Angular Resolved Photoemission Spectroscopy Research Articles

Topological density-wave states in a particle-hole symmetric Weyl metal

We study the instabilities of a particle-hole symmetric Weyl metal with both electron and hole Fermi surfaces (FS) around the Weyl points. For a repulsive interaction, we find that the leading instability is towards a longitudinal spin-density-wave order (SDW$_z$). Besides, there exist three degenerate subleading instabilities: a charge-density-wave (CDW) instability and two transverse spin-density-wave (SDW$_{x,y}$) instabilities. For an attractive interaction the leading instabilities are towards two pair-density-wave orders (PDW) which pair the two FS's separately. Both the PDW and SDW$_z$ order parameters fully gap out FS's, while the CDW and SDW$_{x,y}$ ones leave line nodes on both FS's. For the SDW$_z$ and the PDW states, the surface Fermi arc in the metallic state evolves to a chiral Fermi line which passes the projection of the Weyl points and traverses the full momentum space. For the CDW state, the line node projects to a "drumhead" band localized on the surface, which can lead to a topological charge polarization. We verify the surface states by numerically simulating the angular-resolved photoemission spectroscopy data.

Band-gap engineering by Bi intercalation of graphene on Ir(111)

We report on the structural and electronic properties of a single bismuth layer intercalated underneath a graphene layer grown on an Ir(111) single crystal. Scanning tunneling microscopy (STM) reveals a hexagonal surface structure and a dislocation network upon Bi intercalation, which we attribute to a $\sqrt{3}\times\sqrt{3}R30{\deg}$ Bi structure on the underlying Ir(111) surface. Ab-initio calculations show that this Bi structure is the most energetically favorable, and also illustrate that STM measurements are most sensitive to C atoms in close proximity to intercalated Bi atoms. Additionally, Bi intercalation induces a band gap ($E_g=0.42\,$eV) at the Dirac point of graphene and an overall n-doping ($\sim 0.39\,$eV), as seen in angular-resolved photoemission spectroscopy. We attribute the emergence of the band gap to the dislocation network which forms favorably along certain parts of the moir\'e structure induced by the graphene/Ir(111) interface.

Rashba coupling amplification by a staggered crystal field

There has been increasing interest in materials where relativistic effects induce non-trivial electronic states with promise for spintronics applications. One example is the splitting of bands with opposite spin chirality produced by the Rashba spin-orbit coupling in asymmetric potentials. Sizable splittings have been hitherto obtained using either heavy elements, where this coupling is intrinsically strong, or large surface electric fields. Here by means of angular resolved photoemission spectroscopy and first-principles calculations, we give evidence of a large Rashba coupling of 0.25 eV Å, leading to a remarkable band splitting up to 0.15 eV with hidden spin-chiral polarization in centrosymmetric BaNiS2. This is explained by a huge staggered crystal field of 1.4 V Å−1, produced by a gliding plane symmetry, that breaks inversion symmetry at the Ni site. This unexpected result in the absence of heavy elements demonstrates an effective mechanism of Rashba coupling amplification that may foster spin-orbit band engineering.

Observation of the intrinsic bandgap behaviour in as-grown epitaxial twisted graphene.

Twisted graphene is of particular interest due to several intriguing characteristics, such as its the Fermi velocity, van Hove singularities and electronic localization. Theoretical studies recently suggested the possible bandgap opening and tuning. Here, we report a novel approach to producing epitaxial twisted graphene on SiC (0001) and the observation of its intrinsic bandgap behaviour. The direct deposition of C60 on pre-grown graphene layers results in few-layer twisted graphene confirmed by angular resolved photoemission spectroscopy and Raman analysis. The strong enhanced G band in Raman and sp(3) bonding characteristic in X-ray photoemission spectroscopy suggests the existence of interlayer interaction between adjacent graphene layers. The interlayer spacing between graphene layers measured by transmission electron microscopy is 0.352 ± 0.012 nm. Thermal activation behaviour and nonlinear current-voltage characteristics conclude that an intrinsic bandgap is opened in twisted graphene. Low sheet resistance (~ 160 Ω □(-1) at 10 K) and high mobility (~2,000 cm(2) V(-1) s(-1) at 10 K) are observed.

