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Recent developments in laser-excited photoemission electron microscopy (laser-PEEM) advance the visualization of electronic nematicity and nematic domain structures in iron-based superconductors. In FeSe and BaFe$_2$(As$_{0.87}$P$_{0.13}$)$_2$ superconductors, it has been reported that the thickness of the electronic nematic domain walls is unexpectedly long, leading to the formation of mesoscopic nematicity wave [T. Shimojima $\textit{et al.}$, Science $\textbf{373}$ (2021) 1122]. This finding demonstrates that the nematic coherence length $\xi_{\rm nem}$ can be decoupled from the lattice domain wall. Here, we report that the electronic domain wall thickness shows a distinct variation in related materials: it is similarly long in FeSe$_{0.9}$S$_{0.1}$ whereas it is much shorter in undoped BaFe$_2$As$_2$. We find a correlation between the thick domain walls and the non-Fermi liquid properties of normal-state resistivity above the nematic transition temperature. This suggests that the nematic coherence length can be enhanced by underlying spin-orbital fluctuations responsible for the anomalous transport properties., Comment: 5 pages, 3 figures

We study extremely nonequilibrium transport in correlated kagome magnet Mn$_3$Sn by time-resolved terahertz Faraday rotation spectroscopy. When the photoinjected carrier density exceeds $\sim$10$^{20}$ cm$^{-3}$, a cyclotron resonance is clearly observed, signifying the emergence of unusual carriers with 2000-times higher mobility than those in equilibrium. The result can be attributed to a drastic change in the band structure owing to screening of the electron correlation, highlighting the significant role of many-body effects in this kagome compound in equilibrium. Our study opens up a new phase of transport properties in correlated kagome materials under highly nonequilibrium conditions., Comment: 16 pages, 4 figures

HfO$_2$-based ferroelectrics are one of the most actively developed functional materials for memory devices. However, in HfO$_2$-based ferroelectric devices, dielectric breakdown is a main failure mechanism during repeated polarization switching. Elucidation of the breakdown process may broaden the scope of applications for the ferroelectric HfO$_2$. Here, we report direct observations of a breakdown process in HfO$_2$-based ferroelectric capacitors, by \textit{in-situ} laser-based photoemission electron microscopy (laser-PEEM). We have not only clearly visualized the hard dielectric breakdown (HDB) spot, but also observed the regions responsible for the soft dielectric breakdown (SDB) which is a precursor phenomenon to HDB. It was found that the low-resistance region formed after SDB is wider than the conduction path formed after HDB. Furthermore, our spectromicroscopic analysis revealed that the photoelectron spectrum after SDB shows an enhancement in intensity without spectral-shape modulation, interpreted that the initially existed defects are increased. In the HDB spot, however, an additional shoulder structure was observed. These results provide spectroscopic evidence that the electronic states responsible for the conduction path after SDB are different from those after HDB. Through this work, we propose this microscopic approach as a versatile tool for studying buried materials as they are, accelerating the development of material engineering for advanced electronic devices., Comment: 6 pages

The electronic state of WTe2, a candidate of type-II Weyl semimetal, is investigated by using laser-based spin- and angle-resolved photoemission spectroscopy (SARPES). We prepare the pair of WTe2 samples, one with (001) surface and the other with (00-1) surface, by "sandwich method", and measure the band structures of each surface separately. The Fermi arcs are observed on both surfaces. We identify that the Fermi arcs on the two surfaces are both originating from surface states. We further find a surface resonance band, which connects with the Fermi-arc band, forming a Dirac-cone-like band dispersion. Our results indicate that the bulk electron and hole bands are much closer in momentum space than band calculations.

Nematicity is ubiquitous in electronic phases of high transition temperature superconductors, particularly in iron-based superconductors (IBSCs). Order parameter that characterizes the nematic phase has been investigated in momentum space, but its real-space arrangement remains largely unclear. We use linear dichroism (LD) in low-temperature laser-photoemission electron microscope to map out the nematic order parameter of nonmagentic FeSe and antiferromagnetic BaFe2(As0.87P0.13)2. In contrast to the structural domains that have atomic-scale domain walls, the LD patterns in both materials show peculiar sinusoidal waves of electronic nematicity with mesoscopic wavelength. The analysis reveals that the nematic order has an extremely long coherence length, more than 1000 times longer than the unit cell. Our direct visualization of electronic spatial variation uncovers a new fundamental aspect of quantum liquid crystalline states of correlated electrons in IBSCs., Comment: 15 pages, 4 figures, Supplementary materials

