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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.

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.

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 major breakthroughs in understanding of topological materials over the past decade were all triggered by the discovery of the Z2-type topological insulator-a type of material that is insulating in its interior but allows electron flow on its surface. In three dimensions, a topological insulator is classified as either 'strong' or 'weak'1,2, and experimental confirmations of the strong topological insulator rapidly followed theoretical predictions3-5. By contrast, the weak topological insulator (WTI) has so far eluded experimental verification, because the topological surface states emerge only on particular side surfaces, which are typically undetectable in real three-dimensional crystals6-10. Here we provide experimental evidence for the WTI state in a bismuth iodide, β-Bi4I4. Notably, the crystal has naturally cleavable top and side planes-stacked via van der Waals forces-which have long been desirable for the experimental realization of the WTI state11,12. As a definitive signature of this state, we find a quasi-one-dimensional Dirac topological surface state at the side surface (the (100) plane), while the top surface (the (001) plane) is topologically dark with an absence of topological surface states. We also find that a crystal transition from the β-phase to the α-phase drives a topological phase transition from a nontrivial WTI to a normal insulator at roughly room temperature. The weak topological phase-viewed as quantum spin Hall insulators stacked three-dimensionally13,14-will lay a foundation for technology that benefits from highly directional, dense spin currents that are protected against backscattering.

A quantum spin Hall insulator hosts topological states at the one-dimensional edge, along which backscattering by nonmagnetic impurities is strictly prohibited and dissipationless current flows. Its 3D analogue, a weak topological insulator (WTI), possesses similar quasi-1D topological states confined at side surfaces of crystals. The enhanced confinement could provide a route for dissipationless current and better advantages for applications relative to the widely studied strong topological insulators. However, the topological side surface is usually not cleavable and is thus hard to observe by angle-resolved photoemission spectroscopy (ARPES), which has hindered the revealing of the electronic properties of WTIs. Here, we visualize the topological surface states of the WTI candidate ZrTe5 for the first time by spin and angle-resolved photoemission spectroscopy: a quasi-1D band with spin-momentum locking was revealed on the side surface. We further demonstrate that the bulk band gap in ZrTe5 is controlled by strain to the crystal, realizing a more stabilized WTI state or an ideal Dirac semimetal state depending on the direction of the external strain. The highly directional spin-current and the tunable band gap we found in ZrTe5 will provide an excellent platform for applications., 8 pages, 4 figures. Accepted by Nature Communications

Temperature dependence of the band structure, as well as the spin-polarization on the topologically trivial insulator ${\mathrm{TlBiS}}_{2}$ and nontrivial insulator $\mathrm{Tl}\mathrm{Bi}{\mathrm{Se}}_{2}$, have been investigated by spin- and angle-resolved photoelectron spectroscopy. Despite the recent theoretical prediction [Phys. Rev. Lett. 117, 246401 (2016).], topological phase transition (trivial to nontrivial for ${\mathrm{TlBiS}}_{2}$, nontrivial to trivial for $\mathrm{Tl}\mathrm{Bi}{\mathrm{Se}}_{2}$) does not occur in the observed temperature ranges (from 50 to 400 K for ${\mathrm{TlBiS}}_{2}$, from 50 to 475 K for $\mathrm{Tl}\mathrm{Bi}{\mathrm{Se}}_{2}$). Our results indicate that the discrepancy between the theory and the experiment can be understood by considering the overestimation of lattice parameters and the effect of lattice expansion that is neglected in the previous theory. Although some spin-polarized states are observed in ${\mathrm{TlBiS}}_{2}$, it is probably due to the Rashba-like surface (resonant) states and not the topological surface states. On the other hand, the topological surface states in $\mathrm{Tl}\mathrm{Bi}{\mathrm{Se}}_{2}$ is very robust even at 400 K and the spin-polarized states can be used for the real spintronic devices in the large temperature range.

A large anomalous Hall effect (AHE) has been observed in ferromagnetic ${\mathrm{Fe}}_{3}{\mathrm{Sn}}_{2}$ with breathing kagome bilayers. To understand the underlying mechanism for this, we investigate the electronic structure of ${\mathrm{Fe}}_{3}{\mathrm{Sn}}_{2}$ 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 ${\mathrm{Fe}}_{3}{\mathrm{Sn}}_{2}$ is a magnetic Weyl semimetal.

