arXiv subjects

K. Yamaura

Publications and source records attributed to K. Yamaura.

At least 19 recordsLinked to original sources

arXiv2025

Spin-orbit-entangled electronic structure of Ba$_2$CaOsO$_6$ studied by O $K$-edge resonant inelastic X-ray scattering

Transition-metal ions with $5d^2$ electronic configuration in a cubic crystal field are prone to have a vanishing dipolar magnetic moment but finite higher-order multipolar moments, and they are expected to exhibit exotic physical properties. Through an investigation using resonant inelastic X-ray spectroscopy (RIXS), Raman spectroscopy, and theoretical ligand-field (LF) multiplet and $ab initio$ calculations, we fully characterized the local electronic structure of Ba$_2$CaOsO$_6$, particularly, the crystal-field symmetry of the 5$d^2$ electrons in this anomalous material. The low-energy multiplet excitations from RIXS at the oxygen $K$ edge and Raman-active phonons both show no splitting. These findings are consistent with the ground state of Os ions dominated by magnetic octupoles. Obtained parameters pave the way for further realistic microscopic studies of this highly unusual class of materials, advancing our understanding of spin-orbit physics in systems with higher-order multipoles.

cond-mat.str-el↗

arXiv2024

Polarity vs Chirality: Functionality from competing magneto-structural instabilities

We report a phenomenological magneto-structural model based on competing free-energy terms that couple either polar or chiral distortions in cubic quadruple perovskites, depending on the global direction of magnetic moments. The model naturally explains why some compounds in this material system host magnetically-induced ferroelectricity at low temperature, while others such as CaMn$_3$(Cr$_3$Mn)O$_{12}$, which we characterise experimentally, do not. Importantly, our results suggest a new approach towards developing an applied multiferroic functionality, and can be generalised to other multi-sublattice systems where the magnetic interaction between sublattices is prohibited by spatial inversion.

cond-mat.mtrl-sci↗

arXiv2023

Magnetic inhomogeneities in the quadruple perovskite manganite [Y$_{2-x}$Mn$_x$]MnMnMn$_4$O$_{12}$

A combination of competing exchange interactions and substitutional disorder gives rise to magnetic inhomogeneities in the [Y$_{2-x}$Mn$_x$]MnMnMn$_4$O$_{12}$ $x = 0.23$ and $x = 0.16$ quadruple perovskite manganites. Our neutron powder scattering measurements show that both the $x = 0.23$ and $x = 0.16$ samples separate into two distinct magnetic phases; below T$_{1}$ = 120 $\pm$ 10 K the system undergoes a transition from a paramagnetic phase to a phase characterised by short range antiferromagnetic clusters contained in a paramagnetic matrix, and below T$_{2}$ $\sim$ 65 K, the system is composed of well correlated long range collinear ferrimagnetic order, punctuated by short range antiferromagnetic clusters. A sharp increase in the antiferromagnetic phase fraction is observed below $\sim$ 33 K, concomitant with a decrease in the ferrimagnetic phase fraction. Our results demonstrate that the theoretically proposed AFM phase is stabilised in the [Y$_{2-x}$Mn$_x$]MnMnMn$_4$O$_{12}$ manganites in the presence of dominant B-B exchange interactions, as predicted.

cond-mat.str-el↗

arXiv2020

Evidence for an extended critical fluctuation region above the polar ordering transition in LiOsO$_3$

Metallic LiOsO$_3$ undergoes a continuous ferroelectric-like structural phase transition below $T_c$ = 140 K to realize a polar metal. To understand the microscopic interactions that drive this transition, we study its critical behavior above $T_c$ via electromechanical coupling - distortions of the lattice induced by short-range dipole-dipole correlations arising from Li off-center displacements. By mapping the full angular distribution of second harmonic electric-quadrupole radiation from LiOsO$_3$ and performing a simplified hyper-polarizable bond model analysis, we uncover subtle symmetry-preserving lattice distortions over a broad temperature range extending from $T_c$ up to around 230 K, characterized by non-uniform changes in the short and long Li-O bond lengths. Such an extended region of critical fluctuations may explain anomalous features reported in specific heat and Raman scattering data, and suggests the presence of competing interactions that are not accounted for in existing theoretical treatments. More broadly, our results showcase how electromechanical effects serve as a probe of critical behavior near inversion symmetry breaking transitions in metals.

