arXiv subjects

H. Takagi

Publications and source records attributed to H. Takagi.

At least 55 records · Page 3Linked to original sources

arXiv2019

Unusual Valence State in the Antiperovskites Sr$_3$SnO and Sr$_3$PbO Revealed by X-ray Photoelectron Spectroscopy

The class of antiperovskite compounds $A_3B$O ($A$ = Ca, Sr, Ba; $B$ = Sn, Pb) has attracted interest as a candidate 3D Dirac system with topological surface states protected by crystal symmetry. A key factor underlying the rich electronic structure of $A_3B$O is the unusual valence state of $B$, i.e., a formal oxidation state of $-4$. Practically, it is not obvious whether anionic $B$ can be stabilized in thin films, due to its unusual chemistry, as well as the polar surface of $A_3B$O, which may render the growth-front surface unstable. We report X-ray photoelectron spectroscopy (XPS) measurements of single-crystalline films of Sr$_3$SnO and Sr$_3$PbO grown by molecular beam epitaxy (MBE). We observe shifts in the core-level binding energies that originate from anionic Sn and Pb, consistent with density functional theory (DFT) calculations. Near the surface, we observe additional signatures of neutral or cationic Sn and Pb, which may point to an electronic or atomic reconstruction with possible impact on putative topological surface states.

cond-mat.mes-hall↗

arXiv2019

Robust weak antilocalization due to spin-orbital entanglement in Dirac material Sr$_3$SnO

The presence of both inversion ($P$) and time-reversal ($T$) symmetries in solids leads to a well-known double degeneracy of the electronic bands (Kramers degeneracy). When the degeneracy is lifted, spin textures can be directly observed in momentum space, as in topological insulators or in strong Rashba materials. The existence of spin textures with Kramers degeneracy, however, is very difficult to observe directly. Here, we use quantum interference measurements combined with first-principle band structure calculations to provide evidence for the existence of hidden entanglement between spin and momentum in the antiperovskite-type 3D Dirac material Sr$_3$SnO. We find robust weak antilocalization (WAL) independent of the position of $E_\mathrm{F}$. The observed WAL signal at low doping is fitted using a single interference channel, which implies that the different Dirac valleys are mixed by disorder. Notably, this mixing does not suppress WAL, suggesting contrasting interference physics compared to graphene. We identify scattering among axially spin-momentum locked states as a key process that leads to a spin-orbital entanglement, giving rise to robust WAL. Our work sheds light on the subtle role of spin and pseudospin, when both could contribute to the same quantum effect.

cond-mat.mes-hall↗

arXiv2019

Spin splitting and strain in epitaxial monolayer WSe$_2$ on graphene

We present the electronic and structural properties of monolayer WSe$_{2}$ grown by pulsed-laser deposition on monolayer graphene (MLG) on SiC. The spin splitting in the WSe$_{2}$ valence band at $\overline{\mathrm{K}}$ was $Δ_\mathrm{SO}=0.469\pm0.008$ eV by angle-resolved photoemission spectroscopy (ARPES). Synchrotron-based grazing-incidence in-plane X-ray diffraction (XRD) revealed the in-plane lattice constant of monolayer WSe$_{2}$ to be $a_\mathrm{WSe_2}=3.2757\pm0.0008 \mathrm{Å}$. This indicates a lattice compression of -0.19 % from bulk WSe$_{2}$. By using experimentally determined graphene lattice constant ($a_\mathrm{MLG}=2.4575\pm0.0007 \mathrm{Å}$), we found that a 3$\times$3 unit cell of the slightly compressed WSe$_{2}$ is perfectly commensurate with a 4$\times$4 graphene lattice with a mismatch below 0.03 %, which could explain why the monolayer WSe$_{2}$ is compressed on MLG. From XRD and first-principles calculations, however, we conclude that the observed size of strain is negligibly small to account for a discrepancy in $Δ_\mathrm{SO}$ found between exfoliated and epitaxial monolayers in earlier ARPES. In addition, angle-resolved, ultraviolet and X-ray photoelectron spectroscopy shed light on the band alignment between WSe$_{2}$ and MLG/SiC and indicate electron transfer from graphene to the WSe$_{2}$ monolayer. As further revealed by atomic force microscopy, the WSe$_{2}$ island size depends on the number of carbon layers on top of the SiC substrate. This suggests that the epitaxy of WSe$_{2}$ favors the weak van der Waals interactions with graphene while it is perturbed by the influence of the SiC substrate and its carbon buffer layer.

