Renormalizing the high-harmonic interference via double-slit and grating.

A method to utilize high-harmonic interference in Young's double-slit followed by a grating holds promise for precisely measuring the refractive-index spectrum in the extreme ultraviolet (EUV) region. The measurement is currently bottlenecked by the time it takes to fit the Fresnel interference patterns. The conventional fitting procedure, involving multiple numerical integrals for evaluating the EUV propagation through the slit and grating, takes ≳30min on a standard laptop computer, while the data acquisition time is ∼200s. Here, we apply an analytic Gaussian integral and bypass one of the numerical integrals associated with the grating. The analysis reduces to evaluating a renormalized EUV propagation in a simple double-slit interferometer, and the estimated fitting time on a laptop becomes as short as 112 s. Our study enables real-time analysis during measurements, facilitating mass optical-data collection of EUV lithography materials.

200-Hz longitudinal-mode linewidth found in a free-running mode-locked Yb:fiber laser.

We surveyed the longitudinal-mode linewidth of five homemade mode-locked Yb:fiber lasers by taking the beat note with a Hz-level narrow-linewidth CW laser. We systematically varied the resolution bandwidth of the spectrum analyzer and found that the linewidth can be as narrow as 200 Hz, which surpassed the records for free-running mode-locked lasers in the literature to our best knowledge. Based on the survey, we propose that making the cavity long and simple is a good working hypothesis for narrowing the linewidth and provide practical techniques to reduce the environmental fluctuations.

Effect of physisorption of inert organic molecules on Au(111) surface electronic states.

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.

Gigantic surface lifetime of an intrinsic topological insulator.

The interaction between light and novel two-dimensional electronic states holds promise to realize new fundamental physics and optical devices. Here, we use pump-probe photoemission spectroscopy to study the optically excited Dirac surface states in the bulk-insulating topological insulator Bi_{2}Te_{2}Se and reveal optical properties that are in sharp contrast to those of bulk-metallic topological insulators. We observe a gigantic optical lifetime exceeding 4 µs (1 µs=10^{-6} s) for the surface states in Bi_{2}Te_{2}Se, whereas the lifetime in most topological insulators, such as Bi_{2}Se_{3}, has been limited to a few picoseconds (1 ps=10^{-12} s). Moreover, we discover a surface photovoltage, a shift of the chemical potential of the Dirac surface states, as large as 100 mV. Our results demonstrate a rare platform to study charge excitation and relaxation in energy and momentum space in a two-dimensional system.

Robust protection from backscattering in the topological insulator Bi1.5Sb0.5Te1.7Se1.3.

Electron scattering in the topological surface state (TSS) of the topological insulator Bi1.5Sb0.5Te1.7Se1.3 was studied using quasiparticle interference observed by scanning tunneling microscopy. It was found that not only the 180° backscattering but also a wide range of backscattering angles of 100°-180° are effectively prohibited in the TSS. This conclusion was obtained by comparing the observed scattering vectors with the diameters of the constant-energy contours of the TSS, which were measured for both occupied and unoccupied states using time- and angle-resolved photoemission spectroscopy. The robust protection from backscattering in the TSS is good news for applications, but it poses a challenge to the theoretical understanding of the transport in the TSS.

A new category of "Aha!" driven by touch: A grip sensation into the directional seam on a baseball.

We report an "Aha!" experience which differs from conventional Aha's studied over a century in psychological science. The Aha we introduce is driven by touch instead of the visual and verbal modalities widely studied to date. It can occur when gripping a baseball, with a simple input that the red seam on the ball has a direction. Aided by a symmetry analysis and subsequent survey over literature, we show how our mental and physical representation of a baseball can change suddenly by the seam direction and unravel the factors that make the tactile sense into a joyful-and-insightful sensation. Our study sets a new category of Aha driven by touch, opens a new path to investigate the role of touch in our cognition process, reveals the seam direction as a new degree of freedom in baseball aerodynamics and pitching mechanics, and deepens the insights into throwing a baseball from our fingertips.

