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Hidenori Takagi

Publications and source records attributed to Hidenori Takagi.

At least 19 recordsLinked to original sources

Substrate tuning of the structural and electronic transition in thin flakes of the excitonic insulator candidate Ta$_2$NiSe$_5$

Ta$_2$NiSe$_5$ continues to draw interest for its $T_\textrm{c}$ = 326 K phase transition, whose dual electronic and structural nature reflects a complex interplay of electron-hole (excitonic) and electron-lattice interactions. The majority of studies that have attempted to decipher the relative importance of these interactions, particularly through charge tuning, have been focused on bulk samples. Here, we utilize an all-dry exfoliation and transfer protocol to isolate ultrathin flakes of Ta$_2$NiSe$_5$ on insulating Al$_2$O$_3$ and conducting Au. Using polarized Raman spectroscopy, we uncover the following substrate dependence: Four layers of Ta$_2$NiSe$_5$ on Al$_2$O$_3$ show a sharp structural and electronic transition that is lowered by roughly 40 K from the bulk $T_\textrm{c}$. Meanwhile, four layers of Ta$_2$NiSe$_5$ on Au undergo a structural and electronic transition that is much more gradual with respect to temperature and finishes roughly 150 K below the bulk $T_\textrm{c}$. The pronounced broadening points to an atomic-scale interface effect, wherein electrostatic screening and charge transfer from Au produces a $T_\textrm{c}$ gradient perpendicular to the layers of the flake. We discuss the role of excitonic physics and suggest the possibility for interface engineering to pattern nanoscale junctions in Ta$_2$NiSe$_5$.

cond-mat.str-el↗

Unveiling the nature of collective charge excitations in a cuprate superconductor

Emergent symmetry breakings in condensed matter systems are often intimately linked to collective excitations. For example, the intertwined spin-charge stripe order in cuprate superconductors is associated with spin and charge excitations. While the collective behavior of spin excitations is well established, the nature of charge excitations remains to be understood. Here we present a high-resolution resonant inelastic x-ray scattering (RIXS) study of charge excitations in the stripe-ordered cuprate La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$. The RIXS spectra consist of both charge and phonon excitations around the charge ordering wave vector. By modeling the momentum-dependent phonon intensity, the charge-excitation spectral weight is extracted over a wide energy range. As such, we reveal the highly dispersive nature of the charge excitations, with an energy scale comparable to the spin excitations. Since charge order and superconductivity in cuprates are possibly driven by the same electronic correlations, determining the interaction strength underlying charge order is essential to establishing a comprehensive microscopic model of high-temperature superconductivity.

cond-mat.supr-con↗

Tunable flat band on the surface of a rhombohedral kagome ferromagnet

A central goal in the exploration of kagome-based materials is the realization of a flat band that has meV bandwidth and lies close to the Fermi energy. The prevailing assumption is that band flattening originates from destructive hopping processes on the kagome lattice. We perform scanning tunneling microscopy (STM) on the layered kagome ferromagnet Fe$_3$Sn$_2$ and show that it indeed hosts a flat band near the Fermi energy, which is manifested as a sharp peak in the differential tunneling conductance. First-principles slab calculations reveal, however, that this band is flattened not by the destructive interference of intralayer hopping, but by interlayer hopping between rhombohedral-stacked kagome planes in Fe$_3$Sn$_2$, and is confined to the surface layer. This surface band, forming in the vicinity of the Brillouin zone corners $\bar{K}$ and $\bar{K'}$, exhibits rich magnetic-field dependence, including fine structure due to valley-symmetry breaking by rotated Fe moments, as well as a persistent diamagnetic shift associated with orbital magnetic moments, all reproduced by our calculations. Our results, highlighting the crucial role of layer stacking on the band structure of kagome magnets, demonstrate experimentally an alternative mechanism of generating magnetically tunable flat bands in atomically thin volumes of topological magnets.

cond-mat.str-el↗

Electronic tuning of the soft-phonon transport anomaly in Ta$_2$Ni(S$_x$Se$_{1-x}$)$_5$