cond-mat.mtrl-sci↗

arXiv2019

Link between magnetism and resistivity upturn in cuprates: a thermal conductivity study of La$_{2-x}$Sr$_x$CuO$_4$

A key unexplained feature of cuprate superconductors is the upturn in their normal state electrical resistivity $ρ(T)$ seen at low temperature inside the pseudogap phase. We examined this issue via measurements of the thermal conductivity $κ(T)$ down to 50 mK and in fields up to 17 T on the cuprate La$_{2-x}$Sr$_x$CuO$_4$ at dopings $p = 0.13$, 0.136, 0.143 and 0.18. At $p$ = 0.136, 0.143, and 0.18, we observe an initial increase of the electronic thermal conductivity $κ_0/T$ as a function of field, as expected in a $d$-wave superconductor. For $p$ = 0.136 and 0.143, further increasing the field then leads to a decrease of $κ_0/T$, which correlates with the onset of spin density-wave order as observed in neutron scattering experiments on the same samples. This decrease of $κ_0/T$ with field is imposed by the Wiedemann-Franz law and the high value of the resistivity in the high-field normal state of these samples. Our study therefore provides a direct link between magnetism and the resistivity upturn in the pseudogap phase of cuprates. We discuss this scenario in the broader context of other cuprates.

cond-mat.supr-con↗

arXiv2019

Pressure-induced structural dimerization in the hyperhoneycomb iridate $β$-Li$_2$IrO$_3$ at low temperatures

A pressure-induced collapse of magnetic ordering in $β$-Li$_2$IrO$_3$ at $P_m\sim1.5- 2$ GPa has previously been interpreted as evidence for possible emergence of spin liquid states in this hyperhoneycomb iridate, raising prospects for experimental realizations of the Kitaev model. Based on structural data obtained at \emph{room temperature}, this magnetic transition is believed to originate in small lattice perturbations that preserve crystal symmetry, and related changes in bond-directional anisotropic exchange interactions. Here we report on the evolution of the crystal structure of $β$-Li$_2$IrO$_3$ under pressure at low temperatures ($T\leq50$ K) and show that the suppression of magnetism coincides with a change in lattice symmetry involving Ir-Ir dimerization. The critical pressure for dimerization shifts from 4.4(2) GPa at room temperature to $\sim1.5-2$ GPa below 50 K. While a direct $Fddd \rightarrow C2/c$ transition is observed at room temperature, the low temperature transitions involve new as well as coexisting dimerized phases. Further investigation of the Ir ($L_3$/$L_2$) isotropic branching ratio in x-ray absorption spectra indicates that the previously reported departure of the electronic ground state from a $J_{\rm{eff}}=1/2$ state is closely related to the onset of dimerized phases. In essence, our results suggest that the predominant mechanism driving the collapse of magnetism in $β$-Li$_2$IrO$_3$ is the pressure-induced formation of Ir$_2$ dimers in the hyperhoneycomb network. The results further confirm the instability of the $J_{\rm{eff}}=1/2$ moments and related non-collinear spiral magnetic ordering against formation of dimers in the low-temperature phase of compressed $β$-Li$_2$IrO$_3$.