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.

Topologically Nontrivial Phase-Change Compound GeSb2Te4.

Chalcogenide phase-change materials show strikingly contrasting optical and electrical properties, which has led to their extensive implementation in various memory devices. By performing spin-, time-, and angle-resolved photoemission spectroscopy combined with the first-principles calculation, we report the experimental results that the crystalline phase of GeSb2Te4 is topologically nontrivial in the vicinity of the Dirac semimetal phase. The resulting linearly dispersive bulk Dirac-like bands that cross the Fermi level and are thus responsible for conductivity in the stable crystalline phase of GeSb2Te4 can be viewed as a 3D analogue of graphene. Our finding provides us with the possibility of realizing inertia-free Dirac currents in phase-change materials.

Prolonged photo-carriers generated in a massive-and-anisotropic Dirac material.

Transient electron-hole pairs generated in semiconductors can exhibit unconventional excitonic condensation. Anisotropy in the carrier mass is considered as the key to elongate the life time of the pairs, and hence to stabilize the condensation. Here we employ time- and angle-resolved photoemission spectroscopy to explore the dynamics of photo-generated carriers in black phosphorus. The electronic structure above the Fermi level has been successfully observed, and a massive-and-anisotropic Dirac-type dispersions are confirmed; more importantly, we directly observe that the photo-carriers generated across the direct band gap have the life time exceeding 400 ps. Our finding confirms that black phosphorus is a suitable platform for excitonic condensations, and also open an avenue for future applications in broadband mid-infrared BP-based optoelectronic devices.

Spin-dependent quantum interference in photoemission process from spin-orbit coupled states.

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.

Femtosecond to picosecond transient effects in WSe 2 observed by pump-probe angle-resolved photoemission spectroscopy.

Time-dependent responses of materials to an ultrashort optical pulse carry valuable information about the electronic and lattice dynamics; this research area has been widely studied on novel two-dimensional materials such as graphene, transition metal dichalcogenides (TMDs) and topological insulators (TIs). We report herein a time-resolved and angle-resolved photoemission spectroscopy (TRARPES) study of WSe2, a layered semiconductor of interest for valley electronics. The results for below-gap optical pumping reveal energy-gain and -loss Floquet replica valence bands that appear instantaneously in concert with the pump pulse. Energy shift, broadening, and complex intensity variation and oscillation at twice the phonon frequency for the valence bands are observed at time scales ranging from the femtosecond to the picosecond and beyond. The underlying physics is rich, including ponderomotive interaction, dressing of the electronic states, creation of coherent phonon pairs, and diffusion of charge carriers - effects operating at vastly different time domains.

Signatures of a time-reversal symmetric Weyl semimetal with only four Weyl points.

Through intense research on Weyl semimetals during the past few years, we have come to appreciate that typical Weyl semimetals host many Weyl points. Nonetheless, the minimum nonzero number of Weyl points allowed in a time-reversal invariant Weyl semimetal is four. Realizing such a system is of fundamental interest and may simplify transport experiments. Recently, it was predicted that TaIrTe4 realizes a minimal Weyl semimetal. However, the Weyl points and Fermi arcs live entirely above the Fermi level, making them inaccessible to conventional angle-resolved photoemission spectroscopy (ARPES). Here, we use pump-probe ARPES to directly access the band structure above the Fermi level in TaIrTe4. We observe signatures of Weyl points and topological Fermi arcs. Combined with ab initio calculation, our results show that TaIrTe4 is a Weyl semimetal with the minimum number of four Weyl points. Our work provides a simpler platform for accessing exotic transport phenomena arising in Weyl semimetals.Weyl semimetals are interesting because they are characterized by topological invariants, but specific examples discovered to date tend to have complicated band structures with many Weyl points. Here, the authors show that TaIrTe4 has only four Weyl points, the minimal number required by time-reversal symmetry.

High-resolution three-dimensional spin- and angle-resolved photoelectron spectrometer using vacuum ultraviolet laser light.