Ta$_2$NiSe$_5$ continues to be investigated for its phase transition at $T_\textrm{c}$ = 326 K, where it develops both an electronic gap and a distortion of its Ta/Ni chains. One intriguing feature at $T_\textrm{c}$ seen in thermal transport is the giant anisotropic scattering of phonons moving perpendicular to the chains, which is apparently associated with the softening of a transverse acoustic phonon, but whose microscopic origin and significance demand clarification. By tuning the normal-state band overlap/gap with S substitution, we uncover a close connection between this soft-phonon transport anomaly and underlying electronic instabilities: When Ta$_2$Ni(S$_x$Se$_{1-x}$)$_5$ approaches a band insulator at high $x$, and signatures of the electronic transition are suppressed, the soft-phonon transport anomaly concomitantly vanishes. Our results establish the following picture for the Ta$_2$Ni(S$_x$Se$_{1-x}$)$_5$ family: Near the S end, a sole lattice instability gives rise to a weak structural transition with $T_\textrm{c}$ approaching 130 K. Near the Se end, additional electronic instabilities boost $T_\textrm{c}$ up to 326 K and amplify experimental signatures of the transition. The strong interaction between electrons, holes, and the lattice is manifested as a soft-phonon transport anomaly accompanied by electronic fluctuations, which include excitonic and hybridization-gap fluctuations.

cond-mat.str-el↗

Spinon mediation of witness spin dynamics in herbertsmithite

The kagome lattice of spin-1/2 copper atoms in herbertsmithite is conjectured to sustain a quantum spin liquid state with spinon quasiparticles. Ideally, the kagome crystal planes are each separated by a plane of spinless zinc atoms. However, in real crystals some spin-1/2 copper atoms substitute randomly onto these inter-kagome zinc sites. Here we reconceptualize such 'impurity' atoms as quantum witness spins whose dynamics is designed to probe the spin liquid state. We then introduce spin noise spectroscopy to measure the frequency and temperature dependence of witness spin dynamics, demonstrating that their phenomenology is consistent with extensive interactions between witness spins mediated by propagation of spinons through a quantum spin liquid. Ultimately, a sharp transition occurs at around 260 mK, below which the properties of both spin noise and magnetic susceptibility suggest that the witness spins form a spin glass phase. Among theoretical models considered, we demonstrate that our observations are only consistent with spinon-mediated interactions between witness spins by either a Z2 or U(1) quantum spin liquid, with the former model more closely matching the data. Our work demonstrates that quantum mechanical witness spins may now conceivably be used as a widely applicable probe of quantum spin liquid physics.

cond-mat.str-el↗

Topological Metal-Insulator Transition within the Ferromagnetic state

A major challenge in condensed matter physics is integrating topological phenomena with correlated electron physics to leverage both types of states for next-generation quantum devices. Metal-insulator transitions (MITs) are central to bridging these two domains while simultaneously serving as 'on-off' switches for electronic states. Here, we demonstrate how the prototypical material of K2Cr8O16 undergoes a ferromagnetic MIT accompanied by a change in band topology. Through inelastic x-ray and neutron scattering experiments combined with first-principles theoretical calculations, we demonstrate that this transition is not driven by a Peierls mechanism, given the lack of phonon softening. Instead, we establish the transition as a topological MIT within the ferromagnetic phase (topological-FM-MIT) with potential axionic properties, where electron correlations play a key role in stabilizing the insulating state. This work pioneers the discovery of a topological-FM-MIT and represents a fundamentally new class of topological phase transitions, revealing a unique pathway through which magnetism, topology, and electronic correlations interact.

cond-mat.str-el↗

Quantum size effects on Andreev transport in Nb/Au/Nb Josephson junctions: A combined ab-initio and experimental study

We have measured the critical current density, superconducting coherence length, and superconducting transition temperature of single-domain, epitaxially-grown Nb(110)/Au(111)/Nb(110) trilayers, all of which show a non-monotonic dependence on the thickness of the Au layer. These results are compared with the predictions of a relativistic, ab-initio theory, which incorporates superconducting correlations. We find good agreement with experiment, coming from a rich interplay between superconducting proximity - and quantum size effects, mediated by Andreev bound states. These results suggest that quantum size effects could provide a systematic method of controlling the transport properties of superconducting multilayers.

cond-mat.supr-con↗

Visualizing the internal structure of the charge-density-wave state in CeSbTe

The collective reorganization of electrons into a charge density wave has long served as a textbook example of an ordered phase in condensed matter physics. Two-dimensional square lattices with $p$ electrons are well-suited to the realization of charge density waves, due to the anisotropy of the $p$ orbitals and the resulting one dimensionality of the electronic structure. In spite of a long history of study of charge density waves in square-lattice systems, few reports have recognized the significance of a hidden orbital degree of freedom. The degeneracy of $p_x$ and $p_y$ electrons may give rise to orbital patterns in real space that endow the charge density wave with additional broken symmetries or unusual order parameters. Here, we use scanning tunneling microscopy to visualize the internal structure of the charge-density-wave state of CeSbTe, which contains Sb square lattices with 5$p$ electrons. We image atomic-sized, anisotropic lobes of charge density with periodically modulating anisotropy, which we interpret in terms of a superposition of $p_x$ and $p_y$ bond density waves. Our results support the fact that delocalized $p$ orbitals can reorganize into emergent electronic states of matter.