cond-mat.str-el↗

arXiv2019

Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet

Ruthenium compounds play prominent roles in materials research ranging from oxide electronics to catalysis, and serve as a platform for fundamental concepts such as spin-triplet superconductivity, Kitaev spin-liquids, and solid-state analogues of the Higgs mode in particle physics. However, basic questions about the electronic structure of ruthenates remain unanswered, because several key parameters (including the Hund's-rule, spin-orbit, and exchange interactions) are comparable in magnitude, and their interplay is poorly understood - partly due to difficulties in synthesizing sizable single crystals for spectroscopic experiments. Here we introduce a resonant inelastic x-ray scattering (RIXS) technique capable of probing collective modes in microcrystals of $4d$-electron materials. We present a comprehensive set of data on spin waves and spin-state transitions in the honeycomb antiferromagnet SrRu$_{2}$O$_{6}$, which possesses an unusually high Néel temperature. The new RIXS method provides fresh insight into the unconventional magnetism of SrRu$_{2}$O$_{6}$, and enables momentum-resolved spectroscopy of a large class of $4d$ transition-metal compounds.

cond-mat.str-el↗

arXiv2019

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.

cond-mat.supr-con↗

arXiv2018

Monoclinic SrIrO$_3$ - A Dirac semimetal produced by non-symmorphic symmetry and spin-orbit coupling

SrIrO$_3$ crystallizes in a monoclinic structure of distorted hexagonal perovskite at ambient pressure. The transport measurements show that the monoclinic SrIrO$_3$ is a low-carrier density semimetal, as in the orthorhombic perovskite polymorph. The electronic structure calculation indicates a semimetallic band structure with Dirac bands at two high-symmetry points of Brillouin zone only when spin-orbit coupling is incorporated, suggesting that the semimetallic state is produced by the strong spin-orbit coupling. We argue that the Dirac bands are protected by the non-symmorphic symmetry of lattice.

cond-mat.str-el↗

arXiv2018

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.

cond-mat.supr-con↗

arXiv2018

Pressure-induced collapse of spin-orbital Mott state in the hyperhoneycomb iridate $β$-Li$_2$IrO$_3$

Hyperhoneycomb iridate $β$-Li$_2$IrO$_3$ is a three-dimensional analogue of two-dimensional honeycomb iridates, such as $α$-Li$_2$IrO$_3$, which recently appeared as another playground for the physics of Kitaev-type spin liquid. $β$-Li$_2$IrO$_3$ shows a non-collinear spiral ordering of spin-orbital-entangled $J_{\rm eff}$ = 1/2 moments at low temperature, which is known to be suppressed under a pressure of $\sim$2 GPa. With further increase of pressure, a structural transition is observed at $P_{\rm S}$ $\sim$ 4 GPa at room temperature. Using the neutron powder diffraction technique, the crystal structure in the high-pressure phase of $β$-Li$_2$IrO$_3$ above $P_{\rm S}$ was refined, which indicates the formation of Ir$_2$ dimers on the zig-zag chains, with the Ir-Ir distance even shorter than that of metallic Ir. We argue that the strong dimerization stabilizes the bonding molecular orbital state comprising the two local $d_{zx}$-orbitals on the Ir-O$_2$-Ir bond plane, which conflicts with the equal superposition of $d_{xy}$-, $d_{yz}$- and $d_{zx}$- orbitals in the $J_{\rm eff}$ = 1/2 wave function produced by strong spin-orbit coupling. The results of resonant inelastic x-ray scattering (RIXS) measurements and the electronic structure calculations are fully consistent with the collapse of the $J_{\rm eff}$ = 1/2 state. A subtle competition of various electronic phases is universal in honeycomb-based Kitaev materials.

cond-mat.str-el↗

arXiv2018

Infrared phonon spectra of quasi-one-dimensional Ta$_2$NiSe$_5$ and Ta$_2$NiS$_5$

