Efficiency improvement of spin-resolved ARPES experiments using Gaussian process regression.

The experimental efficiency has been a central concern for time-consuming experiments. Spin- and angle-resolved photoemission spectroscopy (spin-resolved ARPES) is renowned for its inefficiency in spin-detection, despite its outstanding capability to directly determine the spin-polarized electronic properties of materials. Here, we investigate the potential enhancement of the efficiency of spin-resolved ARPES experiments through the integration of measurement informatics. We focus on a representative topological insulator Bi 2 Te 3 , which has well-understood spin-polarized electronic states. We employ Gaussian process regression (GPR) to assess the accumulation of spin polarization information using an indicator known as the GPR score. Our analyses based on the GPR model suggest that the GPR score can serve as a stopping criterion for spin-resolved ARPES experiments. This criterion enables us to conduct efficient spin-resolved ARPES experiments, significantly reducing the time costs by 5-10 times, compared to empirical stopping criteria.

Robust Weak Topological Insulator in the Bismuth Halide Bi_{4}Br_{2}I_{2}.

We apply a topological material design concept for selecting a bulk topology of 3D crystals by different van der Waals stackings of 2D topological insulator layers, and find a bismuth halide Bi_{4}Br_{2}I_{2} to be an ideal weak topological insulator (WTI) with the largest band gap (∼300 meV) among all the WTI candidates, by means of angle-resolved photoemission spectroscopy (ARPES), density functional theory (DFT) calculations, and resistivity measurements. Furthermore, we reveal that the topological surface state of a WTI is not "weak" but rather robust against external perturbations against the initial theoretical prediction by performing potassium deposition experiments. Our results vastly expand future opportunities for fundamental research and device applications with a robust WTI.

Fermi Surface Nesting Driving the RKKY Interaction in the Centrosymmetric Skyrmion Magnet Gd_{2}PdSi_{3}.

The magnetic skyrmions generated in a centrosymmetric crystal were recently first discovered in Gd_{2}PdSi_{3}. In light of this, we observe the electronic structure by angle-resolved photoemission spectroscopy and unveil its direct relationship with the magnetism in this compound. The Fermi surface and band dispersions are demonstrated to have a good agreement with the density functional theory calculations carried out with careful consideration of the crystal superstructure. Most importantly, we find that the three-dimensional Fermi surface has extended nesting which matches well the q vector of the magnetic order detected by recent scattering measurements. The consistency we find among angle-resolved photoemission spectroscopy, density functional theory, and the scattering measurements suggests the Ruderman-Kittel-Kasuya-Yosida interaction involving itinerant electrons to be the formation mechanism of skyrmions in Gd_{2}PdSi_{3}.

Spin polarization of photoelectrons emitted from spin-orbit coupled surface states of Pb/Ge(111).

We report that the spin vector of photoelectrons emitted from an atomic layer Pb grown on a germanium substrate [Pb/Ge(111)] can be controlled using an electric field of light. The spin polarization of photoelectrons excited by a linearly polarized light is precisely investigated by spin- and angle-resolved photoemission spectroscopy. The spin polarization of the photoelectrons observed in the mirror plane reverses between p- and s-polarized lights. Considering the dipole transition selection rule, the surface state of Pb/Ge(111) is represented by a linear combination of symmetric and asymmetric orbital components coupled with spins in mutually opposite directions. The spin direction of the photoelectrons is different from that of the initial state when the electric field vector of linearly polarized light deviates from p- or s-polarization conditions. The quantum interference in the photoexcitation process can determine the direction of the spin vector of photoelectrons.

Broken Screw Rotational Symmetry in the Near-Surface Electronic Structure of AB-Stacked Crystals.

We investigate the electronic structure of 2H-NbS_{2} and h-BN by angle-resolved photoemission spectroscopy (ARPES) and photoemission intensity calculations. Although in bulk form, these materials are expected to exhibit band degeneracy in the k_{z}=π/c plane due to screw rotation and time-reversal symmetries, we observe gapped band dispersion near the surface. We extract from first-principles calculations the near-surface electronic structure probed by ARPES and find that the calculated photoemission spectra from the near-surface region reproduce the gapped ARPES spectra. Our results show that the near-surface electronic structure can be qualitatively different from the bulk electronic structure due to partially broken nonsymmorphic symmetries.

Laser-based angle-resolved photoemission spectroscopy with micrometer spatial resolution and detection of three-dimensional spin vector.

We have developed a state-of-the-art apparatus for laser-based spin- and angle-resolved photoemission spectroscopy with micrometer spatial resolution (µ-SARPES). This equipment is realized by the combination of a high-resolution photoelectron spectrometer, a 6 eV laser with high photon flux that is focused down to a few micrometers, a high-precision sample stage control system, and a double very-low-energy-electron-diffraction spin detector. The setup achieves an energy resolution of 1.5 (5.5) meV without (with) the spin detection mode, compatible with a spatial resolution better than 10 µm. This enables us to probe both spatially-resolved electronic structures and vector information of spin polarization in three dimensions. The performance of µ-SARPES apparatus is demonstrated by presenting ARPES and SARPES results from topological insulators and Au photolithography patterns on a Si (001) substrate.

