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M. Horio

Publications and source records attributed to M. Horio.

At least 37 records · Page 2Linked to original sources

Electronic reconstruction forming a $C_2$-symmetric Dirac semimetal in Ca$_3$Ru$_2$O$_7$

Electronic band structures in solids stem from a periodic potential reflecting the structure of either the crystal lattice or an electronic order. In the stoichiometric ruthenate Ca$_3$Ru$_2$O$_7$, numerous Fermi surface sensitive probes indicate a low-temperature electronic reconstruction. Yet, the causality and the reconstructed band structure remain unsolved. Here, we show by angle-resolved photoemission spectroscopy, how in Ca$_3$Ru$_2$O$_7$ a $C_2$-symmetric massive Dirac semimetal is realized through a Brillouin-zone preserving electronic reconstruction. This Dirac semimetal emerges in a two-stage transition upon cooling. The Dirac point and band velocities are consistent with constraints set by quantum oscillation, thermodynamic, and transport experiments, suggesting that the complete Fermi surface is resolved. The reconstructed structure -- incompatible with translational-symmetry-breaking density waves -- serves as an important test for band structure calculations of correlated electron systems.

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Nematicity in the pseudogap state of cuprate superconductors revealed by angle-resolved photoemission spectroscopy

The nature of the pseudogap and its relationship with superconductivity are one of the central issues of cuprate superconductors. Recently, a possible scenario has been proposed that the pseudogap state is a distinct phase characterized by spontaneous rotational symmetry breaking called "nematicity" based on transport and magnetic susceptibility measurements, where the symmetry breaking was observed below the pseudogap temperature $T^*$. Here, we report a temperature-dependent ARPES study of nematicity in slightly overdoped Bi${}_{1.7}$Pb${}_{0.5}$Sr${}_{1.9}$CaCu${}_2$O${}_{8+δ}$ triggered by a uniaxial strain applied along one of the Cu-O bond directions. While the nematicity was enhanced in the pseudogap state as in the previous studies, it was suppressed in the superconducting state. These results indicate that the pseudogap state is characterized by spontaneous rotational symmetry breaking and that the nematicity may compete with superconductivity. These new experimental insights may provide clues for the nature of the pseudogap and its relation to the superconductivity.

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Extended superconducting dome of electron-doped cuprates after protect annealing revealed by ARPES

The electron-doped cuprates are usually characterized by a more robust antiferromagnetic phase and a much narrower superconducting (SC) dome than those of the hole-doped counterparts. Recently, bulk single crystals of Pr1.3-xLa0.7CexCuO4-δ (PLCCO) prepared by the protect annealing method have been studied extensively and revealed many intriguing properties that were different from those obtained from samples annealed by the conventional methods. Here, we report on a systematic angle-resolved photoemission spectroscopy study of PLCCO single crystals after protect annealing. The results indicate that the actual electron concentration (nFS ) estimated from the Fermi-surface area is significantly larger than the Ce concentration x and the new nFS-based SC dome of PLCCO is more extended towards the overdoped side than the x-based SC dome derived for samples prepared using the conventional annealing method.

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Oxide Fermi liquid universality revealed by electron spectroscopy

We present a combined soft x-ray and high-resolution vacuum-ultraviolet angle-resolved photoemission spectroscopy study of the electron-overdoped cuprate Pr$_{1.3-x}$La$_{0.7}$Ce$_{x}$CuO$_4$ (PLCCO). Demonstration of its highly two-dimensional band structure enabled precise determination of the in-plane self-energy dominated by electron-electron scattering. Through analysis of this self-energy and the Fermi-liquid cut-off energy scale, we find -- in contrast to hole-doped cuprates -- a momentum isotropic and comparatively weak electron correlation in PLCCO. Yet, the self-energies extracted from multiple oxide systems combine to demonstrate a logarithmic divergent relation between the quasiparticle scattering rate and mass. This constitutes a spectroscopic version of the Kadowaki-Woods relation with an important merit -- the demonstration of Fermi liquid quasiparticle lifetime and mass being set by a single energy scale.

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Charge Order Lock-in by Electron-Phonon Coupling in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$

We report an ultrahigh resolution resonant inelastic x-ray scattering (RIXS) study of the in-plane bond-stretching phonon mode in stripe-ordered cuprate La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$. Phonon softening and lifetime shortening are found around the charge ordering wave vector. In addition to these self-energy effects, the electron-phonon coupling is probed by its proportionality to the RIXS cross section. We find an enhancement of the electron-phonon coupling around the charge-stripe ordering wave vector upon cooling into the low-temperature tetragonal structure phase. These results suggest that in addition to electronic correlations, electron-phonon coupling contributes significantly to the emergence of long-range charge-stripe order in cuprates.

