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.

Quasi-Periodic Growth of One-Dimensional Copper Boride on Cu(110).

An unexplored material of copper boride has been realized recently in two-dimensional form at a (111) surface of the fcc copper crystal. Here, one-dimensional (1-D) boron growth was observed on the Cu(110) surface, as probed by atomically resolved scanning probe microscopy. The 1-D copper boride was composed of quasi-periodic atomic chains periodically aligned parallel to each other, as confirmed by Fourier transform analysis. The 1-D growth unexpectedly proceeded across surface steps in a self-assembled manner and extended over several 100 nm. The long-range formation of a 1-D quasi-periodic structure on a surface has been theoretically modeled as a 1-D quasi-crystal and the predicted conditions matched the structural parameters obtained by the experimental work here. The quasi-periodic 1-D copper boride system enabled a way to examine 1-D quasi-crystallinity on an actual material.

Width-dependent band gap of arm-chair graphene nanoribbons formed on vicinal SiC substrates by MBE.

Formation and electronic states of graphene nanoribbons with arm-chair edges (AGNR) are studied on the SiC(0001) vicinal surfaces toward the [11-00] direction. The surface step and terrace structures of both 4H and 6H-SiC substrates are used as the growth templates of one-dimensional arrays of AGNRs, which are prepared using the carbon molecular beam epitaxy followed by hydrogen intercalation. A band gap is observed above theπ-band maximum by angle-resolved photoelectron spectroscopy (ARPES) for the both samples. The average widths of the AGNRs are 6 and 10 nm, and the estimated average band gaps are 0.40 and 0.28 eV for the 4H- and 6H- substrates, respectively. A simple and phenomenological inverse relation between the energy gap and AGNR width works in the analyses of the ARPES data.

Revealing the Hidden Spin-Polarized Bands in a Superconducting Tl Bilayer Crystal.

The interplay of spin-orbit coupling and crystal symmetry can generate spin-polarized bands in materials only a few atomic layers thick, potentially leading to unprecedented physical properties. In the case of bilayer materials with global inversion symmetry, locally broken inversion symmetry can generate degenerate spin-polarized bands, in which the spins in each layer are oppositely polarized. Here, we demonstrate that the hidden spins in a Tl bilayer crystal are revealed by growing it on Ag(111) of sizable lattice mismatch, together with the appearance of a remarkable phenomenon unique to centrosymmetric hidden-spin bilayer crystals: a novel band splitting in both spin and space. The key to success in observing this novel splitting is that the interaction at the interface has just the right strength: it does not destroy the original wave functions of the Tl bilayer but is strong enough to induce an energy separation.

Accelerated Synthesis of Borophane (HB) Sheets through HCl-Assisted Ion-Exchange Reaction with YCrB4.

We present an enhanced method for synthesizing sheets of borophane. Despite the challenges associated with low efficiency, we discovered that incorporating hydrochloric acid into the ion-exchange reaction significantly improved the production yield from 20% to over 50%. After a thorough examination of the reaction, we gained insight into the underlying mechanisms and found that the use of hydrochloric acid provides two key benefits: accelerated production of borophene and isolation of high-purity products. This method has the potential to pave the way for the production of novel topological 2D materials with potential industrial applications.

Two-Dimensional Superconductivity of Ca-Intercalated Graphene on SiC: Vital Role of the Interface between Monolayer Graphene and the Substrate.

Ca-intercalation has enabled superconductivity in graphene on SiC. However, the atomic and electronic structures that are critical for superconductivity are still under discussion. We find an essential role of the interface between monolayer graphene and the SiC substrate for superconductivity. In the Ca-intercalation process, at the interface a carbon layer terminating SiC changes to graphene by Ca-termination of SiC (monolayer graphene becomes a bilayer), inducing more electrons than a free-standing model. Then, Ca is intercalated in between the graphene layers, which shows superconductivity with the updated critical temperature (TC) of up to 5.7 K. In addition, the relation between TC and the normal-state conductivity is unusual, "dome-shaped". These findings are beyond the simple C6CaC6 model in which s-wave BCS superconductivity is theoretically predicted. This work proposes a general picture of the intercalation-induced superconductivity in graphene on SiC and indicates the potential for superconductivity induced by other intercalants.

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.

Subatomic Distortion of Surface Monolayer Lattice Visualized by Moiré Pattern.