Time-, spin-, and angle-resolved photoemission spectroscopy with a 1-MHz 10.7-eV pulse laser.

We describe a setup of time-, spin-, and angle-resolved photoemission spectroscopy (tr-SARPES) employing a 10.7 eV (λ = 115.6 nm) pulse laser at a 1 MHz repetition rate as a probe photon source. This equipment effectively combines the technologies of a high-power Yb:fiber laser, ultraviolet-driven harmonic generation in Xe gas, and a SARPES apparatus equipped with very-low-energy-electron-diffraction spin detectors. A high repetition rate (1 MHz) of the probe laser allows experiments with the photoemission space-charge effects significantly reduced, despite a high flux of 1013 photons/s on the sample. The relatively high photon energy (10.7 eV) also brings the capability of observing a wide momentum range that covers the entire Brillouin zone of many materials while ensuring high momentum resolution. The experimental setup overcomes the low efficiency of spin-resolved measurements, which gets even more severe for the pump-probed unoccupied states, and affords the opportunity to investigate ultrafast electron and spin dynamics of modern quantum materials with energy and time resolutions of 25 meV and 360 fs, respectively.

Semiconducting Electronic Structure of the Ferromagnetic Spinel HgCr_{2}Se_{4} Revealed by Soft-X-Ray Angle-Resolved Photoemission Spectroscopy.

We study the electronic structure of the ferromagnetic spinel HgCr_{2}Se_{4} by soft-x-ray angle-resolved photoemission spectroscopy (SX-ARPES) and first-principles calculations. While a theoretical study has predicted that this material is a magnetic Weyl semimetal, SX-ARPES measurements give direct evidence for a semiconducting state in the ferromagnetic phase. Band calculations based on the density functional theory with hybrid functionals reproduce the experimentally determined band gap value, and the calculated band dispersion matches well with ARPES experiments. We conclude that the theoretical prediction of a Weyl semimetal state in HgCr_{2}Se_{4} underestimates the band gap, and this material is a ferromagnetic semiconductor.

Coexistence of Strong and Weak Topological Orders in a Quasi-One-Dimensional Material.

Topological materials have broad application prospects in quantum computing and spintronic devices. Among them, dual topological materials with low dimensionality provide an excellent platform for manipulating various topological states and generating highly conductive spin currents. However, direct observation of their topological surface states still lacks. Here, we reveal the coexistence of the strong and weak topological phases in a quasi-one-dimensional material, TaNiTe_{5}, by spin- and angle- resolved photoemission spectroscopy. The surface states protected by weak topological order forms Dirac-node arcs in the vicinity of the Fermi energy, providing the opportunity to develop spintronics devices with high carrier density that is tunable by bias voltage.

Multipole polaron in the devil's staircase of CeSb.

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 Néel temperature, ~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 4f orbitals, which renormalizes the Sb 5p band prominently, yielding a kink at a very low energy (~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.

Visualization of the strain-induced topological phase transition in a quasi-one-dimensional superconductor TaSe3.

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 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 and spin- and angle-resolved photoemission spectroscopy to visualize the strain-driven band-structure evolution of the quasi-one-dimensional superconductor TaSe3. We demonstrate that it undergoes reversible strain-induced topological phase transitions from a strong topological insulator phase with spin-polarized, quasi-one-dimensional topological surface states, to topologically trivial semimetal and band insulating phases. The quasi-one-dimensional superconductor TaSe3 provides a suitable platform for engineering the topological spintronics, for example as an on/off switch for a spin current that is robust against impurity scattering.

Spatial Control of Charge Doping in n-Type Topological Insulators.

Spatially controlling the Fermi level of topological insulators and keeping their electronic states stable are indispensable processes to put this material into practical use for semiconductor spintronics devices. So far, however, such a method has not been established yet. Here we show a novel method for doping a hole into n-type topological insulators Bi2X3 (X= Se, Te) that overcomes the shortcomings of the previous reported methods. The key of this doping is to adsorb H2O on Bi2X3 decorated with a small amount of carbon, and its trigger is the irradiation of a photon with sufficient energy to excite the core electrons of the outermost layer atoms. This method allows controlling the doping amount by the irradiation time and acts as photolithography. Such a tunable doping makes it possible to design the electronic states at the nanometer scale and, thus, paves a promising avenue toward the realization of novel spintronics devices based on topological insulators.

Observation and control of the weak topological insulator state in ZrTe5.

A quantum spin Hall (QSH) insulator hosts topological states at the one-dimensional (1D) edge, along which backscattering by nonmagnetic impurities is strictly prohibited. Its 3D analogue, a weak topological insulator (WTI), possesses similar quasi-1D topological states confined at side surfaces. The enhanced confinement could provide a route for dissipationless current and better advantages for applications relative to strong topological insulators (STIs). However, the topological side surface is usually not cleavable and is thus hard to observe. Here, we visualize the topological states of the WTI candidate ZrTe5 by spin and angle-resolved photoemission spectroscopy (ARPES): a quasi-1D band with spin-momentum locking was revealed on the side surface. We further demonstrate that the bulk band gap is controlled by external strain, realizing a more stable WTI state or an ideal Dirac semimetal (DS) state. The highly directional spin-current and the tunable band gap in ZrTe5 will provide an excellent platform for applications.