Using a combination of infrared ellipsometry, time-domain terahertz spectroscopy, and far-infrared reflectometry we have obtained the $ac$-plane complex dielectric function of monoclinic ($C2/c$) Ta$_2$NiSe$_5$ and orthorhombic ($Cmcm$) Ta$_2$NiS$_5$ single crystals. The identified dipole-active phonon modes polarized along $a$ and $c$ axes are in good agreement with density functional theory calculations. With increasing temperature the $a$-axis phonon modes of Ta$_2$NiSe$_5$ become poorly discernible, as they are superimposed on the electronic background which gradually fills the energy gap near the monoclinic-to-orthorhombic phase transition temperature $T_c$ = 326 K. In Ta$_2$NiS$_5$, which does not exhibit such a structural transition and remains orthorhombic down to low temperatures, the $a$-axis phonon modes are superimposed on a persistent broad electronic mode centered near 16 meV. We attribute this difference to strongly overlapping exciton-phonon complexes in Ta$_2$NiSe$_5$, as opposed to isolated instances of the same in Ta$_2$NiS$_5$, and find this to be in good agreement with an excitonic insulator state below $T_c$ in the former, as compared to the absence of one in the latter.

cond-mat.str-el↗

arXiv2018

Magnetotransport in Sr3PbO antiperovskite with three-dimensional massive Dirac electrons

Novel topological phenomena are anticipated for three-dimensional (3D) Dirac electrons. The magnetotransport properties of cubic ${\rm Sr_{3}PbO}$ antiperovskite, theoretically proposed to be a 3D massive Dirac electron system, are studied. The measurements of Shubnikov-de Haas oscillations and Hall resistivity indicate the presence of a low density ($\sim 1 \times 10^{18}$ ${\rm cm^{-3}}$) of holes with an extremely small cyclotron mass of 0.01-0.06$m_{e}$. The magnetoresistance $Δρ_{xx}(B)$ is linear in magnetic field $B$ with the magnitude independent of temperature. These results are fully consistent with the presence of 3D massive Dirac electrons in ${\rm Sr_{3}PbO}$. The chemical flexibility of the antiperovskites and our findings in the family member, ${\rm Sr_{3}PbO}$, point to their potential as a model system in which to explore exotic topological phases.

cond-mat.mtrl-sci↗

arXiv2018

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.

cond-mat.supr-con↗

arXiv2018

Thermodynamic signatures of quantum criticality in cuprates

The three central phenomena of cuprate superconductors are linked by a common doping $p^{\star}$, where the enigmatic pseudogap phase ends, around which the superconducting phase forms a dome, and at which the resistivity exhibits an anomalous linear dependence on temperature as $T \to 0$. However, the fundamental nature of $p^{\star}$ remains unclear, in particular whether it marks a true quantum phase transition. We have measured the specific heat $C$ of the cuprates Eu-LSCO and Nd-LSCO at low temperature in magnetic fields large enough to suppress superconductivity, over a wide doping range across $p^{\star}$. As a function of doping, we find that the electronic term $C_{\rm el}$ is strongly peaked at $p^{\star}$, where it exhibits a $-T$log$T$ dependence as $T \to 0$. These are the classic signatures of a quantum critical point, as observed in heavy-fermion and iron-based superconductors where their antiferromagnetic phase ends. We conclude that the pseudogap phase of cuprates ends at a quantum critical point, whose associated fluctuations are most likely involved in the $d$-wave pairing and the anomalous scattering.

cond-mat.supr-con↗

arXiv2018

Probing the $J_{eff}=0$ ground state and the Van Vleck paramagnetism of the Ir$^{5+}$ ions in the layered Sr$_2$Co$_{0.5}$Ir$_{0.5}$O$_4$

We report a combined experimental and theoretical x-ray magnetic circular dichroism (XMCD) spectroscopy study at the Ir-$L_{2,3}$ edges on the Ir$^{5+}$ ions of the layered hybrid solid state oxide Sr$_2$Co$_{0.5}$Ir$_{0.5}$O$_4$ with the K$_2$NiF$_4$ structure. From theoretical simulation of the experimental Ir-$L_{2,3}$ XMCD spectrum, we found a deviation from a pure $J_{eff}=0$ ground state with an anisotropic orbital-to-spin moment ratio ($L_x/2S_x$ = 0.43 and $L_z/2S_z$ = 0.78). This deviation is mainly due to multiplet interactions being not small compared to the cubic crystal field and due to the presence of a large tetragonal crystal field associated with the crystal structure. Nevertheless, our calculations show that the energy gap between the singlet ground state and the triplet excited state is still large and that the magnetic properties of the Ir$^{5+}$ ions can be well described in terms of singlet Van Vleck paramagnetism.