In matter, any spontaneous symmetry breaking induces a phase transition characterized by an order parameter, such as the magnetization vector in ferromagnets, or a macroscopic many-electron wave-function in superconductors. Phase transitions with unknown order parameter are rare but extremely appealing, as they may lead to novel physics. An emblematic, and still unsolved, example is the transition of the heavy fermion compound URu$_2$Si$_2$ (URS) into the so-called hidden-order (HO) phase when the temperature drops below $T_0 = 17.5$K. Here we show that the interaction between the heavy fermion and the conduction band states near the Fermi level has a key role in the emergence of the HO phase. Using angle resolved photoemission spectroscopy, we find that while the Fermi surfaces of the HO and of a neighboring antiferromagnetic (AFM) phase of well-defined order parameter have the same topography, they differ in the size of some, but not all, of their electron pockets. Such a non-rigid change of the electronic structure indicates that a change in the interaction strength between states near the Fermi level is a crucial ingredient for the HO-to-AFM phase transition., Comment: 23 pages, 14 figures, 1 ancillary movie

Rare-earth intermetallic compounds exhibit rich phenomena induced by the interplay between localized $f$ orbitals and conduction electrons. However, since the energy scale of the crystal-electric-field splitting is only a few millielectronvolts, the nature of the mobile electrons accompanied by collective crystal-electric-field excitations has not been unveiled. Here, we examine the low-energy electronic structures of CeSb through the anomalous magnetostructural transitions below the N$\'{e}$el temperature, $\sim$17 K, termed the 'devil's staircase', using laser angle-resolved photoemission, Raman and neutron scattering spectroscopies. We report another type of electron-boson coupling between mobile electrons and quadrupole crystal-electric-field excitations of the 4$f$ orbitals, which renormalizes the Sb 5$p$ band prominently, yielding a kink at a very low energy ($\sim$7 meV). This coupling strength is strong and exhibits anomalous step-like enhancement during the devil's staircase transition, unveiling a new type of quasiparticle, named the 'multipole polaron', comprising a mobile electron dressed with a cloud of the quadrupole crystal-electric-field polarization., Comment: 21 pages, 4 figures

Control of the phase transition from topological to normal insulators can allow for an on/off switching of spin current. While topological phase transitions have been realized by elemental substitution in semiconducting alloys, such an approach requires the preparation of materials with various compositions, thus it is quite far from a feasible device application, which demands a reversible operation. Here we use angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES to visualize the strain-driven band structure evolution of the quasi-1D superconductor TaSe3. We demonstrate that it undergoes reversible strain-induced topological phase transitions from a strong topological insulator phase with spin-polarized, quasi-1D topological surface states, to topologically trivial semimetal and band insulating phases. The quasi-1D superconductor TaSe3 provides a suitable platform for engineering the topological spintronics, for example as an on/off switch for spin current robust against impurity scattering.

The superconductivity of high transition temperature (Tc) occurs in copper oxides with carrier-doping to an antiferromagnetic (AF) Mott insulator. This discovery more than thirty years ago immediately led to a prediction about the formation of a small Fermi pocket. This structure, however, has not yet been detected, while it could be a key element in relating high-Tc superconductivity to Mott physics. To address this long-standing issue, we investigate the electronic structure of a five-layered Ba2Ca4Cu5O10(F,O)2 with inner CuO2 planes demonstrated to be cleanest ever in cuprates. Most surprisingly, we find small Fermi surface (FS) pockets closed around (pi/2,pi/2) consistently by angle-resolved photoemission spectroscopy (ARPES) and quantum oscillation measurements. The d-wave superconducting gap opens along the pocket, revealing the coexistence between the superconductivity and AF order in the same CuO2 sheet. Our data further indicate that the superconductivity can occur without contribution from the states near the antinodal region, which are shared by other competing excitations such as the charge density wave (CDW) and pseudogap states. This will have significant implications for understanding the superconductivity and puzzling Fermi arc phenomena in cuprates.