Evidence for a higher-order topological insulator in a three-dimensional material built from van der Waals stacking of bismuth-halide chains.

Low-dimensional van der Waals materials have been extensively studied as a platform with which to generate quantum effects. Advancing this research, topological quantum materials with van der Waals structures are currently receiving a great deal of attention. Here, we use the concept of designing topological materials by the van der Waals stacking of quantum spin Hall insulators. Most interestingly, we find that a slight shift of inversion centre in the unit cell caused by a modification of stacking induces a transition from a trivial insulator to a higher-order topological insulator. Based on this, we present angle-resolved photoemission spectroscopy results showing that the real three-dimensional material Bi4Br4 is a higher-order topological insulator. Our demonstration that various topological states can be selected by stacking chains differently, combined with the advantages of van der Waals materials, offers a playground for engineering topologically non-trivial edge states towards future spintronics applications.

Observation of small Fermi pockets protected by clean CuO2 sheets of a high-T c superconductor.

In cuprate superconductors with high critical transition temperature (T c), light hole-doping to the parent compound, which is an antiferromagnetic Mott insulator, has been predicted to lead to the formation of small Fermi pockets. These pockets, however, have not been observed. Here, we investigate the electronic structure of the five-layered Ba2Ca4Cu5O10(F,O)2, which has inner copper oxide (CuO2) planes with extremely low disorder, and find small Fermi pockets centered at (π/2, π/2) of the Brillouin zone by angle-resolved photoemission spectroscopy and quantum oscillation measurements. The d-wave superconducting gap opens along the pocket, revealing the coexistence between superconductivity and antiferromagnetic ordering in the same CuO2 sheet. These data further indicate that superconductivity can occur without contribution from the antinodal region around (π, 0), which is shared by other competing excitations.

Devil's staircase transition of the electronic structures in CeSb.

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 Néel 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 40 years of intense research. 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. Moreover, we 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.

Coexistence of Two Types of Spin Splitting Originating from Different Symmetries.

The symmetry of a surface or interface plays an important role in determining the spin splitting and texture of a two-dimensional band. Spin-polarized bands of a triangular lattice atomic layer (TLAL) consisting of Sn on a SiC(0001) substrate is investigated by spin- and angle-resolved photoelectron spectroscopy. Surprisingly, both Zeeman- and Rashba-type spin-split bands, without and with spin degeneracy, respectively, coexist at a K point of the Sn TLAL. The K point has a threefold symmetry without inversion symmetry according to the crystal structure including the SiC periodicity, meaning that the Zeeman-type is consistent with the symmetry of the lattice while the Rashba-type is inconsistent. Our density functional calculations reveal that the charge density distribution of the Rashba-type (Zeeman-type) band shows (no) inversion symmetry at the K point. Therefore, the symmetry of the charge density distribution agrees with both types of the spin splitting.

Experimental Methods for Spin- and Angle-Resolved Photoemission Spectroscopy Combined with Polarization-Variable Laser.

The goal of this protocol is to present how to perform spin- and angle-resolved photoemission spectroscopy combined with polarization-variable 7-eV laser (laser-SARPES), and demonstrate a power of this technique for studying solid state physics. Laser-SARPES achieves two great capabilities. Firstly, by examining orbital selection rule of linearly polarized lasers, orbital selective excitation can be carried out in SAPRES experiment. Secondly, the technique can show full information of a variation of the spin quantum axis as a function of the light polarization. To demonstrate the power of the collaboration of these capabilities in laser-SARPES, we apply this technique for the investigations of spin-orbit coupled surface states of Bi2Se3. This technique affords to decompose spin and orbital components from the spin-orbit coupled wavefunctions. Moreover, as a representative advantage of using the direct spin detection collaborated with the polarization-variable laser, the technique unambiguously visualizes the light polarization dependence of the spin quantum axis in three-dimension. Laser-SARPES dramatically increases a capability of photoemission technique.

Experimental Determination of the Topological Phase Diagram in Cerium Monopnictides.

Experimental determinations of bulk band topology in the solid states have been so far restricted to only indirect investigation through the probing of surface states predicted by electronic structure calculations. We here present an alternative approach to determine the band topology by means of bulk-sensitive soft x-ray angle-resolved photoemission spectroscopy. We investigate the bulk electronic structures of the series materials, Ce monopnictides (CeP, CeAs, CeSb, and CeBi). By performing a paradigmatic study of the band structures as a function of their spin-orbit coupling, we draw the topological phase diagram 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 phase transition is elucidated in terms of spin-orbit coupling in concert with their semimetallic band structures. Our comprehensive observations provide a new insight into the band topology hidden in the bulk states.