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Kagome superconductors AV3Sb5 (A = K, Rb, Cs) exhibit a characteristic superconducting and charge-density wave (CDW) phase diagram upon carrier doping and chemical substitution. However, the key electronic states responsible for such a phase diagram have yet to be clarified. Here we report a systematic micro-focused angle-resolved photoemission spectroscopy (ARPES) study of Cs(V1-xCrx)3Sb5 as a function of Cr content x, where Cr substitution causes monotonic reduction of superconducting and CDW transition temperatures. We found that the V-derived bands forming saddle points at the M point and Dirac nodes along high-symmetry cuts show an energy shift due to electron doping by Cr substitution, whereas the Sb-derived electron band at the Gamma point remains almost unchanged, signifying an orbital-selective band shift. We also found that band doubling associated with the emergence of three-dimensional CDW identified at x = 0 vanishes at x = 0.25, in line with the disappearance of CDW. A comparison of band diagrams among Ti-, Nb-, and Cr-substituted Cs(V1-xCrx)3Sb5 suggests the importance to simultaneously take into account the two saddle points at the M point and their proximity to the Fermi energy, to understand the complex phase diagram against carrier doping and chemical pressure., Comment: 7 pages, 4 figures

Topotactic chemical reaction (TCR) is a chemical process that transforms one crystalline phase to another while maintaining one or more of the original structural frameworks, typically induced by the local insertion, removal, or replacement of atoms in a crystal. The utilization of TCR in atomic-layer materials and surfaces of bulk crystals leads to exotic quantum phases, as highlighted by the control of topological phases, the emergence of two-dimensional (2D) superconductivity, and the realization of 2D ferromagnetism. Advanced surface-sensitive spectroscopies such as angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM) are leading techniques to visualize the electronic structure of such exotic states and provide us a guide to further functionalize material properties. In this review article, we summarize the recent progress in this field, with particular emphasis on intriguing results obtained by combining spectroscopies and TCR in thin films., Comment: 23 pages, 10 figures

Antiferromagnetic topological insulators (AF TIs) are predicted to exhibit exotic physical properties such as gigantic optical and topological magnetoelectric responses. While a key to achieving such phenomena relies on how to break the symmetry protecting the Dirac-cone surface state (SS) and acquire the mass of Dirac fermions, the mechanism has yet to be clarified. To address this issue, we carried out micro-focused angle-resolved photoemission spectroscopy for GdBi hosting the type-II AF order, and uncovered the stripe-type 2$\times$1 reconstruction of the Fermi surface associated with the AF band folding. Intriguingly, in contrast to NdBi with the type-I AF order displaying the surface-selective Dirac-fermion mass, GdBi shows massless behavior irrespective of AF domains due to the robust topological protection. These results strongly suggest a crucial role of the ThetaTD (time-reversal and translational) symmetry to create the Dirac-fermion mass in AF TIs., Comment: 18 pages, 5 figures

We have performed micro-focused angle-resolved photoemission spectroscopy on NdSb which exhibits the type-I antiferromagnetism below TN = 16 K. We succeeded in selectively observing the band structure for all three types of single-q antiferromagnetic (AF) domains at the surface. We found that two of the three surfaces whose AF-ordering vector lies within the surface plane commonly show twofold symmetric surface states (SSs) around the bulk-band edges, whereas the other surface with an out-of-plane AF-ordering vector displays fourfold symmetric shallow electronlike SS at the Brillouin-zone center. We suggest that these SSs commonly originate from the combination of the PT (space-inversion and time-reversal) symmetry breaking at the surface and the band folding due to the AF order. The present results pave a pathway toward understanding the relationship between the symmetry and the surface electronic states in antiferromagnets., Comment: 23 pages, 7 figures