We describe a spin- and angle-resolved photoelectron spectroscopy (SARPES) apparatus with a vacuum-ultraviolet (VUV) laser (hν = 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(∘) 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.

Electronic structure and relaxation dynamics in a superconducting topological material.

Topological superconductors host new states of quantum matter which show a pairing gap in the bulk and gapless surface states providing a platform to realize Majorana fermions. Recently, alkaline-earth metal Sr intercalated Bi2Se3 has been reported to show superconductivity with a Tc ~ 3 K and a large shielding fraction. Here we report systematic normal state electronic structure studies of Sr0.06Bi2Se3 (Tc ~ 2.5 K) by performing photoemission spectroscopy. Using angle-resolved photoemission spectroscopy (ARPES), we observe a quantum well confined two-dimensional (2D) state coexisting with a topological surface state in Sr0.06Bi2Se3. Furthermore, our time-resolved ARPES reveals the relaxation dynamics showing different decay mechanism between the excited topological surface states and the two-dimensional states. Our experimental observation is understood by considering the intra-band scattering for topological surface states and an additional electron phonon scattering for the 2D states, which is responsible for the superconductivity. Our first-principles calculations agree with the more effective scattering and a shorter lifetime of the 2D states. Our results will be helpful in understanding low temperature superconducting states of these topological materials.

Discovery of a new type of topological Weyl fermion semimetal state in MoxW1-xTe2.

The recent discovery of a Weyl semimetal in TaAs offers the first Weyl fermion observed in nature and dramatically broadens the classification of topological phases. However, in TaAs it has proven challenging to study the rich transport phenomena arising from emergent Weyl fermions. The series MoxW1-xTe2 are inversion-breaking, layered, tunable semimetals already under study as a promising platform for new electronics and recently proposed to host Type II, or strongly Lorentz-violating, Weyl fermions. Here we report the discovery of a Weyl semimetal in MoxW1-xTe2 at x=25%. We use pump-probe angle-resolved photoemission spectroscopy (pump-probe ARPES) to directly observe a topological Fermi arc above the Fermi level, demonstrating a Weyl semimetal. The excellent agreement with calculation suggests that MoxW1-xTe2 is a Type II Weyl semimetal. We also find that certain Weyl points are at the Fermi level, making MoxW1-xTe2 a promising platform for transport and optics experiments on Weyl semimetals.

Ultrafast electron dynamics at the Dirac node of the topological insulator Sb2Te3.

Topological insulators (TIs) are a new quantum state of matter. Their surfaces and interfaces act as a topological boundary to generate massless Dirac fermions with spin-helical textures. Investigation of fermion dynamics near the Dirac point (DP) is crucial for the future development of spintronic devices incorporating topological insulators. However, research so far has been unsatisfactory because of a substantial overlap with the bulk valence band and a lack of a completely unoccupied DP. Here, we explore the surface Dirac fermion dynamics in the TI Sb2Te3 by time- and angle-resolved photoemission spectroscopy (TrARPES). Sb2Te3 has an in-gap DP located completely above the Fermi energy (EF). The excited electrons in the upper Dirac cone stay longer than those below the DP to form an inverted population. This was attributed to a reduced density of states (DOS) near the DP.

Coherent and Incoherent Excitations of Electron-Doped SrTiO3.

Resonant photoemission at the Ti 2p and O 1s edges on a Nb-doped SrTiO(3) thin film revealed that the coherent state (CS) at the Fermi level (E(F)) had a mainly Ti 3d character whereas the incoherent in-gap state (IGS) positioned approximately 1.5 eV below E(F) had a mixed character of Ti 3d and O 2p states. This indicates that the IGS is formed by a spectral-weight transfer from the CS and subsequent spectral-weight redistribution through d-p hybridization. We discuss the evolution of the excitation spectrum with 3d band filling and rationalize the IGS through a mechanism similar to that proposed by Haldane and Anderson.