cond-mat.str-el↗

arXiv2020

Magnetically driven loss of centrosymmetry in metallic Pb2CoOsO6

We report magnetic, transport, neutron diffraction, and muon spin rotation data showing that Pb$_2$CoOsO$_6$, a newly synthesized metallic double-perovskite with a centrosymmetric space group at room temperature, exhibits a continuous second-order phase transition at 45 K to a magnetically ordered state with a non-centrosymmetric space group. The absence of inversion symmetry is very uncommon in metals, particularly metallic oxides. In contrast to the recently reported ferroelectric-like structural transition in LiOsO$_3$, the phase transition in Pb$_2$CoOsO$_6$ is driven by a long-range collinear antiferromagnetic order, with propagation vector $\textbf{k} = (\frac{1}{2},0,\frac{1}{2})$, which relieves the frustration associated with the symmetry of themagnetic exchanges. This magnetically-driven loss of inversion symmetry represents a new frontier in the search for novel metallic behavior.

cond-mat.str-el↗

arXiv2019

High-$T_c$ Iron-phosphide Superconductivity Enhanced by Reemergent Antiferromagnetic Spin Fluctuations in (Sr$_4$Sc$_2$O$_6$)Fe$_2$(As$_{1-x}$P$_{x}$)$_2$ probed by NMR

We report a systematic NMR study on [Sr$_4$Sc$_2$O$_6$]Fe$_2$(As$_{1-x}$P$_x$)$_2$, for which the local lattice parameters of the iron-pnictogen (Fe$Pn$) layer are similar to those of the series LaFe(As$_{1-x'}$P$_{x'}$)O, which exhibit two segregated antiferromagnetic (AFM) order phases, AFM1 at $x'$=0-0.2 and AFM2 at $x'$=0.4-0.7. Our results revealed that the parent AFM1 phase at $x$=0 disappears at $x$=0.3-0.4, corresponding to a pnictogen height ($h_{pn}$) from the Fe-plane of 1.3-1.32 Å, which is similar to that of LaFe(As$_{1-x'}$P$_{x'}$)O and various parent Fe-pnictides. By contrast, the AFM2 order reported for LaFe(As$_{0.4}$P$_{0.6}$)O does not appear at $x\sim$0.8, although the local lattice parameters of the Fe$Pn$ layer and the microscopic electronic states are quite similar. Despite the absence of the {\it static} AFM2 order, reemergent {\it dynamical} AFM spin fluctuations were observed at approximately $x\sim$0.8, which can be attributed to the instability of the AFM2 phase. We suggest this re-enhancement of AFM spin fluctuations to play a significant role in enhancing the $T_c$ to 17 K for $x$=0.8-1. Finally, we discuss the universality and diversity of the complicated magnetic ground states from a microscopic point of view, including the difference in the origins of the AFM1 and AFM2 phases, and their relations with the high superconducting transitions in Fe-pnictides.

cond-mat.supr-con↗

arXiv2019

Evidence for the weakly coupled electron mechanism in an Anderson-Blount polar metal

