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We describe a setup of time-, spin-, and angle-resolved photoemission spectroscopy (tr-SARPES) employing a 10.7-eV ($\lambda$=115.6 nm) pulse laser at 1-MHz repetition rate as a probe photon source. This equipment effectively combines 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 (VLEED) 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 10$^{13}$ 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 a low efficiency of spin-resolved measurements, which gets even more severe for the pump-probed unoccupied states, and affords for investigating ultrafast electron and spin dynamics of modern quantum materials with energy and time resolutions of 25 meV and 360 fs, respectively., Comment: 11 pages, 7 figures

Layers of twisted bilayer graphene exhibit varieties of exotic quantum phenomena1-5. Today, the twist angle {\Theta} has become an important degree of freedom for exploring novel states of matters, i.e. two-dimensional superconductivity ( {\Theta} = 1.1{\deg})6, 7 and a two-dimensional quasicrystal ({\Theta} = 30{\deg})8, 9. We report herein experimental observation on the photo-induced ultrafast dynamics of Dirac fermions in the quasicrystalline 30{\deg} twisted bilayer graphene (QCTBG). We discover that hot carriers are asymmetrically distributed between the two graphene layers, followed by the opposing femtosecond relaxations, by using time- and angle-resolved photoemission spectroscopy. The key mechanism involves the differing carrier transport between layers and the transient doping from the substrate interface. The ultrafast dynamics scheme continues after the Umklapp scattering, which is induced by the incommensurate interlayer stacking of the quasi-crystallinity. The dynamics in the atomic layer opens the possibility of new applications and creates interdisciplinary links in the optoelectronics of van der Waals crystals.

The emergence of quantization at the nanoscale, the quantum size effect (QSE), allows flexible control of matter and is a rich source of advanced functionalities. A QSE-induced transition into an insulating phase in semimetallic nanofilms was predicted for bismuth a half-century ago and has regained new interest with regard to its surface states exhibiting nontrivial electronic topology. Here, we reveal an unexpected mechanism of the transition by high-resolution angle-resolved photoelectron spectroscopy combined with theoretical calculations. Anomalous evolution and degeneracy of quantized energy levels indicate that increased Coulomb repulsion from the surface states deforms a quantum confinement potential with decreasing thickness. The potential deformation drastically modulates spatial distributions of quantized wave functions, which leads to acceleration of the transition even beyond the original QSE picture. This discovery establishes a complete picture of the long-discussed problem in bismuth and highlights the new class of size effects dominating nanoscale transport in systems with metallic surface states., Comment: 22 pages, 10 figures (Supplementary Information included), accepted for publication in Science Advances

Electronic states on the Bi/InAs(110)-(2$\times$1) surface and its spin-polarized structure are revealed by angle-resolved photoelectron spectroscopy (ARPES), spin-resolved ARPES, and density-functional-theory calculation. The surface state showed quasi-one-dimensional (Q1D) dispersion and a nearly metallic character; the top of the hole-like surface band is just below the Fermi level. The size of the Rashba parameter ($\alpha_{\rm R}$) reached quite a large value ($\sim$5.5 eV\AA). The present result would provide a fertile playground for further studies of the exotic electronic phenomena in 1D or Q1D systems with the spin-split electronic states as well as for advanced spintronic devices., Comment: 8 pages (double column), 7 figures and 1 table

Alkali-metal adsorption on the surface of materials is widely used for in situ surface electron doping, particularly for observing unoccupied band structures by angle-resolved photoemission spectroscopy (ARPES). However, the effects of alkali-metal atoms on the resulting band structures have yet to be fully investigated, owing to difficulties in both experiments and calculations. Here, we combine ARPES measurements on cesium-adsorbed ultrathin bismuth films with first-principles calculations of the electronic charge densities and demonstrate a simple method to evaluate alkali-metal induced band deformation. We reveal that deformation of bismuth surface bands is directly correlated with vertical charge-density profiles at each electronic state of bismuth. In contrast, a change in the quantized bulk bands is well described by a conventional rigid-band-shift picture. We discuss these two aspects of the band deformation holistically, considering spatial distributions of the electronic states and cesium-bismuth hybridization, and provide a prescription for applying alkali-metal adsorption to a wide range of materials., Comment: 8 pages, 7 figures

One-dimensional (1D) electronic states were discovered on 1D surface atomic structure of Bi fabricated on semiconductor InSb(001) substrates by angle-resolved photoelectron spectroscopy (ARPES). The 1D state showed steep, Dirac-cone-like dispersion along the 1D atomic structure with a finite direct bandgap opening as large as 150 meV. Moreover, spin-resolved ARPES revealed the spin polarization of the 1D unoccupied states as well as that of the occupied states, the orientation of which inverted depending on the wave vector direction parallel to the 1D array on the surface. These results reveal that a spin-polarized quasi-1D carrier was realized on the surface of 1D Bi with highly efficient backscattering suppression, showing promise for use in future spintronic and energy-saving devices., Comment: 9 pages (4 figures for the main text, 7 for supplemental material). To be published in Physical Review Materials (Copyright is transferred to APS)