Objective: Analysis of the electroencephalogram (EEG) for epileptic spike and seizure detection or brain-computer interfaces can be severely hampered by the presence of artifacts. The aim of this study is to describe and evaluate a fast automatic algorithm for ongoing correction of artifacts in continuous EEG recordings, which can be applied offline and online. Methods: The automatic algorithm for ongoing correction of artifacts is based on fast blind source separation. It uses a sliding window technique with overlapping epochs and features in the spatial, temporal and frequency domain to detect and correct ocular, cardiac, muscle and powerline artifacts. Results: The approach was validated in an independent evaluation study on publicly available continuous EEG data with 2035 marked artifacts. Validation confirmed that 88% of the artifacts could be removed successfully (ocular: 81%, cardiac: 84%, muscle: 98%, powerline: 100%). It outperformed state-of-the-art algorithms both in terms of artifact reduction rates and computation time. Conclusions: Fast ongoing artifact correction successfully removed a good proportion of artifacts, while preserving most of the EEG signals. Significance: The presented algorithm may be useful for ongoing correction of artifacts, e.g., in online systems for epileptic spike and seizure detection or brain-computer interfaces., Comment: 16 pages, 4 figures, 3 tables

Recently discovered kagome superconductors AV3Sb5 (A = K, Rb, Cs) exhibit exotic bulk and surface physical properties such as charge-density wave (CDW) and chirality, whereas their origins remain unresolved. By using micro-focused angle-resolved photoemission spectroscopy, we discovered that AV3Sb5 commonly exhibits two distinct polar surfaces depending on the termination; electron- and hole-doped ones for the A- and Sb-termination, respectively. We observed that the kagome-derived band shows a clear splitting in the A-terminated surface while it is absent in the Sb-terminated counterpart, indicative of the polarity-dependent CDW at the surface. Close comparison of the band-dependent splitting reveals that the three-dimensional CDW structure of the K-terminated surface is different from that of the Rb- or Cs-terminated surface, suggesting the diversity of the CDW ground state. These results provide important insight into the origin of CDW in kagome superconductors AV3Sb5., Comment: 10 pages, 8 figures

Interplay between fermiology and electron correlation is crucial for realizing exotic quantum phases. Transition-metal dichalcogenide (TMD) 1T-TaS2 has sparked a tremendous attention owing to its unique Mott-insulating phase coexisting with the charge-density wave (CDW). However, how the fermiology and electron correlation are associated with such properties has yet to be claried. Here we demonstrate that monolayer 1T-NbTe2 is a new class of two-dimensional TMD which has the star-of-David lattice similarly to bulk TaS2 and isostructural monolayer NbSe2, but exhibits a metallic ground state with an unusual lattice periodicity root19xroot19 characterized by the sparsely occupied star-of-David lattice. By using angle-resolved photoemission and scanning-tunneling spectroscopies in combination with first-principles band-structure calculations, we found that the hidden Fermi-surface nesting and associated CDW formation are a primary cause to realize this unique correlated metallic state with no signature of Mott gap. The present result points to a vital role of underlying fermiology to characterize the Mott phase of TMDs., Comment: To be published in Physical Review B

We performed angle-resolved photoemission spectroscopy with micro-focused beam on a topological line-nodal compound CaSb2 which undergoes a superconducting transition at the onset Tc~1.8 K, to clarify the Fermi-surface topology relevant to the occurrence of superconductivity. We found that a three-dimensional hole pocket at the G point is commonly seen for two types of single-crystalline samples fabricated by different growth conditions. On the other hand, the carrier-doping level estimated from the position of the chemical potential was found to be sensitive to the sample fabrication condition. The cylindrical electron pocket at the Y(C) point predicted by the calculations is absent in one of the two samples, despite the fact that both samples commonly show superconductivity with similar Ts's. This suggests a key role of the three-dimensional hole pocket to the occurrence of superconductivity, and further points to an intriguing possibility to control the topological nature of superconductivity by carrier tuning in CaSb2., Comment: 7 pages, 3 figures

Polar surface and interface play a pivotal role for realizing exotic properties of materials, and a search for such polar states is of crucial importance for expanding materials' functionality. Here we report micro-focused angle-resolved photoemission spectroscopy of CsV3Sb5, a member of recently discovered kagome superconductors AV3Sb5 (A = K, Rb, Cs), and show evidence for the polar nature of cleaved surface which is characterized by Cs- and Sb-terminated surfaces with markedly different fermiology. The Cs-terminated surface shows intriguing doubling of V-derived bands at low temperature associated with the band folding due to the three-dimensional charge-density wave (CDW), whereas the Sb-terminated one shows no band doubling or resultant CDW-gap opening indicative of the suppression of bulk-originated CDW due to polar charge. Such polar-surface-dependent band structure must be incorporated for understanding the origin of unconventional superconducting and charge order at the surface of AV3Sb5., Comment: 10 pages, 13 figures