Over 50 years ago, Anderson and Blount proposed that ferroelectric-like structural phase transitions may occur in metals, despite the expected screening of the Coulomb interactions that often drive polar transitions. Recently, theoretical treatments have suggested that such transitions require the itinerant electrons be decoupled from the soft transverse optical phonons responsible for polar order. However, this decoupled electron mechanism (DEM) has yet to be experimentally observed. Here we utilize ultrafast spectroscopy to uncover evidence of the DEM in LiOsO$_3$, the first known band metal to undergo a thermally driven polar phase transition ($T_c$ =140 K). We demonstrate that intra-band photo-carriers relax by selectively coupling to only a subset of the phonon spectrum, leaving as much as 60 % of the lattice heat capacity decoupled. This decoupled heat capacity is shown to be consistent with a previously undetected and partially displacive TO polar mode, indicating the DEM in LiOsO$_3$.

cond-mat.str-el↗

arXiv2019

Nature of the magnetism of iridium in the double perovskite Sr2CoIrO6

We report on our investigation on the magnetism of the iridate double perovskite Sr$_2$CoIrO$_6$, a nominally Ir$^{5+}$ Van Vleck $J_{eff}=0$ system. Using x-ray absorption (XAS) and x-ray magnetic circular dichroism (XMCD) spectroscopy at the Ir-$L_{2,3}$ edges, we found a nearly zero orbital contribution to the magnetic moment and thus an apparent breakdown of the $J_{eff}=0$ ground state. By carrying out also XAS and XMCD experiments at the Co-$L_{2,3}$ edges and by performing detailed full atomic multiplet calculations to simulate all spectra, we discovered that the compound consists of about 90% Ir$^{5+}$ ($J_{eff}=0$) and Co$^{3+}$ ($S=2$) and 10% Ir$^{6+}$ ($S=3/2$) and Co$^{2+}$ ($S=3/2$). The magnetic signal of this minority Ir$^{6+}$ component is almost equally strong as that of the main Ir$^{5+}$ component. We infer that there is a competition between the Ir$^{5+}$-Co$^{3+}$ and the Ir$^{6+}$-Co$^{2+}$ configurations in this stoichiometric compound.

cond-mat.str-el↗

arXiv2019

Crossover from itinerant to localized magnetic excitations through the metal-insulator transition in NaOsO$_{\text{3}}$

NaOsO$_{\text{3}}$ undergoes a metal-insulator transition (MIT) at 410 K, concomitant with the onset of antiferromagnetic order. The excitation spectra have been investigated through the MIT by resonant inelastic x-ray scattering (RIXS) at the Os L$_{\text{3}}$ edge. Low resolution ($ΔE \sim$ 300 meV) measurements over a wide range of energies reveal that local electronic excitations do not change appreciably through the MIT. This is consistent with a picture in which structural distortions do not drive the MIT. In contrast, high resolution ($ΔE \sim $ 56 meV) measurements show that the well-defined, low energy magnons in the insulating state weaken and dampen upon approaching the metallic state. Concomitantly, a broad continuum of excitations develops which is well described by the magnetic fluctuations of a nearly antiferromagnetic Fermi liquid. By revealing the continuous evolution of the magnetic quasiparticle spectrum as it changes its character from itinerant to localized, our results provide unprecedented insight into the nature of the MIT in \naoso. In particular, the presence of weak correlations in the paramagnetic phase implies a degree of departure from the ideal Slater limit.

cond-mat.str-el↗

arXiv2019

The magnetic structure and spin-flop transition in the A-site columnar-ordered quadruple perovskite $\mathrm{TmMn_3O_6}$

We present the magnetic structure of $\mathrm{TmMn_3O_6}$, solved via neutron powder diffraction - the first such study of any $R\mathrm{Mn_3O_6}$ A-site columnar-ordered quadruple perovskite to be reported. We demonstrate that long range magnetic order develops below 74 K, and at 28 K a spin-flop transition occurs driven by $f$-$d$ exchange and rare earth single ion anisotropy. In both magnetic phases the magnetic structure may be described as a collinear ferrimagnet, contrary to conventional theories of magnetic order in the manganite perovskites. Instead, we show that these magnetic structures can be understood to arise due to ferro-orbital order, the A, A$'$ and A$''$ site point symmetry, $mm2$, and the dominance of A-B exchange over both A-A and B-B exchange, which together are unique to the $R\mathrm{Mn_3O_6}$ perovskites.