Atomic structure of epitaxial graphene sidewall nanoribbons: flat graphene, miniribbons, and the confinement gap.

Graphene nanoribbons grown on sidewall facets of SiC have demonstrated exceptional quantized ballistic transport up to 15 μm at room temperature. Angular-resolved photoemission spectroscopy (ARPES) has shown that the ribbons have the band structure of charge neutral graphene, while bent regions of the ribbon develop a bandgap. We present scanning tunneling microscopy and transmission electron microscopy of armchair nanoribbons grown on recrystallized sidewall trenches etched in SiC. We show that the nanoribbons consist of a single graphene layer essentially decoupled from the facet surface. The nanoribbons are bordered by 1-2 nm wide bent miniribbons at both the top and bottom edges of the nanoribbons. We establish that nanoscale confinement in the graphene miniribbons is the origin of the local large band gap observed in ARPES. The structural results presented here show how this gap is formed and provide a framework to help understand ballistic transport in sidewall graphene.

Tuning the Dirac point position in Bi(2)Se(3)(0001) via surface carbon doping.

Angular resolved photoemission spectroscopy in combination with abinitio calculations show that trace amounts of carbon doping of the Bi_{2}Se_{3} surface allows the controlled shift of the Dirac point within the bulk band gap. In contrast to expectation, no Rashba-split two-dimensional electron gas states appear. This unique electronic modification is related to surface structural modification characterized by an expansion of the top Se-Bi spacing of ≈11% as evidenced by surface x-ray diffraction. Our results provide new ways to tune the surface band structure of topological insulators.

Nonequilibrium probe of paired electron pockets in the underdoped cuprates

We propose an experimental method that can be used generally to test whether the cuprate pseudogap involves precursor pairing that acts to gap out the Fermi surface. The proposal involves angular-resolved photoemission spectroscopy (ARPES) performed in the presence of a transport current driven through the sample. We illustrate this proposal with a specific model of the pseudogap that contains a phase-incoherent paired electron and unpaired hole Fermi surfaces. We show that even a weak current tilts the paired band and modifies the pairing gap in a characteristic way directly measurable by ARPES. Stronger currents can also reveal the Fermi surface through direct suppression of pairing. The proposed experiment is sufficiently general such that it can be used to reveal putative Fermi surfaces that have been reconstructed from other types of periodic order and are gapped out due to pairing. The observation of the predicted phenomena should help resolve the central question about the existence of pairs in the enigmatic pseudogap regime.

Phonon structure in dispersion curves and density of states of massive Dirac fermions

Dirac fermions exist in many solid state systems including graphene, silicene and other two dimensional membranes such as are found in group VI dichalcogenides, as well as on the surface of some insulators where such states are protected by topology. Coupling of those fermions to phonons introduces new structures in their dispersion curves and, in the case of massive Dirac fermions, can shift and modify the gap. We show how these changes present in angular-resolved photoemission spectroscopy of the dressed charge carrier dispersion curves and scanning tunneling microscopy measurements of their density of states. In particular we focus on the region around the band gap. In this region the charge carrier spectral density no longer consists of a dominant quasiparticle peak and a smaller incoherent phonon related background. The quasiparticle picture has broken down and this leads to important modification in both dispersion curves and density of states.

Absence of a Dirac cone in silicene on Ag(111): First-principles density functional calculations with a modified effective band structure technique

We investigate the currently debated issue of the existence of the Dirac cone in silicene on an Ag(111) surface, using first-principles calculations based on density functional theory to obtain the band structure. By unfolding the band structure in the Brillouin zone of a supercell to that of a primitive cell, followed by projecting onto Ag and silicene subsystems, we demonstrate that the Dirac cone in silicene on Ag(111) is destroyed. Our results clearly indicate that the linear dispersions observed in both angular-resolved photoemission spectroscopy (ARPES) [P. Vogt et al, Phys. Rev. Lett. 108, 155501 (2012)] and scanning tunneling spectroscopy (STS) [L. Chen et al, Phys. Rev. Lett. 109, 056804 (2012)] come from the Ag substrate and not from silicene.