For solid-state materials, the electronic structure, E(k), is critical in determining a crystal's physical properties. By experimentally detecting the electronic structure, the fundamental physics can be revealed. Angle-resolved photoemission spectroscopy (ARPES) is a powerful technique for directly observing the electronic structure with energy- and momentum-resolved information. Over the past decades, major improvements in the energy and momentum resolution, alongside the extension of ARPES observables to spin (SpinARPES), micrometer or nanometer lateral dimensions (MicroARPES/NanoARPES), and femtosecond timescales (TrARPES), have led to major scientific advances. These advantages have been achieved across a wide range of quantum materials, such as high-temperature superconductors, topological materials, two-dimensional materials and heterostructures. This primer introduces key aspects of ARPES principles, instrumentation, data analysis, and representative scientific cases to demonstrate the power of the method. Perspectives and challenges on future developments are also discussed., Comment: Invited Review article for Nature Reviews Methods Primers

Kagome lattices offer a fertile ground to explore exotic quantum phenomena associated with electron correlation and band topology. The recent discovery of superconductivity coexisting with charge-density wave (CDW) in the kagome metals KV3Sb5, RbV3Sb5, and CsV3Sb5 suggests an intriguing entanglement of electronic order and superconductivity. However, the microscopic origin of CDW, a key to understanding the superconducting mechanism and its possible topological nature, remains elusive. Here, we report angle-resolved photoemission spectroscopy of KV3Sb5 and demonstrate a substantial reconstruction of Fermi surface in the CDW state that accompanies the formation of small three-dimensional pockets. The CDW gap exhibits a periodicity of undistorted Brillouin zone along the out-of-plane wave vector, signifying a dominant role of the in-plane inter-saddle-point scattering to the mechanism of CDW. The characteristics of experimental band dispersion can be captured by first-principles calculations with the inverse star-of-David structural distortion. The present result indicates a direct link between the low-energy excitations and CDW, and puts constraints on the microscopic theory of superconductivity in alkali-metal kagome lattices., Comment: 25 pages, 3 figures

Kagome metals AV3Sb5 (A = K, Rb, and Cs) exhibit a characteristic superconducting ground state coexisting with charge-density wave (CDW), whereas the mechanisms of the superconductivity and CDW have yet to be clarified. Here we report a systematic ARPES study of Cs(V1-xNbx)3Sb5 as a function of Nb content x, where isovalent Nb substitution causes an enhancement of superconducting transition temperature (Tc) and the reduction of CDW temperature (TCDW). We found that the Nb substitution shifts the Sb-derived electron band at the Gamma point downward and simultaneously moves the V-derived band around the M point upward to lift up the saddle point (SP) away from the Fermi level, leading to the reduction of CDW-gap magnitude and TCDW. This indicates a primary role of the SP density of states to stabilize CDW. The present result also suggests that the enhancement of superconductivity by Nb substitution is caused by the cooperation between the expansion of the Sb-derived electron pocket and the recovery of the V-derived density of states at the Fermi level., Comment: 6 pages, 3 figures

Kagome metals AV3Sb5 (A = K, Rb, and Cs) exhibit a unique superconducting ground state coexisting with charge-density wave (CDW), whereas how these characteristics are affected by carrier doping remains unexplored because of the lack of an efficient carrier-doping method. Here we report successful electron doping to CsV3Sb5 by Cs dosing, as visualized by angle-resolved photoemission spectroscopy. We found that the electron doping with Cs dosing proceeds in an orbital-selective way, as characterized by a marked increase in electron filling of the Sb 5pz and V 3dxz/yz bands as opposed to relatively insensitive nature of the V 3dxy/x2-y2 bands. By monitoring the temperature evolution of the CDW gap around the M point, we found that the CDW can be completely killed by Cs dosing while keeping the saddle point with the V 3dxy/x2-y2 character almost pinned at the Fermi level. The present result suggests a crucial role of multi-orbital effect to the occurrence of CDW, and provides an important step toward manipulating the CDW and superconductivity in AV3Sb5., Comment: 7 pages, 3 figures