cond-mat.str-el↗

arXiv2018

Direct observation of electron density reconstruction at the metal-insulator transition in NaOsO3

5d transition metal oxides offer new opportunities to test our understanding of the interplay of correlation effects and spin-orbit interactions in materials in the absence of a single dominant interaction. The subtle balance between solid-state interactions can result in new mechanisms that minimize the interaction energy, and in material properties of potential use for applications. We focus here on the 5d transition metal oxide NaOsO3, a strong candidate for the realization of a magnetically driven transition from a metallic to an insulating state exploiting the so-called Slater mechanism. Experimental results are derived from non-resonant and resonant x-ray single crystal diffraction at the Os L-edges. A change in the crystallographic symmetry does not accompany the metal-insulator transition in the Slater mechanism and, indeed, we find no evidence of such a change in NaOsO3. An equally important experimental observation is the emergence of the (300) Bragg peak in the resonant condition with the onset of magnetic order. The intensity of this space-group forbidden Bragg peak continuously increases with decreasing temperature in line with the square of intensity observed for an allowed magnetic Bragg peak. Our main experimental results, the absence of crystal symmetry breaking and the emergence of a space-group forbidden Bragg peak with developing magnetic order, support the use of the Slater mechanism to interpret the metal-insulator transition in NaOsO3. We successfully describe our experimental results with simulations of the electronic structure and, also, with an atomic model based on the established symmetry of the crystal and magnetic structure.

cond-mat.str-el↗

arXiv2018

The magnetic structures of rare-earth quadruple perovskite manganites $R$Mn$_7$O$_{12}$

We report a neutron powder diffraction study of $R$Mn$_7$O$_{12}$ quadruple perovskite manganites with $R$ = La, Ce, Nd, Sm, and Eu. We show that in all measured compounds concomitant magnetic ordering of the $A$ and $B$ manganese sublattices occurs on cooling below the N$\mathrm{\acute{e}}$el temperature. The respective magnetic structures are collinear, with one uncompensated Mn$^{3+}$ moment per formula unit as observed in bulk magnetisation measurements. We show that both LaMn$_7$O$_{12}$ and NdMn$_7$O$_{12}$ undergo a second magnetic phase transition at low temperature, which introduces a canting of the $B$ site sublattice moments that is commensurate in LaMn$_7$O$_{12}$ and incommensurate in NdMn$_7$O$_{12}$. This spin canting is consistent with a magnetic instability originating in the $B$ site orbital order. Furthermore, NdMn$_7$O$_{12}$ displays a third magnetic phase transition at which long range ordering of the Nd sublattice modifies the periodicity of the incommensurate spin canting. Our results demonstrate a rich interplay between transition metal magnetism, orbital order, and the crystal lattice, which may be fine tuned by cation substitution and rare earth magnetism.

cond-mat.str-el↗

arXiv2017

Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6

The electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J=3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the magnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin-gap and ordered local moment is observed, however the magnetic structure, Neel temperature and exchange interactions are unaltered. To explain this behavior it is necessary to include both spin-orbit coupling and hybridization, indicating the importance of an intermediate coupling approach when describing 5$d$ oxides.

cond-mat.str-el↗

arXiv2017

Strongly Gapped Spin-Wave Excitation in the Insulating Phase of NaOsO3

NaOsO3 hosts a rare manifestation of a metal-insulator transition driven by magnetic correlations, placing the magnetic exchange interactions in a central role. We use resonant inelastic x-ray scattering to directly probe these magnetic exchange interactions. A dispersive and strongly gapped (58 meV) excitation is observed indicating appreciable spin-orbit coupling in this 5d3 system. The excitation is well described within a minimal model Hamiltonian with strong anisotropy and Heisenberg exchange (J1=J2=13.9 meV). The observed behavior places NaOsO3 on the boundary between localized and itinerant magnetism.