cond-mat.mes-hall↗

Large Seebeck coefficient driven by "pudding mold" flat band in hole-doped CuRhO$_2$

We report the measurement, using angle-resolved photoemission spectroscopy, of the metallic electronic structure of the hole-doped thermoelectric oxide CuRh$_{0.9}$Mg$_{0.1}$O$_2$. The material is found to have a ``pudding mold'' type band structure, with a nearly flat band edge located near the Fermi level, which is thought to be the origin of the thermoelectric behavior of this material. The experimental data match the density functional theory of the undoped parent compound, simply corrected by a rigid shift of the bands. Transport calculations based on the observed band structure yield a Seebeck coefficient of $\sim 200 \,μ$V/K for the undoped parent material, consistent with experimental measurements. Our results show that CuRhO$_2$ is a textbook example of how pure band-structural effects can result in a large thermoelectric figure of merit, demonstrating that flat band edges in oxides are a realistic route for the efficient conversion of thermal energy.

cond-mat.str-el↗

Hund flat band in a frustrated spinel oxide

Electronic flat bands associated with quenched kinetic energy and heavy electron mass have attracted great interest for promoting strong electronic correlations and emergent phenomena such as high-temperature charge fractionalization and superconductivity. Intense experimental and theoretical research has been devoted to establishing the rich non-trivial metallic and heavy fermion phases intertwined with such localized electronic states. Here, we investigate the transition metal oxide spinel LiV2O4, an enigmatic heavy fermion compound lacking localized f orbital states. We use angle-resolved photoemission spectroscopy and dynamical mean field theory to reveal a new kind of correlation-induced flat band with suppressed inter-atomic electron hopping arising from intra-atomic Hund coupling. The appearance of heavy quasiparticles is ascribed to a proximate orbital-selective Mott state characterized by fluctuating local moments as evidenced by complementary magnetotransport measurements. The spectroscopic fingerprints of long-lived quasiparticles and their disappearance with increasing temperature further support the emergence of a high-temperature bad metal state observed in transport data. This work resolves a long-standing puzzle on the origin of heavy fermion behavior and unconventional transport in LiV2O4. Simultaneously, it opens a new path to achieving flat bands through electronic interactions in d-orbital systems with geometrical frustration, potentially enabling the realization of exotic phases of matter such as the fractionalized Fermi liquids.

cond-mat.str-el↗

Spiral Spin Liquid Noise

An emerging concept for identification of different types of spin liquids is through the use of spontaneous spin noise. Here we develop spin noise spectroscopy for spin liquid studies by considering Ca$_{10}$Cr$_7$O$_{28}$, a material hypothesized to be either a quantum or a spiral spin liquid. By enhancing techniques introduced for magnetic monopole noise studies we measure the time and temperature dependence of spontaneous flux $\varPhi(t, T)$ and thus magnetization $M(t, T)$ of Ca$_{10}$Cr$_7$O$_{28}$ samples. The resulting power spectral density of magnetization noise $S_M(ω,T)$ reveals intense spin fluctuations with $S_M(ω,T) \propto ω^{-α(T)}$ and 0.84 < $α(T)$ < 1.04 . Both the variance $σ_M^2(T)$ and the correlation function $C_M(t,T)$ of this spin noise undergo crossovers at a temperature $T^* \approx$ 450 mK. While predictions for quantum spin liquids are inconsistent with this phenomenology, those from Monte-Carlo simulations of a 2D spiral spin liquid state in Ca$_{10}$Cr$_7$O$_{28}$ yield overall quantitative correspondence with the measured frequency and temperature dependences of $S_M(ω,T), C_M(t,T)$ and $σ_M^2(T)$, thus indicating that Ca$_{10}$Cr$_7$O$_{28}$ is a spiral spin liquid.