Mapping of the local lattice distortion is required to understand the details of the chemical and physical properties of thin films. However, the resolution by the direct microscopic methods was insufficient to detect the local distortion. Here, we have demonstrated that the local distortion of a monatomic film on a substrate is estimated with high resolution using the moiré pattern of the topographic scanning tunneling microscopy image. The analysis focused on the apparently low centers of the moiré pattern of the hexagonal iron nitride monolayer on the Cu(111) substrate. The local distortion was visualized by estimating the displacement of the experimentally detected center position from the ideal position that is extracted from the adjacent center positions. The map of the local distortion revealed that the subsurface impurities are preferentially located on the largely distorted areas. This approach is widely applicable to other thin films on the substrates.

Atomic-layer Rashba-type superconductor protected by dynamic spin-momentum locking.

Spin-momentum locking is essential to the spin-split Fermi surfaces of inversion-symmetry broken materials, which are caused by either Rashba-type or Zeeman-type spin-orbit coupling (SOC). While the effect of Zeeman-type SOC on superconductivity has experimentally been shown recently, that of Rashba-type SOC remains elusive. Here we report on convincing evidence for the critical role of the spin-momentum locking on crystalline atomic-layer superconductors on surfaces, for which the presence of the Rashba-type SOC is demonstrated. In-situ electron transport measurements reveal that in-plane upper critical magnetic field is anomalously enhanced, reaching approximately three times the Pauli limit at T = 0. Our quantitative analysis clarifies that dynamic spin-momentum locking, a mechanism where spin is forced to flip at every elastic electron scattering, suppresses the Cooper pair-breaking parameter by orders of magnitude and thereby protects superconductivity. The present result provides a new insight into how superconductivity can survive the detrimental effects of strong magnetic fields and exchange interactions.

Orbital Angular Momentum Induced Spin Polarization of 2D Metallic Bands.

The electrons in 2D systems with broken inversion symmetry are spin-polarized due to spin-orbit coupling and provide perfect targets for observing exotic spin-related fundamental phenomena. We observe a Fermi surface with a novel spin texture in the 2D metallic system formed by indium double layers on Si(111) and find that the primary origin of the spin-polarized electronic states of this system is the orbital angular momentum and not the so-called Rashba effect. The present results deepen the understanding of the physics arising from spin-orbit coupling in atomic-layered materials with consequences for spintronic devices and the physics of the superconducting state.

Ultrafast Unbalanced Electron Distributions in Quasicrystalline 30° Twisted Bilayer Graphene.

Ultrafast carrier dynamics in a graphene system are very important in terms of optoelectronic devices. Recently, a twisted bilayer graphene has been discovered that possesses interesting electronic properties owing to strong modifications in interlayer couplings. Thus, a better understanding of ultrafast carrier dynamics in a twisted bilayer graphene is highly desired. Here, we reveal the unbalanced electron distributions in a quasicrystalline 30° twisted bilayer graphene (QCTBG), using time- and angle-resolved photoemission spectroscopy on the femtosecond time scale. We distinguish time-dependent electronic behavior between the upper- and lower-layer Dirac cones and gain insight into the dynamical properties of replica bands, which show characteristic signatures due to Umklapp scatterings. The experimental results are reproduced by solving a set of rate equations among the graphene layers and substrate. We find that the substrate buffer layer plays a key role in initial carrier injections to the upper and lower layers. Our results demonstrate that QCTBG can be a promising element for future devices.

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.

Electronic and magnetic properties of the Fe2N monolayer film tuned by substrate symmetry.

The robust bonding between Fe and N atoms has the potential to fabricate a ferromagnetic Fe2N monolayer of a square lattice independently of the symmetry of the substrate. The electronic and magnetic properties tuned by the symmetry of the substrates are investigated by comparing the results of scanning tunnel microscopy and x-ray absorption spectroscopy/magnetic circular dichroism of the square Fe2N monolayer on the Cu(1 1 1) substrate with that on the Cu(0 0 1) substrate. A periodic electronic modulation of the Fe2N monolayer on the Cu(1 1 1) substrate is induced by the stripe superlattice due to the difference of the lattice symmetry between the Fe2N monolayer and the Cu(1 1 1) substrate. The electronic and magnetic properties of the monolayer are largely affected by the hybridization with the Cu substrate and the Fe magnetic moment is much reduced compared to the monolayer on the Cu(0 0 1) substrate.