Interfacing bulk conducting topological Bi$_2$Se$_3$ films with s-wave superconductors initiates strong superconducting order in the nontrivial surface states. However, bulk insulating topological (Bi$_{1-x}$Sb$_{x})_2$Te$_3$ films on bulk Nb instead exhibit a giant attenuation of surface superconductivity, even for films only two-layers thick. This massive suppression of proximity pairing is evidenced by ultrahigh-resolution band mappings and by contrasting quantified superconducting gaps with those of heavily n-doped topological Bi$_2$Se$_3$/Nb. The results underscore the limitations of using superconducting proximity effects to realize topological superconductivity in nearly intrinsic systems., Comment: Accepted at Physical Review Letters: https://journals.aps.org/prl/accepted/b0073Y70Ddc12c71a13a3ac871102f6c7e1a1bd7b

Solids with competing interactions often undergo complex phase transitions with a variety of long-periodic modulations. Among such transition, devil's staircase is the most complex phenomenon, and for it, CeSb is the most famous material, where a number of the distinct phases with long-periodic magnetostructures sequentially appear below the Neel temperature. An evolution of the low-energy electronic structure going through the devil's staircase is of special interest, which has, however, been elusive so far despite the 40-years of intense researches. Here we use bulk-sensitive angle-resolved photoemission spectroscopy and reveal the devil's staircase transition of the electronic structures. The magnetic reconstruction dramatically alters the band dispersions at each transition. We moreover find that the well-defined band picture largely collapses around the Fermi energy under the long-periodic modulation of the transitional phase, while it recovers at the transition into the lowest-temperature ground state. Our data provide the first direct evidence for a significant reorganization of the electronic structures and spectral functions occurring during the devil's staircase., Comment: 22 pages, 5 figures

The van der Waals (vdW) materials with low dimensions have been extensively studied as a platform to generate exotic quantum properties. Advancing this view, a great deal of attention is currently paid to topological quantum materials with vdW structures. Here, we provide a new concept of designing topological materials by the vdW stacking of quantum spin Hall insulators (QSHIs). Most interestingly, a slight shift of inversion center in the unit cell caused by a modification of stacking is found to induce the topological variation from a trivial insulator to a higher-order topological insulator (HOTI). Based on that, we present the first experimental realization of a HOTI by investigating a bismuth bromide Bi4Br4 with angle-resolved photoemission spectroscopy (ARPES). The unique feature in bismuth halides capable of selecting various topology only by differently stacking chains, combined with the great advantage of the vdW structure, offers a fascinating playground for engineering topologically non-trivial edge-states toward future spintronics applications., Comment: Nature Materials, in press. The final version of this article is available online at https://doi.org/10.1038/s41563-020-00871-7

A large anomalous Hall effect (AHE) has been observed in ferromagnetic $\textrm{Fe}_3\textrm{Sn}_2$ with breathing kagome bilayers. To understand the underlying mechanism for this, we investigate the electronic structure of $\textrm{Fe}_3\textrm{Sn}_2$ by angle-resolved photoemission spectroscopy (ARPES). In particular, we use both vacuum ultraviolet light (VUV) and soft x ray (SX), which allow surface-sensitive and relatively bulk-sensitive measurements, respectively, and distinguish bulk states from surface states, which should be unlikely related to the AHE. While VUV-ARPES observes two-dimensional bands mostly due to surface states, SX-ARPES reveals three-dimensional band dispersions with a periodicity of the rhombohedral unit cell in the bulk. Our data show a good consistency with a theoretical calculation based on density functional theory, suggesting a possibility that $\textrm{Fe}_3\textrm{Sn}_2$ is a magnetic Weyl semimetal., Comment: 6 pages, 4 figures

Multi-layered materials provide fascinating platforms to realize various functional properties, possibly leading to future electronic devices controlled by external fields. In particular, layered magnets coupled with conducting layers have been extensively studied recently for possible control of their transport properties via the spin structure. Successful control of quantum-transport properties in the materials with antiferromagnetic (AFM) layers, so-called natural spin-valve structure, has been reported for the Dirac Fermion and topological/axion materials. However, a bulk crystal in which magnetic and superconducting layers are alternately stacked has not been realized until now, and the search for functional properties in it is an interesting yet unexplored field in material science. Here, we discover superconductivity providing such an ideal platform in EuSn2As2 with the van der Waals stacking of magnetic Eu layers and superconducting Sn-As layers, and present the first demonstration of a natural spin-valve effect on the superconducting current. Below the superconducting transition temperature (Tc), the electrical resistivity becomes zero in the in-plane direction. In contrast, it, surprisingly, remains finite down to the lowest temperature in the out-of-plane direction, mostly due to the structure of intrinsic magnetic Josephson junctions in EuSn2As2. The magnetic order of the Eu layers (or natural spin-valve) is observed to be extremely soft, allowing one to easy control of the out-of-plane to in-plane resistivities ratio from 1 to infinity by weak external magnetic fields. The concept of multi-functional materials with stacked magnetic-superconducting layers will open a new pathway to develop novel spintronic devices with magnetically controllable superconductivity., Comment: 17 pages, 4 figures