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., 43 pages, 12 figures

Spin–orbit interaction entangles the orbitals with the different spins. The spin–orbital-entangled states were discovered in surface states of topological insulators. However, the spin–orbital-entanglement is not specialized in the topological surface states. Here, we show the spin–orbital texture in a surface state of Bi(111) by laser-based spin- and angle-resolved photoelectron spectroscopy (laser-SARPES) and describe three-dimensional spin-rotation effect in photoemission resulting from spin-dependent quantum interference. Our model reveals that, in the spin–orbit-coupled systems, the spins pointing to the mutually opposite directions are independently locked to the orbital symmetries. Furthermore, direct detection of coherent spin phenomena by laser-SARPES enables us to clarify the phase of the dipole transition matrix element responsible for the spin direction in photoexcited states. These results permit the tuning of the spin polarization of optically excited electrons in solids with strong spin–orbit interaction., Spin–orbit coupling produces spin–orbital-entanglement in quasiparticle eigenstates. Here, Yaji et al. present a general description of spin–orbital-entangled states and establish a model for dipole transition based on spin-dependent quantum interference, that permits optical spin control.

By measuring the spin polarization of GeTe films as a function of light polarization we observed that the bulk states are fully spin polarized in the initial state, in strong contrast with observations for other systems with a strong spin orbit interaction and the surface derived states in the same system. In agreement with state of the art theory, our experimental results show that fully spin polarized bulk states are an intrinsic property of the ferroelectric Rashba semiconductor amp; 945; GeTe 111 . The fact that the measured spin polarization vector does not change with light polarization can be explained by the absence of a mixing of states with a different total angular momentum J

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.

We fabricated spin-polarized surface electronic states with tunable Fermi levels from a semiconductor to low-dimensional metal in the Bi/GaSb(110)-$(2\ifmmode\times\else\texttimes\fi{}1)$ surface using angle-resolved photoelectron spectroscopy (ARPES) and spin-resolved ARPES. The spin-polarized surface band of Bi/GaSb(110) exhibits quasi-one-dimensional character with the Rashba parameter ${\ensuremath{\alpha}}_{\mathrm{R}}$ of 4.1 and 2.6 eV\AA{} at the $\overline{\mathrm{\ensuremath{\Gamma}}}$ and $\overline{\mathrm{Y}}$ points of the surface Brillouin zone, respectively. The Fermi level of the surface electronic state is tuned in situ by element-selective Ar-ion sputtering on the GaSb substrate. The giant Rashba-type spin splitting with switchable metallic/semiconducting character on a semiconductor substrate makes this system a promising candidate for future research in low-dimensional spintronic phenomena.

The semimetallic behavior of the so-called ``failed Kondo insulator'' CeNiSn has been ascribed to a nodal line in the Kondo hybridization derived from a particular symmetry of the Ce $4f$ orbitals ground state. Here we investigate the geometry of the CeNiSn conduction band by combined angle-resolved photoemission spectroscopy (ARPES) in the high-temperature regime and Open core generalized gradient approximation plus spin-orbit coupling calculations, in order to determine how the nodal hybridization takes place. We identify the Fermi sheet involved in the semimetallic regime from its locus and its shape, respectively, in agreement with the expected nodal line and with quantum oscillations. We further extrapolate and discuss the low-temperature Fermi surface in terms of the expected nodal hybridization with a localized $f$-level. The obtained hypothetical low-temperature Fermi surface is compatible with the description from quantum oscillations, and with both the highly anisotropic magnetoresistance and the isotropic Nernst effect. This work offers an overview of the conduction band of CeNiSn before hybridization, and it paves the way to a definitive understanding of its low-temperature state. In addition, this work serves as a basis for more challenging low-temperature ARPES measurements.

The modification of the Au(111) Shockley surface state (SS) by an n-alkane molecule (n-tetratetracontane) monolayer was observed by angle-resolved ultraviolet photoemission spectroscopy. Although there is little chance of chemical interaction in this ideal physisorption system, the volume of the Fermi surface of the SS was significantly reduced accompanied by the formation of large interface electric dipoles. Moreover, Rashba splitting of the SS by spin-orbit interactions was slightly increased upon n-tetratetracontane adsorption, which arose from the decrease in the symmetry of the wave function around the Au nuclei at the surface. The detailed information about the simple physisorption system presented in this paper provides basic knowledge for understanding the electronic structure at the interface between other organic molecules and metal substrates.