Study on Formation Process and Models of Linear Fe Cluster Structure on a Si(111)-7 × 7-CH3OH Surface.

STM results showed that Fe atoms were deposited on a Si(111)-7 × 7 reconstructed surface, which was saturated with CH3OH molecules. Fe atomic linear structure was composed of stable clusters and in-situ observed by the scanning tunneling microscopy (STM). The aim to improve its application of magnetic memory material, both formation process and models, has been explored in this paper. By combining surface images and mass spectrometer data, an intermediate layer model was established. In terms of thermal stability, the most favorable adsorption sites of CH3OH were further explored. After that, Fe atoms were deposited on the Si(111)-7 × 7-CH3OH surface, forming a linear cluster structure. On the one hand, a new Fe cluster model was put forward in this paper, which was established with height measurement and 3D surface display technology. This model is also affected by the evaporation temperature, which can be consistent with the atomic stacking pattern of face centered cubic structures. On the other hand, the slight height change suggested the stability of linear structures. Even in the condition of thin air introduction, Fe cluster showed a good performance, which suggested the possibility of magnetic memory application in the future. These investigations are believed to have, to a certain extent, increased the probability of forming Fe linear clusters on the surface of silicon substrate, especially according to the models and surface technology we adjusted.

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.

Surface electronic states of Au-induced nanowires on Ge(0 0 1).

The electronic states of Au-induced atomic nanowires on Ge(0 0 1) (Au/Ge(0 0 1) NWs) have been studied by angle-resolved photoelectron spectroscopy with linearly polarized light. We have found three electron pockets around the [Formula: see text] line, where the Fermi surfaces are closed in a surface Brillouin zone (SBZ). The results indicate 2D Fermi surfaces of Au/Ge(0 0 1) NWs whereas the atomic structure is 1D. On the basis of the polarization-dependent spectra, the relation between SBZ and the direction of the atomic NW, and the symmetry of the surface state are clarified. These are very useful for further studies on the atomic structure of NWs.

Discovery of 2D Anisotropic Dirac Cones.

2D anisotropic Dirac cones are observed in χ3 borophene, a monolayer boron sheet, using high-resolution angle-resolved photoemission spectroscopy. The Dirac cones are centered at the X and X' points. The data also reveal that the hybridization between borophene and Ag(111) is very weak, which explains the preservation of the Dirac cones. As χ3 borophene has been predicated to be a superconductor, the results may stimulate further research interest in the novel physics of borophene, such as the interplay between Cooper pairs and the massless Dirac fermions.

Evidence for in-gap surface states on the single phase SmB6(001) surface.

Structural and electronic properties of the SmB6(001) single-crystal surface prepared by Ar+ ion sputtering and controlled annealing are investigated by scanning tunneling microscopy. In contrast to the cases of cleaved surfaces, we observe a single phase surface with a non-reconstructed p(1 × 1) lattice on the entire surface at an optimized annealing temperature. The surface is identified as Sm-terminated on the basis of spectroscopic measurements. On a structurally uniform surface, the emergence of the in-gap state, a robust surface state against structural variation, is further confirmed inside a Kondo hybridization gap at 4.4 K by temperature and atomically-resolved spatial dependences of the differential conductance spectrum near the Fermi energy.

Modulation of Electron-Phonon Coupling in One-Dimensionally Nanorippled Graphene on a Macrofacet of 6H-SiC.

Local electron-phonon coupling of a one-dimensionally nanorippled graphene is studied on a SiC(0001) vicinal substrate. We have characterized local atomic and electronic structures of a periodically nanorippled graphene (3.4 nm period) prepared on a macrofacet of the 6H-SiC crystal using scanning tunneling microscopy/spectroscopy (STM/STS) and angle-resolved photoelectron spectroscopy (ARPES). The rippled graphene on the macrofacets distributes homogeneously over the 6H-SiC substrate in a millimeter scale, and thus replica bands are detected by the macroscopic ARPES. The STM/STS results indicate the strength of electron-phonon coupling to the out-of-plane phonon at the K̅ points of graphene is periodically modified in accordance with the ripple structure. We propose an interface carbon nanostructure with graphene nanoribbons between the surface rippled graphene and the substrate SiC that periodically modifies the electron-phonon coupling in the surface graphene.