experimental-methods-for-spin-angle-resolved-photoemission

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 ...

University of Tokyo

Self-assembled MnN nanoislands have been prepared on Cu(001) substrate. The nanoislands show a square shape and a well-defined size. They are regularly arrayed with a periodicity of (3.5+/-0.1) nanometer and form a two-dimensional square superstructure. The MnN island superstructure is stabilized by a short-range mechanism. A structural model has been proposed to explain the self-assembly and the high quality of the superstructure.

Self-assembled MnN superstructure.

Atomic motion through excitation of extended surface electronic states on Ge(001) is studied using extraction of electrons by scanning tunneling microscopy and density functional theory. Single-electron excitation into the surface states nonlocally alters the tilting orientation of the surface Ge dimer, and the change rate depends on the excitation energy. Theoretical investigations identify the excited electronic states for the dimer motion, and clarify the strong coupling between the surface state electrons and a local vibrational mode of the dimer for changing the tilting orientation.

Local vibrational excitation through extended electronic states at a germanium surface.

Atomic and electronic structures of the Ge(111) (√3 × √3)R30°-Au surface with two metallic bands are studied by scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES). The bias-voltage-dependent periodic structure observed by STM is consistent with the electronic structure calculated for an optimized conjugate honeycomb chained trimer (CHCT) model. Electrons are selectively doped to the electron-like surface metallic band by excess Au atoms, which form triangle structures with the Au trimers of the CHCT model. The discrepancy for the bottom energy of the electron-like band between the ARPES results and those of the calculation is attributed to the doping. The triangle structure is mobile at room temperature, but stable at 80 K. Both Au and Ge atoms deposited at room temperature on the Ge(111) (√3 × √3)R30°-Au surface dope electrons to the electron-like surface metallic band. Moreover, the Au atoms increase the spin-orbit interaction at the surface, and thus make the splitting of the spin-polarized band due to the interaction larger than that before the deposition.

Selective doping in a surface band and atomic structures of the Ge(111) (√3 × √3)R30°-Au surface.

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. 

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

The Fe atoms were deposited on the Si(111)-7 × 7 surface, which has been saturated with the C2H5OH molecules. Then, the Fe clusters were formed on Si(111)-7 × 7-C2H5OH surface and in situ observed by the scanning tunneling microscopy (STM). The STM images showed that with the increase of Fe clusters, the size of clusters was about 5 nm and they self-assembled in straightly linked chain crossing the step to lower or upper terrace. X-ray photoelectron spectroscopy (XPS) was in situ carried out on the surface of Fe/Si(111)-7 × 7-C2H5OH samples before and after the introduction of thin air (4.5 × 10(-2) Langmuir) into the STM chamber. The XPS results showed that the Fe clusters are stable in the abovementioned thin air condition at room temperature. Based on the STM and XPS results, the driving force making one-dimensional straightly linked chain structure might be the magnetic force of the Fe clusters. The formation of straightly linked Fe clusters chains suggests the formation of single magnetic domain Fe clusters.

Formation of linearly linked Fe clusters on Si(111)-7 × 7-C2H5OH surface.

We report the thermally induced unconventional cracking of graphene to generate zigzag edges. This crystallography-selective cracking was observed for as-grown graphene films immediately following the cooling process subsequent to chemical vapor deposition (CVD) on Cu foil. Results from Raman spectroscopy show that the crack-derived edges have smoother zigzag edges than the chemically formed grain edges of CVD graphene. Using these cracks as nanogaps, we were also able to demonstrate the carrier tuning of graphene through the electric field effect. Statistical analysis of visual observations indicated that the crack formation results from uniaxial tension imparted by the Cu substrates together with the stress concentration at notches in the polycrystalline graphene films. On the basis of simulation results using a simplified thermal shrinkage model, we propose that the cooling-induced tension is derived from the transient lattice expansion of narrow Cu grains imparted by the thermal shrinkage of adjacent Cu grains. 

Selective Formation of Zigzag Edges in Graphene Cracks.

A Weyl semimetal is a new state of matter that hosts Weyl fermions as quasiparticle excitations. The Weyl fermions at zero energy correspond to points of bulk-band degeneracy, called 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 lies completely in the plane of the surface. 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 nondegenerate property of the Fermi arcs is important for establishing its exact topological nature, which reveals 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. 

Spin Polarization and Texture of the Fermi Arcs in the Weyl Fermion Semimetal TaAs.