The structure and electronic structure of a system comprising molecular layers of n-alkane adsorbed on Au(1 1 1) were investigated to understand the origin of the interfacial electric dipole layer. These alkane molecules are inert and thus van der Waals (vdW) interaction is the primary adsorptive force. Although these vdW interfaces are regarded as ideal physical adsorption systems unlikely to chemically interact with the metal surface, a large interfacial electric dipole layer over 1 eV is formed. It is important to elucidate the mechanism underlying the generation of such large dipole layers to understand the electrode interface in organic semiconductor devices. Thus, this paper elucidates the details of the vdW interface, in particular between tetratetracontane (TTC) and Au(1 1 1). First, the mechanism of growth of the TTC layer up to monolayer thickness was revealed using a low-energy electron-diffraction method. Second, the interface states were newly formed, as determined using angle-resolved photoelectron spectroscopy, X-ray photoemission spectroscopy, and near-edge absorption fine-structure spectroscopy. Our findings indicate, unexpectedly, that a relatively strong inter-orbital interaction governs this vdW interface, similar to a weak chemisorption system rather than a physisorption system.

We reveal the orbital-selective metal-insulator transition in a $4d$ multiorbital system, ${\mathrm{Sr}}_{3}{({\mathrm{Ru}}_{1\ensuremath{-}x}{\mathrm{Mn}}_{x})}_{2}{\mathrm{O}}_{7}\phantom{\rule{4pt}{0ex}}(x=0\ensuremath{-}0.2)$, by means of angle-resolved photoemission spectroscopy. With a small substitution $(x=0.05)$ of Mn with localized $3d$ orbitals, the spectra for the $4{d}_{xy}$ band become incoherent with a large gap, while the $4{d}_{xz/yz}$ bands stay metallic with sharp quasiparticle peaks. Intriguingly, this lifts band hybridization among $4d$ orbitals, and causes a two- to one-dimensional crossover in the remaining Fermi surface. Significant nesting in the remaining Fermi surface is implied to induce the reported magnetic ordering, and yields the insulating bulk state at higher Mn substitution, where all bands are gapped and totally incoherent. The availability of orbital-selective tuning of the pseudogap by a small impurity will prompt further theoretical studies of Hund's metals, which were recognized only recently in condensed matter physics.

This work was partly supported by the bilateral collaboration program between RFBR (Russia; No. 15-52-50017) and JSPS (Japan) and also by KAKENHI Grants No. 17H06138 and No. 18H03683. K.S. was financially supported by a Grant-in-Aid for JSPS Fellows (No. 16J03874). The study has also been supported by the Russian Science Foundation (Grant No. 17-12-01047) and RFBR (Grant No. 17-08-00955) for growing the single crystals and characterizing the samples. I.V.S. acknowledges financial support from the Russian Science Foundation (Grant No. 18-12-00169) for band structure calculations and the Ministry of Education and Science of the Russian Federation within governmental program Megagrants (State Task No. 3.9003.2017/9.10) for charge density calculations. This work has been partly performed in the framework of the nanoscience foundry and fine analysis (NFFA-MIUR Italy, Progetti Internazionali) facility. E.V.C. acknowledges financial support from the Saint Petersburg State University Project No. 15.61.202.2015 and the Spanish Ministry of Science and Innovation Grant No. FIS2016-75862-P.

Using high-resolution spin-resolved photoemission spectroscopy, we observed a thermal spin depolarization to which all spin-polarized electrons contribute. Furthermore we observed a distinct minority spin state near the Fermi level and a corresponding depolarization that seldom contributes to demagnetization. The origin of this depolarization has been identified as the many-body effect characteristics of half-metallic ferromagnets. Our investigation opens an experimental field of itinerant ferromagnetic physics focusing on phenomena with sub-meV energy scale., 19 pages, 10 figures

The spin texture of the spin-split surface states on Bi(111) has been comprehensively investigated by high energy and angular resolution spin- and angle-resolved photoelectron spectroscopy. A large out-of-plane spin component that alternately changes its sign is clearly observed. There is no evidence for peculiar polarization oscillation of the in-plane spin component, which was suggested to be due to breaking of the time-reversal symmetry in a previous report [A. Takayama et al., Phys. Rev. Lett. 106, 166401 (2011)]. The observed band structure and spin polarization are well reproduced by the $kp$ model Hamiltonian considering the ${C}_{3v}$ crystal symmetry, and the in-plane polarization variation at the different $k$ points can be understood by the photoemission final-state effect.