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Decoupling of Lattice and Orbital Degrees of Freedom in an Iron-Pnictide Superconductor

The interplay of structural and electronic phases in iron-based superconductors is a central theme in the search for the superconducting pairing mechanism. While electronic nematicity, defined as the breaking of four-fold symmetry triggered by electronic degrees of freedom, is competing with superconductivity, the effect of purely structural orthorhombic order is unexplored. Here, using x-ray diffraction (XRD), we reveal a new structural orthorhombic phase with an exceptionally high onset temperature ($T_\mathrm{ort} \sim 250$ K), which coexists with superconductivity ($T_\mathrm{c} = 25$ K), in an electron-doped iron-pnictide superconductor far from the underdoped region. Furthermore, our angle-resolved photoemission spectroscopy (ARPES) measurements demonstrate the absence of electronic nematic order as the driving mechanism, in contrast to other underdoped iron pnictides where nematicity is commonly found. Our results establish a new, high temperature phase in the phase diagram of iron-pnictide superconductors and impose strong constraints for the modeling of their superconducting pairing mechanism.

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High-Temperature Charge-Stripe Correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$

We use resonant inelastic x-ray scattering to investigate charge-stripe correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$. By differentiating elastic from inelastic scattering, it is demonstrated that charge-stripe correlations precede both the structural low-temperature tetragonal phase and the transport-defined pseudogap onset. The scattering peak amplitude from charge stripes decays approximately as $T^{-2}$ towards our detection limit. The in-plane integrated intensity, however, remains roughly temperature independent. Therefore, although the incommensurability shows a remarkably large increase at high temperature, our results are interpreted via a single scattering constituent. In fact, direct comparison to other stripe-ordered compounds (La$_{1.875}$Ba$_{0.125}$CuO$_4$, La$_{1.475}$Nd$_{0.4}$Sr$_{0.125}$CuO$_4$ and La$_{1.875}$Sr$_{0.125}$CuO$_4$) suggests a roughly constant integrated scattering intensity across all these compounds. Our results therefore provide a unifying picture for the charge-stripe ordering in La-based cuprates. As charge correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$ extend beyond the low-temperature tetragonal and pseudogap phase, their emergence heralds a spontaneous symmetry breaking in this compound.

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Cooperative Interactions Govern the Fermiology of the Polar Metal Ca$_3$Ru$_2$O$_7$

The antiferromagnetic Ruddlesden-Popper ruthenate Ca$_3$Ru$_2$O$_7$ is a model polar metal, combining inversion symmetry breaking with metallic conductivity; however, its low temperature ($T < 48$ K) crystal structure and Fermi surface topology remain ambiguous despite numerous measurements and theoretical studies. Here we perform both first principles calculations with static correlations and angle resolved photoelectron spectroscopy experiments to construct a complete model of Ca$_3$Ru$_2$O$_7$, reconciling inconsistencies among interpretations of electrical transport, thermopower measurements, and momentum- and energy-resolved band dispersions. The solution relies on treating the interplay among Coulomb repulsion, magnetic ordering, spin-orbit interactions, and the RuO$_6$ octahedral degrees-of-freedom on equal footing. For temperatures $30<T < 48$ K, we propose weak electron-electron interactions produce a symmetry-preserving metal-semimetal transition with Weyl nodes in proximity to the Fermi level, whereas a new orthorhombic $Pn2_1a$ structure emerges for $T<30$ K, exhibiting charge and spin density waves from enhanced Coulombic interactions.

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Band-dependent superconducting gap in SrFe$_{2}$(As$_{0.65}$P$_{0.35}$)$_{2}$ studied by angle-resolved photoemission spectroscopy

The isovalent-substituted iron pnictide compound SrFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ exhibits multiple evidence for nodal superconductivity via various experimental probes, such as the penetration depth, nuclear magnetic resonance and specific heat measurements. The direct identification of the nodal superconducting (SC) gap structure is challenging, partly because the presence of nodes is not protected by symmetry but instead caused by an accidental sign change of the order parameter, and also because of the three-dimensionality of the electronic structure. We have studied the SC gaps of SrFe$_{2}$(As$_{0.65}$P$_{0.35}$)$_{2}$ in three-dimensional momentum space by synchrotron and laser-based angle-resolved photoemission spectroscopy. The three hole Fermi surfaces (FSs) at the zone center have SC gaps with different magnitudes, whereas the SC gaps of the electron FSs at the zone corner are almost isotropic and $k_{z}$-independent. We propose that the SC gap of the outer hole FS changes sign around the Z-X [($0, 0, 2π$)-($π,π, 2π$)] direction.