cond-mat.str-el↗

Impact of synthesis method on the structure and function of high entropy oxides

The term sample dependence describes the troublesome tendency of nominally equivalent samples to exhibit different physical properties. High entropy oxides (HEOs) are a class of materials where sample dependence has the potential to be particularly profound due to their inherent chemical complexity. In this work, we prepare a spinel HEO of identical nominal composition by five distinct methods, spanning a range of thermodynamic and kinetic conditions: solid state, high pressure, hydrothermal, molten salt, and combustion syntheses. By structurally characterizing these five samples across all length scales with a variety of x-ray methods, we find that while the average structure is unaltered, the samples vary significantly in their local structures and their microstructures. The most profound differences are observed at intermediate length scales, both in terms of crystallite morphology and cation homogeneity. As revealed by x-ray fluorescence microscopy ideal cation homogeneity is achieved only in the case of combustion synthesis. These structural differences in turn significantly alter the observed functional properties, which we demonstrate via characterization of their magnetic response. While ferrimagnetic order is retained across all five samples, the sharpness of the transition, the size of the saturated moment, and the coercivity all show marked variations with synthesis method. We conclude that the chemical flexibility inherent to HEOs is complemented by strong synthesis method dependence, providing another axis along which to optimize these materials for a wide range of applications.

cond-mat.mtrl-sci↗

Closing of the Mott gap near step edges in NiS2

A prototypical charge-transfer type Mott insulator NiS2 pyrite exhibits a metal-insulator transition with bandwidth control. Recent discoveries on surface-specific electronic states on other 3d transition-metal disulfide pyrites motivate us to further investigate the surface of NiS2, where metallic surface conduction is discussed. Here, the spectroscopic-imaging scanning-tunneling-microscopy observations revealed that the surface is not metallic, contrary to the expectation. Instead, the Mott gap is closed near step edges, suggesting possible electrical conduction from one-dimensional channels. The edge anomaly was observed irrespective of its magnetic order and is limited to the insulator phases.

cond-mat.str-el↗

Effect of high pressure synthesis conditions on the formation of high entropy oxides

High entropy materials are often entropy stabilized, meaning that the configurational entropy from multiple elements sharing a single lattice site stabilizes the structure. In this work, we study how high-pressure synthesis conditions can stabilize or destabilize a high entropy oxide (HEO). We study the high-pressure and high-temperature phase equilibria of two well-known families of HEOs: the rock-salt structured compound (Mg,Co,Ni,Cu,Zn)O including some cation substitutions and the spinel structured (Cr,Mn,Fe,Co,Ni)$_3$O$_4$. Syntheses were performed at various temperatures, pressures, and oxygen activity levels resulting in dramatically different synthesis outcomes. In particular, in the rock salt HEO we observe the competing tenorite and wurtzite phases and the possible formation of a layered rock salt phase, while the spinel HEO is highly susceptible to decomposition into a mixture of rock-salt and corundum phases. At the highest tested pressures, 15 GPa, we discover the transformation of the spinel HEO into a metastable modified ludwigite-type structure with nominal formula (Cr,Mn,Fe,Co,Ni)$_4$O$_5$. The relationship between the synthesis conditions and the final reaction product is not straightforward. Nonetheless, we conclude that high-pressure conditions provide an important opportunity to synthesize high entropy phases that cannot be formed any other way.

cond-mat.mtrl-sci↗

Discovery of Superconductivity and Electron-Phonon Drag in the Non-Centrosymmetric Weyl Semimetal LaRhGe$_3$

We present an exploration of the effect of electron-phonon coupling and broken inversion symmetry on the electronic and thermal properties of the semimetal LaRhGe$_3$. Our transport measurements reveal evidence for electron-hole compensation at low temperatures, resulting in a large magnetoresistance of 3000% at 1.8 K and 14 T. The carrier concentration is on the order of $10^{21}\rm{/cm}^3$ with high carrier mobilities of $2000~\rm{cm}^2/\rm{Vs}$. When coupled to our theoretical demonstration of symmetry-protected $\textit{almost movable}$ Weyl nodal lines, we conclude that LaRhGe$_3$ supports a Weyl semimetallic state. We discover superconductivity in this compound with a $T_{\text c}$ of 0.39(1) K and $B_{\rm{c}}(0)$ of 2.2(1) mT, with evidence from specific heat and transverse-field muon spin relaxation. We find an exponential dependence in the normal state electrical resistivity below $\sim50$ K, while Seebeck coefficient and thermal conductivity measurements each reveal a prominent peak at low temperatures, indicative of strong electron-phonon interactions. To this end, we examine the temperature-dependent Raman spectra of LaRhGe$_3$ and find that the lifetime of the lowest energy $A_1$ phonon is dominated by phonon-electron scattering instead of anharmonic decay. We conclude that LaRhGe$_3$ has strong electron-phonon coupling in the normal state, while the superconductivity emerges from weak electron-phonon coupling. These results open up the investigation of electron-phonon interactions in the normal state of superconducting non-centrosymmetric Weyl semimetals.