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

Spin-resolved band structures of $L$-gap surface states on Ag(111) and Cu(111) are investigated by spin- and angle-resolved photoelectron spectroscopy (SARPES) with a vacuum-ultraviolet laser. The observed spin textures of the Ag(111) and Cu(111) surface states agree with that expected by the conventional Rashba effect. The Rashba parameter of the Ag(111) surface state is estimated quantitatively and is $80%$ of that of Cu(111). The surface-state wave function is found to be predominantly of even mirror symmetry with negligible odd contribution by SARPES using a linearly polarized light. The results are consistent with our theoretical calculations for the orbital-resolved surface state.

Spin states of photoelectrons excited from spin-polarized surface states of Bi(111) surfaces are theoretically studied. The electronic states with a mirror symmetry are focused on in particular. We present a method for calculating spin expectation values of photoelectrons using results of density-functional methods in the plane-wave basis. We show that the free-electron approximation for final states is not sufficient for explaining an experimental result obtained in spin- and angle-resolved photoelectron spectroscopy. We point out two effects of the time-reversal symmetry in photoelectron emission. One is that the out-of-plane component of spin orientation is reversed to that of the time-reversed state. This property may be used for distinguishing the orientation of samples by shedding light with polarizations that break the mirror symmetry. Another is the asymmetry in photoemission intensity between an initial state and its time-reversed state due to the breaking of the time-reversal symmetry intrinsic in the photoemission process.

The Dirac-cone surface states of topological insulators are characterized by a chiral spin texture in k-space with the electron spin locked to its parallel momentum. Mid-infrared pump pulses can induce spin-polarized photocurrents in such a topological surface state by optical transitions between the occupied and unoccupied part of the Dirac cone. We monitor the ultrafast dynamics of the corresponding asymmetric electron population in momentum space directly by time- and angle-resolved two-photon photoemission (2PPE). The elastic scattering times of 2.5 ps deduced for Sb2Te3 corresponds to a mean-fee path of 0.75 μm in real space.

We present energy-momentum mapping of surface Dirac photocurrent in the topological insulator Sb$_2$Te$_3$ by means of time- and angle-resolved two-photon photoemission spectroscopy combined with polarization-variable mid-infrared pulse laser. It is demonstrated that the direct optical transition from the occupied to the unoccupied part of the surface Dirac-cone permits the linear and circular photogalvanic effect which thereby enables us to coherently control the surface electric-current by laser polarization. Moreover, the surface current mapping directly visualizes ultrafast current dynamics in the Dirac cone in the time domain. We unravel the ultrafast intraband relaxation dynamics of the inelastic scattering and momentum scattering separately. Our observations pave the pathway for coherent optical control over surface Dirac electrons in topological insulators.

We use spin- and angle-resolved photoemission spectroscopy (SARPES) combined with polarization-variable laser and investigate the spin-orbit coupling effect under interband hybridization of Rashba spin-split states for the surface alloys Bi/Ag(111) and Bi/Cu(111). In addition to the conventional band mapping of photoemission for Rashba spin-splitting, the different orbital and spin parts of the surface wavefucntion are directly imaged into energy-momentum space. It is unambiguously revealed that the interband spin-orbit coupling modifies the spin and orbital character of the Rashba surface states leading to the enriched spin-orbital entanglement and the pronounced momentum dependence of the spin-polarization. The hybridization thus strongly deviates the spin and orbital characters from the standard Rashba model. The complex spin texture under interband spin-orbit hybridyzation proposed by first-principles calculation is experimentally unraveled by SARPES with a combination of p- and s-polarized light., 6 pages, 4 figures

We investigate the surface electronic structures of polar 1T'-MoTe2, the Weyl semimetal candidate realized through the nonpolar-polar structural phase transition, by utilizing the laser angle-resolved photoemission spectroscopy (ARPES) combined with first-principles calculations. Two kinds of domains with different surface band dispersions are observed from a single-crystalline sample. The spin-resolved measurements further reveal that the spin polarizations of the surface and the bulk-derived states show the different domain-dependences, indicating the opposite bulk polarity. For both domains, some segment-like band features resembling the Fermi arcs are clearly observed. The patterns of the arcs present the marked contrast between the two domains, respectively agreeing well with the slab calculation of (0 0 1) and (0 0 -1) surfaces. The present result strongly suggests that the Fermi arc connects the identical pair of Weyl nodes on one side of the polar crystal surface, whereas it connects between the different pairs of Weyl nodes on the other side., 13 pages, 4 figures