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$d$-wave superconducting gap observed in protect-annealed electron-doped cuprate superconductors Pr$_{1.3-x}$La$_{0.7}$Ce$_{x}$CuO$_{4}$

For electron-doped cuprates, the strong suppression of antiferromagnetic spin correlation by efficient reduction annealing by the "protect-annealing" method leads to superconductivity not only with lower Ce concentrations but also with higher transition temperatures. To reveal the nature of this superconducting state, we have performed angle-resolved photoemission spectroscopy measurements of protect-annealed electron-doped superconductors Pr$_{1.3-x}$La$_{0.7}$Ce$_{x}$CuO$_{4}$ and directly investigated the superconducting gap. The gap was found to be consistent with $d$-wave symmetry, suggesting that strong electron correlation persists and hence antiferromagnetic spin fluctuations remain a candidate that mediates Copper pairing in the protect-annealed electron-doped cuprates.

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Strain-Engineering Mott-Insulating La$_2$CuO$_4$

The transition temperature $T_\textrm{c}$ of unconventional superconductivity is often tunable. For a monolayer of FeSe, for example, the sweet spot is uniquely bound to titanium-oxide substrates. By contrast for La$_{2-\mathrm{x}}$Sr$_\mathrm{x}$CuO$_4$ thin films, such substrates are sub-optimal and the highest $T_\textrm{c}$ is instead obtained using LaSrAlO$_4$. An outstanding challenge is thus to understand the optimal conditions for superconductivity in thin films: which microscopic parameters drive the change in $T_\mathrm{c}$ and how can we tune them? Here we demonstrate, by a combination of x-ray absorption and resonant inelastic x-ray scattering spectroscopy, how the Coulomb and magnetic-exchange interaction of La$_2$CuO$_4$ thin films can be enhanced by compressive strain. Our experiments and theoretical calculations establish that the substrate producing the largest $T_\textrm{c}$ under doping also generates the largest nearest neighbour hopping integral, Coulomb and magnetic-exchange interaction. We hence suggest optimising the parent Mott state as a strategy for enhancing the superconducting transition temperature in cuprates.

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Band Structure of Overdoped Cuprate Superconductors: Density Functional Theory Matching Experiments

A comprehensive angle resolved photoemission spectroscopy study of the band structure in single layer cuprates is presented with the aim of uncovering universal trends across different materials. Five different hole- and electron-doped cuprate superconductors (La$_{1.59}$Eu$_{0.2}$Sr$_{0.21}$CuO$_4$, La$_{1.77}$Sr$_{0.23}$CuO$_4$, Bi$_{1.74}$Pb$_{0.38}$Sr$_{1.88}$CuO$_{6+δ}$, Tl$_{2}$Ba$_{2}$CuO$_{6+δ}$, and Pr$_{1.15}$La$_{0.7}$Ce$_{0.15}$CuO$_{4}$) have been studied with special focus on the bands with predominately $d$-orbital character. Using light polarization analysis, the $e_g$ and $t_{2g}$ bands are identified across these materials. A clear correlation between the $d_{3z^2-r^2}$ band energy and the apical oxygen distance $d_\mathrm{A}$ is demonstrated. Moreover, the compound dependence of the $d_{x^2-y^2}$ band bottom and the $t_{2g}$ band top is revealed. Direct comparison to density functional theory (DFT) calculations employing hybrid exchange-correlation functionals demonstrates excellent agreement. We thus conclude that the DFT methodology can be used to describe the global band structure of overdoped single layer cuprates on both the hole and electron doped side.

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Three-Dimensional Fermi Surface of Overdoped La-Based Cuprates

We present a soft x-ray angle-resolved photoemission spectroscopy study of the overdoped high-temperature superconductors La$_{2-x}$Sr$_x$CuO$_4$ and La$_{1.8-x}$Eu$_{0.2}$Sr$_x$CuO$_4$. In-plane and out-of-plane components of the Fermi surface are mapped by varying the photoemission angle and the incident photon energy. No $k_z$ dispersion is observed along the nodal direction, whereas a significant antinodal $k_z$ dispersion is identified. Based on a tight-binding parametrization, we discuss the implications for the density of states near the van-Hove singularity. Our results suggest that the large electronic specific heat found in overdoped La$_{2-x}$Sr$_x$CuO$_4$ can not be assigned to the van-Hove singularity alone. We therefore propose quantum criticality induced by a collapsing pseudogap phase as a plausible explanation for observed enhancement of electronic specific heat.