cond-mat.str-el↗

arXiv2018

Pseudogap temperature $T^\star$ of cuprate superconductors from the Nernst effect

We use the Nernst effect to delineate the boundary of the pseudogap phase in the temperature-doping phase diagram of cuprate superconductors. New data for the Nernst coefficient $ν(T)$ of YBa$_{2}$Cu$_{3}$O$_{y}$ (YBCO), La$_{1.8-x}$Eu$_{0.2}$Sr$_x$CuO$_4$ (Eu-LSCO) and La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ (Nd-LSCO) are presented and compared with previous data including La$_{2-x}$Sr$_x$CuO$_4$ (LSCO). The temperature $T_ν$ at which $ν/T$ deviates from its high-temperature behaviour is found to coincide with the temperature at which the resistivity deviates from its linear-$T$ dependence, which we take as the definition of the pseudogap temperature $T^\star$- in agreement with gap opening detected in ARPES data. We track $T^\star$ as a function of doping and find that it decreases linearly vs $p$ in all four materials, having the same value in the three LSCO-based cuprates, irrespective of their different crystal structures. At low $p$, $T^\star$ is higher than the onset temperature of the various orders observed in underdoped cuprates, suggesting that these orders are secondary instabilities of the pseudogap phase. A linear extrapolation of $T^\star(p)$ to $p=0$ yields $T^\star(p\to 0)\simeq T_N(0)$, the Néel temperature for the onset of antiferromagnetic order at $p=0$, suggesting that there is a link between pseudogap and antiferromagnetism. With increasing $p$, $T^\star(p)$ extrapolates linearly to zero at $p\simeq p_{\rm c2}$, the critical doping below which superconductivity emerges at high doping, suggesting that the conditions which favour pseudogap formation also favour pairing. We also use the Nernst effect to investigate how far superconducting fluctuations extend above $T_{\rm c}$, as a function of doping, and find that a narrow fluctuation regime tracks $T_{\rm c}$, and not $T^\star$. This confirms that the pseudogap phase is not a form of precursor superconductivity.

cond-mat.supr-con↗

arXiv2018

Direct observation of strain-induced orbital valence band splitting in HfSe$_2$ by sodium intercalation

By using angle-resolved photoemission spectroscopy (ARPES), the variation of the electronic structure of HfSe$_2$ has been studied as a function of sodium intercalation. We observe how this drives a band splitting of the p-orbital valence bands and a simultaneous reduction of the indirect band gap by values of up to 400 and 280 meV respectively. Our calculations indicate that such behaviour is driven by the band deformation potential, which is a result of our observed anisotropic strain induced by sodium intercalation. The applied uniaxial strain calculations based on density functional theory (DFT) agree strongly with the experimental ARPES data. These findings should assist in studying the physical relationship between doping and strain, as well as for large-scale two-dimensional straintronics.

cond-mat.mtrl-sci↗

arXiv2017

Pseudogap phase of cuprate superconductors confined by Fermi surface topology

The properties of cuprate high-temperature superconductors are largely shaped by competing phases whose nature is often a mystery. Chiefly among them is the pseudogap phase, which sets in at a doping $p^*$ that is material-dependent. What determines $p^*$ is currently an open question. Here we show that the pseudogap cannot open on an electron-like Fermi surface, and can only exist below the doping $p_{FS}$ at which the large Fermi surface goes from hole-like to electron-like, so that $p^*$ $\leq$ $p_{FS}$. We derive this result from high-magnetic-field transport measurements in La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ under pressure, which reveal a large and unexpected shift of $p^*$ with pressure, driven by a corresponding shift in $p_{FS}$. This necessary condition for pseudogap formation, imposed by details of the Fermi surface, is a strong constraint for theories of the pseudogap phase. Our finding that $p^*$ can be tuned with a modest pressure opens a new route for experimental studies of the pseudogap.

cond-mat.supr-con↗