Growth, electronic and magnetic properties of $\gamma'$-Fe$_{4}$N atomic layers on Cu(001) are studied by scanning tunneling microscopy/spectroscopy and x-ray absorption spectroscopy/magnetic circular dichroism. A continuous film of ordered trilayer $\gamma'$-Fe$_{4}$N is obtained by Fe deposition under N$_{2}$ atmosphere onto monolayer Fe$_{2}$N/Cu(001), while the repetition of a bombardment with 0.5 keV N$^{+}$ ions during growth cycles results in imperfect bilayer $\gamma'$-Fe$_{4}$N. The increase in the sample thickness causes the change of the surface electronic structure, as well as the enhancement in the spin magnetic moment of Fe atoms reaching $\sim$ 1.4 $\mu_{\mathrm B}$/atom in the trilayer sample. The observed thickness-dependent properties of the system are well interpreted by layer-resolved density of states calculated using first principles, which demonstrates the strongly layer-dependent electronic states within each surface, subsurface, and interfacial plane of the $\gamma'$-Fe$_{4}$N atomic layers on Cu(001)., Comment: 9 pages, 7 figures, 2 tables

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., Comment: 6 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 accepts 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 unambiguously revealed that the linearly polarized laser can simultaneously excite spin-up and spin-down states and these quantum spin-basis are coherently superposed in photoelectron states. The superposition and the resulting spin rotation is arbitrary 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.

We show a new way to stabilize epitaxial structures against transforming bulk stable phases for Fe thin films on a vicinal Cu(001) surface. Atomically-resolved observations by scanning tunneling microscopy reveal that high-density Cu steps serve as strain relievers for keeping epitaxially-stabilized Fe fcc(001) lattice even at a transient thickness towards the bulk stable bcc(110) lattice. Spectroscopic measurements further clarify the intrinsic electronic properties of the fcc Fe thin film in real space, implying electronic differences between 6 and 7 monolayer thick films induced by the modification of the lattice constant in the topmost layers., Comment: 5 pages, 5 figures

Mixing of atoms at the interface was studied for Mn/Fe magnetic hetero-epitaxial layers on Cu(001) by scanning tunneling microscopy/spectroscopy. The formation of a surface alloy was observed when the Mn layer was thinner than 3 atomic layers. From the fourth layer, Fe segregation is suppressed, and a pure Mn surface appears. Accordingly, spectroscopic measurements revealed the electronic difference between the surface alloy and Mn layers. The surface electronic structure of the fourth Mn layer is slightly different from that of the fifth layers, which is attributed to the hybridization of the fourth layer with the underneath Fe-Mn alloy., Comment: 8 pages, 4 figures

The topology of pure Bi is controversial because of its very small ($\sim$10 meV) band gap. Here we perform high-resolution angle-resolved photoelectron spectroscopy measurements systematically on 14$-$202 bilayers Bi films. Using high-quality films, we succeed in observing quantized bulk bands with energy separations down to $\sim$10 meV. Detailed analyses on the phase shift of the confined wave functions precisely determine the surface and bulk electronic structures, which unambiguously show nontrivial topology. The present results not only prove the fundamental property of Bi but also introduce a capability of the quantum-confinement approach., Comment: 6 pages, 5 figures

The electronic states of Au-induced atomic nanowires on Ge(001) (Au/Ge(001) NWs) have been investigated by angle-resolved photoelectron spectroscopy with linearly polarized light. We have found three electron pockets around $\bar{J}\bar{K}$, where the Fermi surfaces are closed in a surface Brillouin zone, indicating that the surface states of Au/Ge(001) NWs are two-dimensional whereas the atomic structure is one-dimensional. The two-dimensional metallic states exhibit remarkable suppression of the photoelectron intensity near a Fermi energy. This suppression can be explained by the correlation and localization effects in disordered metals, which is a deviation from a Fermi-liquid model., Comment: 5 pages, 4 figures

We have studied initial growth of Sn atoms on Ge(001) surfaces at room temperature and 80 K by scanning tunneling microscopy. For Sn deposition onto the Ge(001) substrate at room temperature, the Sn atoms form two kinds of one-dimensional structures composed of ad-dimers with different alignment, in the <310> and the <110> directions, and epitaxial structures. For Sn deposition onto the substrate at 80 K, the population of the dimer chains aligning in the <310> direction increases. The diffusion barrier of the Sn adatom on the substrate kinetically determines the population of the dimer chain. We propose that the diffusion barrier height depends on surface strain induced by the adatom. The two kinds of dimer chains appearing on the Ge(001) and Si(001) surfaces with adatoms of the group-IV elements are systematically interpreted in terms of the surface stain., Comment: 12 figures