cond-mat.supr-con↗

Continuum of magnetic excitations in the Kitaev honeycomb iridate D$_3$LiIr$_2$O$_6$

Inelastic neutron scattering (INS) measurements of powder D$_3(^{7}$Li)($^{193}$Ir)$_2$O$_6$ reveal low energy magnetic excitations with a scattering cross section that is broad in $|Q|$ and consistent with a Kitaev spin-liquid (KSL) state. The magnetic nature of the excitation spectrum is demonstrated by longitudinally polarized neutron studies. The total magnetic moment of 1.7(2)$μ_B$/Ir inferred from the total magnetic scattering cross section is consistent with the effective moment inferred from magnetic susceptibility data and expectations for the $J_{\rm eff}=1/2$ single ion state. The rise in the dynamic correlation function ${\cal S}(Q,ω)$ for $\hbarω<5~$meV can be described by a nearest-neighbor Kitaev model with interaction strength $K\approx-13(5)$~meV. Exchange disorder associated with the mixed D-Li site could play an important role in stabilizing the low $T$ quantum fluctuating state.

cond-mat.str-el↗

Unconventional crystal structure of the high-pressure superconductor La$_3$Ni$_2$O$_7$

The discovery of high-temperature superconductivity in La$_3$Ni$_2$O$_7$ at pressures above 14 GPa has spurred extensive research efforts. Yet, fundamental aspects of the superconducting phase, including the possibility of a filamentary character, are currently subjects of controversial debates. Conversely, a crystal structure with NiO$_6$ octahedral bilayers stacked along the $c$-axis direction was consistently posited in initial studies on La$_3$Ni$_2$O$_7$. Here we reassess this structure in optical floating zone-grown La$_3$Ni$_2$O$_7$ single crystals that show signs of filamentary superconductivity. Employing scanning transmission electron microscopy and single-crystal x-ray diffraction under high pressures, we observe multiple crystallographic phases in these crystals, with the majority phase exhibiting alternating monolayers and trilayers of NiO$_6$ octahedra, signifying a profound deviation from the previously suggested bilayer structure. Using density functional theory, we disentangle the individual contributions of the monolayer and trilayer structural units to the electronic band structure of La$_3$Ni$_2$O$_7$, providing a firm basis for advanced theoretical modeling and future evaluations of the potential of the monolayer-trilayer structure for hosting superconductivity.

cond-mat.supr-con↗

Quantum critical Bose gas in the two-dimensional limit in the honeycomb antiferromagnet YbCl$_3$ under magnetic fields

BEC is a quantum phenomenon, where a macroscopic number of bosons occupy the lowest energy state and acquire coherence at low temperatures. It is realized not only in $^4$He and dilute atomic gases, but also in quantum magnets, where hardcore bosons, introduced by the Matsubara-Matsuda transformation of spins, condense. In 3D antiferromagnets, an XY-type long-range ordering (LRO) occurs near a magnetic-field-induced transition to a fully polarized state (FP) and has been successfully described as a BEC in the last few decades. An attractive extension of the BEC in 3D magnets is to make their 2D analogue. For a strictly 2D system, BEC cannot take place due to the presence of a finite density of states at zero energy, and a Berezinskii-Kosterlitz-Thouless (BKT) transition may instead emerge. In a realistic quasi-2D magnet consisting of stacked 2D magnets, a small but finite interlayer coupling stabilizes marginal LRO and BEC, but such that 2D physics, including BKT fluctuations, is still expected to dominate. A few systems were reported to show such 2D-limit BEC, but at very high magnetic fields that are difficult to access. The honeycomb $S$ = 1/2 Heisenberg antiferromagnet YbCl$_3$ with an intra-layer coupling $J\sim$ 5 K exhibits a transition to a FP state at a low in-plane magnetic field of $H_{\rm s}$ = 5.93 T. Here, we demonstrate that the LRO right below $H_{\rm s}$ is a BEC in the 2D-limit stabilized by an extremely small interlayer coupling $J_{\perp}$ of 10$^{-5}J$. At the quantum critical point Hs, we capture 2D-limit quantum fluctuations as the formation of a highly mobile, interacting 2D Bose gas in the dilute limit. A much-reduced effective boson-boson repulsion Ueff as compared with that of a prototypical 3D system indicates the presence of a logarithmic renormalization of interaction unique to 2D.

cond-mat.mtrl-sci↗