Interference of spin-up and spin-down eigenstates depicts spin rotation of electrons, which is a fundamental concept of quantum mechanics and presents technological challenges for the electrical spin manipulation. Here, we visualize this coherent spin physics through laser spin- and angle-resolved photoemission spectroscopy on a spin-orbital entangled surface state of a topological insulator. It is revealed that the linearly polarized laser can simultaneously excite spin-up and spin-down states, and these quantum-spin bases are coherently superposed in photoelectron states. The superposition and the resulting spin rotation is manipulated by the direction of the laser field. Moreover, the full observation of the spin rotation displays the phase of the quantum states. This presents a new facet of laser-photoemission technique for investigation of quantum-spin physics, opening new possibilities in the field of quantum spintronic applications.

Photoemission established KHgSb as a nonsymmorphic topological insulator, which hosts hourglass-shaped surface states., Topological insulators (TIs) host novel states of quantum matter characterized by nontrivial conducting boundary states connecting valence and conduction bulk bands. All TIs discovered experimentally so far rely on either time-reversal or mirror crystal symmorphic symmetry to protect massless Dirac-like boundary states. Several materials were recently proposed to be TIs with nonsymmorphic symmetry, where a glide mirror protects exotic surface fermions with hourglass-shaped dispersion. However, an experimental confirmation of this new fermion is missing. Using angle-resolved photoemission spectroscopy, we provide experimental evidence of hourglass fermions on the (010) surface of crystalline KHgSb, whereas the (001) surface has no boundary state, in agreement with first-principles calculations. Our study will stimulate further research activities of topological properties of nonsymmorphic materials.

The measured electronic structure of Nd${}_{2}$Ir${}_{2}$O${}_{7}$ through its metal-insulator transition indicates an unusual Slater to Mott crossover with reducing temperature. This constrains theoretical models which suggest this material has topologically protected magnetic states.

We combine tunable midinfrared (mid-IR) pump pulses with time- and angle-resolved two-photon photoemission to study ultrafast photoexcitation of the topological surface state (TSS) of Sb_{2}Te_{3}. It is revealed that mid-IR pulses permit a direct excitation from the occupied to the unoccupied part of the TSS across the Dirac point. The novel optical coupling induces asymmetric transient populations of the TSS at ±k_{∥}, which reflects a macroscopic photoexcited electric surface current. By observing the decay of the asymmetric population, we directly investigate the dynamics of the long-lived photocurrent in the time domain. Our discovery promises important advantages of photoexcitation by mid-IR pulses for spintronic applications.

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 describe a spin- and angle-resolved photoelectron spectroscopy (SARPES) apparatus with a vacuum-ultraviolet (VUV) laser ($h\nu$= 6.994 eV) developed at the Laser and Synchrotron Research Center at the Institute for Solid State Physics, The University of Tokyo. The spectrometer consists of a hemispherical photoelectron analyzer equipped with an electron deflector function and twin very-low-energy-electron-diffraction-type spin detectors, which allows us to analyze the spin vector of a photoelectron three-dimensionally with both high energy and angular resolutions. The combination of the high-performance spectrometer and the high-photon-flux VUV laser can achieve an energy resolution of 1.7 meV for SARPES. We demonstrate that the present laser-SARPES machine realizes a quick SARPES on the spin-split band structure of a Bi(111) film even with 7 meV energy and 0.7$^\circ$ angular resolutions along the entrance-slit direction. This laser-SARPES machine is applicable to the investigation of spin-dependent electronic states on an energy scale of a few meV., Comment: 15 pages, 5 figures

A Weyl semimetal is a new state of matter that host Weyl fermions as quasiparticle excitations. The Weyl fermions at zero energy correspond to points of bulk band degeneracy, Weyl nodes, which are separated in momentum space and are connected only through the crystal's boundary by an exotic Fermi arc surface state. We experimentally measure the spin polarization of the Fermi arcs in the first experimentally discovered Weyl semimetal TaAs. Our spin data, for the first time, reveal that the Fermi arcs' spin polarization magnitude is as large as 80% and possesses a spin texture that is completely in-plane. Moreover, we demonstrate that the chirality of the Weyl nodes in TaAs cannot be inferred by the spin texture of the Fermi arcs. The observed non-degenerate property of the Fermi arcs is important for the establishment of its exact topological nature, which reveal that spins on the arc form a novel type of 2D matter. Additionally, the nearly full spin polarization we observed (~80%) may be useful in spintronic applications., 4 figures, 15 pages