Surface states of platinum-induced atomic nanowires on a germanium (0 0 1) surface, which shows a structural phase transition at 80 K, were studied by angle-resolved photoelectron spectroscopy (ARPES). We observed four one-dimensional metallic surface states, among which, two bands were reported in our previous study (Yaji et al 2013 Phys. Rev. B 87 241413). One of the newly-found two bands is a quasi-one-dimensional state and is split into two due to the Rashba effect. Photoelectron intensity from one of the spin-polarized branches is reduced at a boundary of the surface Brillouin zone below the phase transition temperature. The reduction of the photoelectron intensity in the low temperature phase is interpreted as the interference of photoelectrons, not as the Peierls instability. We also discuss the low energy properties of the metallic surface states and their spin splitting using high-resolution ARPES with a vacuum ultraviolet laser.

One-dimensional metallic surface states of Pt-induced atomic nanowires on Ge(0 0 1).

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.

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

Production of chemical fuels by direct solar energy conversion in a photoelectrochemical cell is of great practical interest for developing a sustainable energy system. Various nanoscale designs such as nanowires, nanotubes, heterostructures and nanocomposites have been explored to increase the energy conversion efficiency of photoelectrochemical water splitting. Here we demonstrate a self-organized nanocomposite material concept for enhancing the efficiency of photocarrier separation and electrochemical energy conversion. Mechanically robust photoelectrodes are formed by embedding self-assembled metal nanopillars in a semiconductor thin film, forming tubular Schottky junctions around each pillar. The photocarrier transport efficiency is strongly enhanced in the Schottky space charge regions while the pillars provide an efficient charge extraction path. Ir-doped SrTiO3 with embedded iridium metal nanopillars shows good operational stability in a water oxidation reaction and achieves over 80% utilization of photogenerated carriers under visible light in the 400- to 600-nm wavelength range. 

Photoelectrochemical water splitting enhanced by self-assembled metal nanopillars embedded in an oxide semiconductor photoelectrode.

The effects of Pb intercalation on the structural and electronic properties of epitaxial single-layer graphene grown on SiC(0001) substrate are investigated using scanning tunneling microscopy (STM), noncontact atomic force microscopy, Kelvin probe force microscopy (KPFM), X-ray photoelectron spectroscopy, and angle-resolved photoemission spectroscopy (ARPES) methods. The STM results show the formation of an ordered moiré superstructure pattern induced by Pb atom intercalation underneath the graphene layer. ARPES measurements reveal the presence of two additional linearly dispersing π-bands, providing evidence for the decoupling of the buffer layer from the underlying SiC substrate. Upon Pb intercalation, the Si 2p core level spectra show a signature for the existence of PbSi chemical bonds at the interface region, as manifested in a shift of 1.2 eV of the bulk SiC component toward lower binding energies. The Pb intercalation gives rise to hole-doping of graphene and results in a shift of the Dirac point energy by about 0.1 eV above the Fermi level, as revealed by the ARPES measurements. The KPFM experiments have shown that decoupling of the graphene layer by Pb intercalation is accompanied by a work function increase. The observed increase in the work function is attributed to the suppression of the electron transfer from the SiC substrate to the graphene layer. The Pb intercalated structure is found to be stable in ambient conditions and at high temperatures up to 1250 °C. These results demonstrate that the construction of a graphene-capped Pb/SiC system offers a possibility of tuning the graphene electronic properties and exploring intriguing physical properties such as superconductivity and spintronics. 

Effects of Pb Intercalation on the Structural and Electronic Properties of Epitaxial Graphene on SiC.

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

Honeycomb structures of group IV elements can host massless Dirac fermions with nontrivial Berry phases. Their potential for electronic applications has attracted great interest and spurred a broad search for new Dirac materials especially in monolayer structures. We present a detailed investigation of the β_{12} sheet, which is a borophene structure that can form spontaneously on a Ag(111) surface. Our tight-binding analysis revealed that the lattice of the β_{12} sheet could be decomposed into two triangular sublattices in a way similar to that for a honeycomb lattice, thereby hosting Dirac cones. Furthermore, each Dirac cone could be split by introducing periodic perturbations representing overlayer-substrate interactions. These unusual electronic structures were confirmed by angle-resolved photoemission spectroscopy and validated by first-principles calculations. Our results suggest monolayer boron as a new platform for realizing novel high-speed low-dissipation devices.

Dirac Fermions in Borophene.

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.

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

Structural and electronic properties of the SmB(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.

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

2D anisotropic Dirac cones are observed in χ 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 χ 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.

Discovery of 2D Anisotropic Dirac Cones.

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.

Fumio Komori

Institute for Solid State Physics

University of Tokyo

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