Topological insulators and semimetals as well as unconventional iron-based superconductors have attracted major recent attention in condensed matter physics. Previously, however, little overlap has been identified between these two vibrant fields, even though the principal combination of topological bands and superconductivity promises exotic unprecedented avenues of superconducting states and Majorana bound states (MBSs), the central building block for topological quantum computation. Along with progressing laser-based spin-resolved and angle-resolved photoemission spectroscopy (ARPES) towards high energy and momentum resolution, we have resolved topological insulator (TI) and topological Dirac semimetal (TDS) bands near the Fermi level ($E_{\text{F}}$) in the iron-based superconductors Li(Fe,Co)As and Fe(Te,Se), respectively. The TI and TDS bands can be individually tuned to locate close to $E_{\text{F}}$ by carrier doping, allowing to potentially access a plethora of different superconducting topological states in the same material. Our results reveal the generic coexistence of superconductivity and multiple topological states in iron-based superconductors, rendering these materials a promising platform for high-$T_{\text{c}}$ topological superconductivity., Comment: 9 pages, 6 figures. arXiv admin note: substantial text overlap with arXiv:1803.00846, arXiv:1803.00845

Given the parallelism between the physical properties of Ce and Yb based magnets and heavy fermions due to the electron-hole symmetry, it has been rather odd that the transition temperature of the Yb based compounds is normally very small, as low as $\sim$ 1 K or even lower, whereas Ce counterparts may often have the transition temperature well exceeding 10 K. Here, we report our experimental discovery of the transition temperature reaching 20 K for the first time in a Yb based compound at ambient pressure. The Mn substitution at the Al site in an intermediate valence state of $\alpha$-YbAlB$_{4}$ not only induces antiferromagnetic transition at a record high temperature of 20 K but also transforms the heavy fermion liquid state in $\alpha$-YbAlB$_{4}$ into a highly resistive metallic state proximate to a Kondo insulator., Comment: 7 pages, 3 figures

Topological Dirac semimetals (TDSs) exhibit bulk Dirac cones protected by time reversal and crystal symmetry, as well as surface states originating from non-trivial topology. While there is a manifold possible onset of superconducting order in such systems, few observations of intrinsic superconductivity have so far been reported for TDSs. We observe evidence for a TDS phase in FeTe$_{1-x}$Se$_x$ ($x$ = 0.45), one of the high transition temperature ($T_c$) iron-based superconductors. In angle-resolved photoelectron spectroscopy (ARPES) and transport experiments, we find spin-polarized states overlapping with the bulk states on the (001) surface, and linear magnetoresistance (MR) starting from 6 T. Combined, this strongly suggests the existence of a TDS phase, which is confirmed by theoretical calculations. In total, the topological electronic states in Fe(Te,Se) provide a promising high $T_c$ platform to realize multiple topological superconducting phases., Comment: 6 pages, 4 figures

The major breakthroughs in the understanding of topological materials over the past decade were all triggered by the discovery of the Z$_2$ topological insulator (TI). In three dimensions (3D), the TI is classified as either "strong" or "weak", and experimental confirmations of the strong topological insulator (STI) rapidly followed the theoretical predictions. In contrast, the weak topological insulator has so far eluded experimental verification, since the topological surface states emerge only on particular side surfaces which are typically undetectable in real 3D crystals. Here we provide experimental evidence for the WTI state in a bismuth iodide, $\beta$-Bi4I4. Significantly, the crystal has naturally cleavable top and side planes both stacked via van-der-Waals forces, which have long been desirable for the experimental realization of the WTI state. As a definitive signature of it, we find quasi-1D Dirac TSS at the side-surface (100) while the top-surface (001) is topologically dark. Furthermore, a crystal transition from the $\beta$- to $\alpha$-phase drives a topological phase transition from a nontrivial WTI to the trivial insulator around room temperature. This topological phase, viewed as quantum spin Hall (QSH) insulators stacked three-dimensionally, and excellent functionality with on/off switching will lay a foundation for new technology benefiting from highly directional spin-currents with large density protected against backscattering., Comment: 18 pages, 4 figures

