting order parameter. Meanwhile, the muon Knight shift at 60 kOe shows no obvious reduction below $T_c$, suggesting that the local spin susceptibility is preserved upon a superconducting transition. Considering these observations, possible unconventional superconductivity of Na$_{0.35}$CoO$_2$1.3H$_2$O is discussed.

cond-mat.supr-con

Unconventional Upper- and Lower-Critical Fields and Normal-State Magnetic Susceptibility of the Novel Superconducting Compound $Na_{0.35} Co O_2 \cdot 1.3 H_2O$

Magnetic properties of the novel layered superconductor, Na$_{0.35}$CoO$_{2}$$\cdot$1.3H$_{2}$O have been investigated. From the temperature dependence and field dependence of the magnetization, the superconducting transition temperature, as well as upper- and lower-critical fields have been estimated to be $T_{C}=4.6$ K, $H_{C2}(0)=61.0$ T and $H_{C1}(0)=28.1$ Oe. These values give quite unusual phenomenological parameters, \textit{i.e.}, coherent length, penetration depth and Ginzburg-Landau parameter of $ξ=2.32$ nm, $λ=5.68\times 10^{3}$ Å and $κ\equivλ/ξ=244$, suggesting an unconventional nature of superconductivity. Normal-state magnetic susceptibility shows an upturn below 130 K, which is confirmed to be inherent by high-field magnetization data. The upturn may have relevance to the mechanism of the superconductivity.

cond-mat.supr-con