Angle-resolved photoemission spectroscopy using a micro-focused beam spot (micro-ARPES) is becoming a powerful tool to elucidate key electronic states of exotic quantum materials. We have developed a versatile micro-ARPES system based on synchrotron radiation beam focused with a Kirkpatrick-Baez mirror optics. The mirrors are monolithically installed on a stage, which is driven with five-axes motion, and are vibrationally separated from the ARPES measurement system. Spatial mapping of the Auphotolithography pattern on Si signifies the beam spot size of 10 $\mu$m (horizontal) x 12 $\mu$m (vertical) at the sample position, which is well suited to resolve the fine structure in local electronic states. Utilization of the micro beam and the high precision sample motion system enables the accurate spatially resolved band-structure mapping, as demonstrated by the observation of a small band anomaly associated with tiny sample bending near the edge of a cleaved topological insulator single crystal., Comment: 21 pages, 8 figures

Combination of low-dimensionality and electron correlation is vital for exotic quantum phenomena such as the Mott-insulating phase and high-temperature superconductivity. Transition-metal dichalcogenide (TMD) 1T-TaS2 has evoked great interest owing to its unique nonmagnetic Mott-insulator nature coupled with a charge-density-wave (CDW). To functionalize such a complex phase, it is essential to enhance the CDW-Mott transition temperature TCDW-Mott, whereas this was difficult for bulk TMDs with TCDW-Mott < 200 K. Here we report a strong-coupling 2D CDW-Mott phase with a transition temperature onset of ~530 K in monolayer 1T-TaSe2. Furthermore, the electron correlation derived lower Hubbard band survives under external perturbations such as carrier doping and photoexcitation, in contrast to the bulk counterpart. The enhanced Mott-Hubbard and CDW gaps for monolayer TaSe2 compared to NbSe2, originating in the lattice distortion assisted by strengthened correlations and disappearance of interlayer hopping, suggest stabilization of a likely nonmagnetic CDW-Mott insulator phase well above the room temperature. The present result lays the foundation for realizing monolayer CDW-Mott insulator based devices operating at room temperature.

Quasiparticle - a key concept to describe interacting particles - characterizes electron-electron interaction in metals (Fermi liquid) and electron pairing in superconductors. While this concept essentially relies on the simplification of hard-to-solve many-body problem into one-particle picture and residual effects, a difficulty in disentangling many-body effects from experimental quasiparticle signature sometimes hinders unveiling intrinsic low-energy dynamics, as highlighted by the fierce controversy on the origin of Dirac-band anomaly in graphene and dispersion kink in high-temperature superconductors. Here, we propose an approach to solve this fundamental problem - the Bayesian modelling of quasiparticles. We have chosen a topological insulator $\mathrm{TlBi(S,Se)_2}$ as a model system to formulate an inverse problem of quasiparticle spectra with semiparametric Bayesian analysis, and successfully extracted one-particle and many-body characteristics, i.e. the intrinsic energy gap and unusual lifetime in Dirac-quasiparticle bands. Our approach is widely applicable to clarify the quasiparticle dynamics of quantum materials.

Kagome metals AV3Sb5 (A = K, Rb, and Cs) exhibit superconductivity at 0.9-2.5 K and charge-density wave (CDW) at 78-103 K. Key electronic states associated with the CDW and superconductivity remain elusive. Here, we investigate low-energy excitations of CsV3Sb5 by angle-resolved photoemission spectroscopy. We found an energy gap of 70-100 meV at the Dirac-crossing points of linearly dispersive bands, pointing to an importance of spin-orbit coupling. We also found a signature of strongly Fermi-surface and momentum-dependent CDW gap characterized by the larger energy gap of maximally 70 meV for a band forming a saddle point around the M point, the smaller (0-18 meV) gap for a band forming massive Dirac cones, and a zero gap at the Gamma-centered electron pocket. The observed highly anisotropic CDW gap which is enhanced around the M point signifies an importance of scattering channel connecting the saddle points, laying foundation for understanding the nature of CDW and superconductivity in AV3Sb5., Comment: 10 pages, 9 figures