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Two-dimensional type-II Dirac fermions in layered oxides

Relativistic massless Dirac fermions can be probed with high-energy physics experiments, but appear also as low-energy quasi-particle excitations in electronic band structures. In condensed matter systems, their massless nature can be protected by crystal symmetries. Classification of such symmetry-protected relativistic band degeneracies has been fruitful, although many of the predicted quasi-particles still await their experimental discovery. Here we reveal, using angle-resolved photoemission spectroscopy, the existence of two-dimensional type-II Dirac fermions in the high-temperature superconductor La$_{1.77}$Sr$_{0.23}$CuO$_4$. The Dirac point, constituting the crossing of $d_{x^2-y^2}$ and $d_{z^2}$ bands, is found approximately one electronvolt below the Fermi level ($E_\mathrm{F}$) and is protected by mirror symmetry. If spin-orbit coupling is considered, the Dirac point degeneracy is lifted and the bands acquire a topologically non-trivial character. In certain nickelate systems, band structure calculations suggest that the same type-II Dirac fermions can be realised near $E_\mathrm{F}$.

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Angle-resolved photoemission spectroscopy of the low-energy electronic structure of superconducting Pr$_2$CuO$_4$ driven by oxygen non-stoichiometry

Bulk crystals of electron-doped cuprates with the T'-type structure require both Ce substitutions and reduction annealing for the emergence of superconductivity while the reduction annealing alone can induce superconductivity in thin films of the T'-type cuprates. In order to reveal low-energy electronic states which are responsible for the superconductivity, we have conducted angle-resolved photoemission spectroscopy measurements on thin films of the superconducting Ce-free T'-type cuprate Pr$_2$CuO$_4$. The results indicate that the overall band structure and the Fermi surface area of the superconducting Pr$_2$CuO$_4$ are similar to those of superconducting Ce-doped bulk single crystals, highlighting the importance of the actual electron concentration rather than the Ce concentration when discussing the physical properties of the T'-type cuprates.

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Electronic Structure of Ce-Doped and -Undoped Nd$_2$CuO$_4$ Superconducting Thin Films Studied by Hard X-ray Photoemission and Soft X-ray Absorption Spectroscopy

In order to realize superconductivity in cuprates with the T'-type structure, not only chemical substitution (Ce doping) but also post-growth reduction annealing is necessary. In the case of thin films, however, well-designed reduction annealing alone without Ce doping can induce superconductivity in the T'-type cuprates. In order to unveil the origin of superconductivity in the Ce-undoped T'-type cuprates, we have performed bulk-sensitive hard x-ray photoemission and soft x-ray absorption spectroscopies on superconducting and non-superconducting Nd$_{2-x}$Ce$_x$CuO$_4$ ($x=$ 0, 0.15, and 0.19) thin films. By post-growth annealing, core-level spectra exhibited dramatic changes, which we attributed to the enhancement of core-hole screening in the CuO$_2$ plane and the shift of chemical potential along with changes in the band filling. The result suggests that the superconducting Nd$_2$CuO$_4$ film is doped with electrons and that the electronic states are similar to those of Ce-doped superconductors.

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Direct Observation of Orbital Hybridisation in a Cuprate Superconductor

The minimal ingredients to explain the essential physics of layered copper-oxide (cuprates= materials remains heavily debated. Effective low energy single-band models of the copper-oxygen orbitals are widely used because there exists no strong experimental evidence supporting multiband structures. Here we report angle-resolved photoelectron spectroscopy experiments on La-based cuprates that provide direct observation of a two-band structure. This electronic structure, qualitatively consistent with density functional theory, is parametrised by a two-orbital ($d_{x^2-y^2}$ and $d_{z^2}$) tight-binding model. We quantify the orbital hybridisation which provides an explanation for the Fermi surface topology and the proximity of the van-Hove singularity to the Fermi level. Our analysis leads to a unification of electronic hopping parameters for single-layer cuprates and we conclude that hybridisation, restraining d-wave pairing, is an important optimisation element for superconductivity.

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Spin-Orbital Excitations in Ca$_{2}$RuO$_4$ Revealed by Resonant Inelastic X-ray Scattering

The strongly correlated insulator Ca$_{2}$RuO$_4$ is considered as a paradigmatic realization of both spin-orbital physics and a band-Mott insulating phase, characterized by orbitally selective coexistence of a band and a Mott gap. We present a high-resolution oxygen $K$-edge resonant inelastic X-ray scattering study of the antiferromagnetic Mott insulating state of Ca$_{2}$RuO$_4$. A set of low-energy ($\sim$80 and 400 meV) and high-energy ($\sim$1.3 and 2.2 eV) excitations are reported that show strong incident light polarization dependence. Our results strongly support a spin-orbit coupled band-Mott scenario and explore in detail the nature of its exotic excitations. Guided by theoretical modelling, we interpret the low-energy excitations as a result of composite spin-orbital excitations. Their nature unveil the intricate interplay of crystal-field splitting and spin-orbit coupling in the band-Mott scenario. The high-energy excitations correspond to intra-atomic singlet-triplet transitions at an energy scale set by the Hund's coupling. Our findings give a unifying picture of the spin and orbital excitations in the band-Mott insulator Ca$_{2}$RuO$_4$.

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