cond-mat.str-el↗

arXiv2016

Spin-orbit coupling controlled $J=3/2$ electronic ground state in 5$d^{3}$ oxides

Entanglement of spin and orbital degrees of freedom drives the formation of novel quantum and topological physical states. Discovering new spin-orbit entangled ground states and emergent phases of matter requires both experimentally probing the relevant energy scales and applying suitable theoretical models. Here we report resonant inelastic x-ray scattering measurements of the transition metal oxides Ca$_3$LiOsO$_6$ and Ba$_2$YOsO$_6$. We invoke an intermediate coupling approach that incorporates both spin-orbit coupling and electron-electron interactions on an even footing and reveal the ground state of $5d^3$ based compounds, which has remained elusive in previously applied models, is a novel spin-orbit entangled J=3/2 electronic ground state. This work reveals the hidden diversity of spin-orbit controlled ground states in 5d systems and introduces a new arena in the search for spin-orbit controlled phases of matter.

cond-mat.str-el↗

arXiv2016

Anomalous carrier density independent superconductivity in iron pnictides

Dome-shape superconductivity phase diagram can commonly be observed in cuprate and iron-based systems via tuning parameters such as charge carrier doping, pressure, bond angle, and etc. We report doping electrons from transition-metal elements (TM = Co, Ni) substitution can induce high-Tc superconductivity around 35 K in Ca0.94La0.06Fe2As2, which emerges abruptly before the total suppression of the innate spin-density-wave/anti-ferromagnetism (SDW/AFM) state. Unexpectedly, the onset critical temperature for the high-Tc superconductivity stays constant for a wide range of TM doping. Possible extrinsic factors like phase separation, chemical inhomogeneity, and charge carrier cancelation effect are all excluded. This anomalous charge carrier density independent SC is very similar to the interface superconductivity in La2-xSrxCuO4-La2CuO4 bilayer system. The further verified two-dimensional (2D) nature of superconductivity by the Tinkham's angular-dependent critical field model as well as by the angle-resolved magneto-resistance measurements jointly supports the idea of interfacial effect induced high-Tc superconductivity.

cond-mat.supr-con↗

arXiv2015

Electronic correlation assisted ferroelectric metallic state in LiOsO$_3$

LiOsO$_3$ has been recently identified as the first unambiguous "ferroelectric metal", experimentally realizing a prediction from 1965 by Anderson and Blount. In this work, we investigate the metallic state in LiOsO$_3$ by means of infrared spectroscopy supplemented by Density Functional Theory and Dynamical Mean Field Theory calculations. Our measurements and theoretical calculations clearly show that LiOsO$_3$ is a very bad metal with a small quasiparticle weight, close to a Mott-Hubbard localization transition. The agreement between experiments and theory allows us to ascribe all the relevant features in the optical conductivity to strong electron-electron correlations within the $t_{2g}$ manifold of the osmium atoms.

cond-mat.str-el↗

arXiv2015

Fragility of ferromagnetic double exchange interactions and pressure tuning of magnetism in 3d-5d double perovskite Sr2FeOsO6

The ability to tune exchange (magnetic) interactions between 3d transition metals in perovskite structures has proven to be a powerful route to discovery of novel properties. Here we demonstrate that the introduction of 3d-5d exchange pathways in double perovskites enables additional tunability, a result of the large spatial extent of 5d wave functions. Using x-ray probes of magnetism and structure at high pressure, we show that compression of Sr2FeOsO6 drives an unexpected continuous change in the sign of Fe-Os exchange interactions and a transition from antiferromagnetic to ferrimagnetic order. We analyze the relevant electron-electron interactions, shedding light into fundamental differences with the more thoroughly studied 3d-3d systems.

cond-mat.str-el↗