We have performed angle-resolved photoemission spectroscopy on EuIn2As2 which is predicted to be an axion insulator in the antiferromagnetic state. By utilizing soft-x-ray and vacuum-ultraviolet photons, we revealed a three-dimensional hole pocket centered at the Gamma point of bulk Brillouin zone together with a heavily hole-doped surface state in the paramagnetic phase. Upon entering the antiferromagnetic phase, the band structure exhibits a marked reconstruction characterized by the emergence of a "M"-shaped bulk band near the Fermi level. The qualitative agreement with first-principles band-structure calculations suggests the occurrence of bulk-band inversion at the Gamma point in the antiferromagnetic phase. We suggest that EuIn2As2 provides a good opportunity to study the exotic quantum phases associated with possible axion-insulator phase., Comment: 8 pages, 5 figures

We investigated the Dirac-cone state and its modulation when an ultrathin film of topological insulator Bi2Se3 was epitaxially grown on a van-der-Waals ferromagnet Cr2Si2Te6 (CST) by angle-resolved photoemission spectroscopy. We observed a gapless Dirac-cone surface state in 6 quintuple-layer (QL) Bi2Se3 on CST, whereas the Dirac cone exhibits a gap of 0.37 eV in 2QL counterpart. Intriguingly, this gap is much larger than those for Bi2Se3 films on Si(111). We also revealed no discernible change in the gap magnitude across the ferromagnetic transition of CST, suggesting the very small characteristic length and energy scale of the magnetic proximity effect. The present results suggest a crucial role of interfacial coupling for modulating Dirac electrons in topological-insulator hybrids.

We have performed angle-resolved photoemission spectroscopy of Bi(111) thin films grown on Si(111), and investigated the evolution of band structure with temperature. We revealed an unexpectedly large temperature variation of the energy dispersion for the Rashba-split surface state and the quantum-well states, as seen in the highly momentum-dependent energy shift as large as 0.1 eV. A comparison of the band dispersion between experiment and first-principles band-structure calculations suggests that the interlayer spacing at the topmost Bi bilayer expands upon temperature increase. The present study provides a new pathway for investigating the interplay between lattice and electronic states through the temperature dependence of band structure., Comment: 7 pages, 4 figures

We have performed high-resolution angle-resolved photoemission spectroscopy of ternary pnictide CaAuAs which is predicted to be a three-dimensional topological Dirac semimetal (TDS). By accurately determining the bulk-band structure, we have revealed the coexistence of three-dimensional and quasi-two-dimensional Fermi surfaces with dominant hole carriers. The band structure around the Brillouin-zone center is characterized by an energy overlap between hole and electron pockets, in excellent agreement with first-principles band-structure calculations. This indicates the occurrence of bulk-band inversion, supporting the TDS state in CaAuAs. Because of the high tunability in the chemical composition besides the TDS nature, CaAuAs provides a precious opportunity for investigating the quantum phase transition from TDS to other exotic topological phases., Comment: 6 pages, 4 figures

The discovery of high-temperature (Tc) superconductivity in monolayer FeSe on SrTiO3 raised a fundamental question whether high Tc is commonly realized in monolayer iron-based superconductors. Tetragonal FeS is a key material to resolve this issue because bulk FeS is a superconductor with Tc comparable to that of isostructural FeSe. However, difficulty in synthesizing tetragonal monolayer FeS due to its metastable nature has hindered further investigations. Here we report elucidation of band structure of monolayer FeS on SrTiO3, enabled by a unique combination of in-situ topotactic reaction and molecular-beam epitaxy. Our angle-resolved photoemission spectroscopy on FeS and FeSe revealed marked similarities in the electronic structure, such as heavy electron doping and interfacial electron-phonon coupling, both of which have been regarded as possible sources of high Tc in FeSe. However, surprisingly, high-Tc superconductivity is absent in monolayer FeS. This is linked to the weak superconducting pairing in electron-doped multilayer FeS in which the interfacial effects are absent. Our results strongly suggest that the cross-interface electron-phonon coupling enhances Tc only when it cooperates with the pairing interaction inherent to the superconducting layer. This finding provides a key insight to explore new heterointerface high-Tc superconductors., Comment: 6 pages, 3 figures