We report an angle-resolved photoemission (ARPES) study of $\beta$-YbAlB$_4$, which is known to harbor unconventional quantum criticality (QC) without any tuning. We directly observe a quasiparticle peak (QP), emerging from hybridization, characterized by a binding energy and an onset of coherence both at about 4 meV. This value conforms with a previously observed reduced Kondo scale at about 40 K. Consistency with an earlier study of carriers in $\beta$-YbAlB$_4$ via the Hall effect strongly suggests that this QP is responsible for the QC in $\beta$-YbAlB$_4$. A comparison with the sister polymorph $\alpha$-YbAlB$_4$, which is not quantum critical at ambient pressure, further supports this result. Indeed, within the limitation of our instrumental resolution, our ARPES measurements do not show tangible sign of hybridization in this locally isomorphic system, while the conduction band we observe is essentially the same as in $\beta$-YbAlB$_4$. We therefore claim that we identified by ARPES the carriers responsible for the QC in $\beta$-YbAlB$_4$. The observed dispersion and the underlying hybridization of this QP are discussed in the context of existing theoretical models., Comment: 12 pages including Supplemental Materials, with 5 figures and 3 supplemental figures

Recent discovery of both gapped and gapless topological phases in weakly correlated electron systems has introduced various relativistic particles and a number of exotic phenomena in condensed matter physics. The Weyl fermion is a prominent example of three dimensional (3D), gapless topological excitation, which has been experimentally identified in inversion symmetry breaking semimetals. However, their realization in spontaneously time reversal symmetry (TRS) breaking magnetically ordered states of correlated materials has so far remained hypothetical. Here, we report a set of experimental evidence for elusive magnetic Weyl fermions in Mn$_3$Sn, a non-collinear antiferromagnet that exhibits a large anomalous Hall effect even at room temperature. Detailed comparison between our angle resolved photoemission spectroscopy (ARPES) measurements and density functional theory (DFT) calculations reveals significant bandwidth renormalization and damping effects due to the strong correlation among Mn 3$d$ electrons. Moreover, our transport measurements have unveiled strong evidence for the chiral anomaly of Weyl fermions, namely, the emergence of positive magnetoconductance only in the presence of parallel electric and magnetic fields. The magnetic Weyl fermions of Mn$_3$Sn have a significant technological potential, since a weak field ($\sim$ 10 mT) is adequate for controlling the distribution of Weyl points and the large fictitious field ($\sim$ a few 100 T) in the momentum space. Our discovery thus lays the foundation for a new field of science and technology involving the magnetic Weyl excitations of strongly correlated electron systems., Comment: 43 pages, 12 figures

We use bulk-sensitive soft X-ray angle-resolved photoemission spectroscopy and investigate bulk electronic structures of Ce monopnictides (CeX; X=P, As, Sb and Bi). By exploiting a paradigmatic study of the band structures as a function of their spin-orbit coupling (SOC), we draw the topological phase diagram of CeX and unambiguously reveal the topological phase transition from a trivial to a nontrivial regime in going from CeP to CeBi induced by the band inversion. The underlying mechanism of the topological phase transition is elucidated in terms of SOC in concert with their semimetallic band structures. Our comprehensive observations provide a new insight into the band topology hidden in the bulk of solid states., Comment: 5 pages, 4 figures

We determine the band structure and spin texture of WTe2 by spin- and angle-resolved photoemission spectroscopy (SARPES). With the support of first-principles calculations, we reveal the existence of spin polarization of both the Fermi arc surface states and bulk Fermi pockets. Our results support WTe2 to be a type-II Weyl semimetal candidate and provide important information to understand its extremely large and nonsaturating magnetoresistance., Comment: Published version

We present an angle-resolved photoemission study of the electronic structure of the three-dimensional pyrochlore iridate Nd2Ir2O7 through its magnetic metal-insulator transition. Our data reveal that metallic Nd2Ir2O7 has a quadratic band, touching the Fermi level at the Gamma point, similarly to that of Pr2Ir2O7. The Fermi node state is, therefore, a common feature of the metallic phase of the pyrochlore iridates. Upon cooling below the transition temperature, this compound exhibits a gap opening with an energy shift of quasiparticle peaks like a band gap insulator. The quasiparticle peaks are strongly suppressed, however, with further decrease of temperature, and eventually vanish at the lowest temperature, leaving a non-dispersive flat band lacking long-lived electrons. We thereby identify a remarkable crossover from Slater to Mott insulators with decreasing temperature. These observations explain the puzzling absence of Weyl points in this material, despite its proximity to the zero temperature metal-insulator transition.