Strongly Spin-Orbit Coupled Two-Dimensional Electron Gas Emerging near the Surface of Polar Semiconductors

We investigate the two-dimensional highly spin-polarized electron accumulation layers commonly appearing near the surface of n-type polar semiconductors BiTeX (X=I, Br, and Cl) by angular-resolved photoemission spectroscopy. Because of the polarity and the strong spin-orbit interaction built in the bulk atomic configurations, the quantized conduction-band subbands show giant Rashba-type spin splitting. The characteristic 2D confinement effect is clearly observed also in the valence bands down to the binding energy of 4 eV. The X-dependent Rashba spin-orbit coupling is directly estimated from the observed spin-split subbands, which roughly scales with the inverse of the band-gap size in BiTeX.

Valence band electronic structure characterization of the rutile TiO2 (110)-(1 × 2) reconstructed surface

The electronic structure of the TiO2 (110)-(1×2) surface has been studied by means of angular resolved ultraviolet photoemission spectroscopy (ARUPS). The valence band dispersion along the high symmetry surface directions, [001] and [1–10], has been recorded. The experimental data show no dispersion of the band-gap Ti 3d states. However, the existence of dispersive bands along the [001] direction located at about 7eV below the Fermi level is reported. The existence of two different contributions in the emission from the defects-related state located in the gap of the surface is univocally shown for the first time.

Spin and charge structure of the surface states in topological insulators

We investigate the spin and charge densities of surface states of the three-dimensional topological insulator Bi${}_{2}$Se${}_{3}$, starting from the continuum description of the material [Zhang et al., Nat. Phys. 5, 438 (2009)]. The spin structure on surfaces other than the $(111)$ surface has additional complexity because of a misalignment of the contributions coming from the two sublattices of the crystal. For these surfaces we expect new features to be seen in the spin-resolved angular resolved photoemission spectroscopy (ARPES) experiments, caused by a nonhelical spin polarization of electrons at the individual sublattices as well as by the interference of the electron waves emitted coherently from two sublattices. We also show that the position of the Dirac crossing in the spectrum of the surface states depends on the orientation of the interface. This leads to contact potentials and surface charge redistribution at edges between different facets of the crystal.

Large Single Crystals of Graphene on Melted Copper Using Chemical Vapor Deposition

A simple method is presented for synthesizing large single crystal graphene domains on melted copper using atmospheric pressure chemical vapor deposition (CVD). This is achieved by performing the reaction above the melting point of copper (1090 °C) and using a molybdenum or tungsten support to prevent balling of the copper from dewetting. By controlling the amount of hydrogen during growth, individual single crystal domains of monolayer graphene greater than 200 μm are produced within a continuous film. Stopping growth before a complete film is formed reveals individual hexagonal domains of graphene that are epitaxially aligned in their orientation. Angular resolved photoemission spectroscopy is used to show that the graphene grown on copper exhibits a linear dispersion relationship and no sign of doping. HRTEM and electron diffraction reveal a uniform high quality crystalline atomic structure of monolayer graphene.

Thin layer composition profiling with angular resolved x-ray photoemission spectroscopy: Factors affecting quantitative results

Composition profiling of thin films in the nanometer range is critical to the development of future electronic devices. However, the number of techniques with such depth resolution is limited. Among them, angle-resolved x-ray photoelectron spectroscopy (ARXPS) can be used for thin layers up to a few nanometers, but it is not yet a fully established method. In order to evaluate its capabilities for use as a routine and general method, the authors evaluate both its intrinsic capabilities in comparison with other methods and the factors affecting quantification by analyzing its variability when applied at various laboratory locations with different tools and data treatments. For this purpose, dedicated samples based on multilayers of HfO2 and SiON were produced with a well-determined layer structure. The results show that ARXPS, including depth profiling reconstruction, is very efficient and compares favorably with nuclear analysis techniques. It allows the separation of the surface contamination signal from the interfacial layer signal and allows determination of the coverage quantitatively. An accuracy of ±10% is achieved for most elements except for nitrogen, where strong peak interference with hafnium and a low intensity increase the inaccuracy up to 20%. This study also highlights several technique limitations. First, the quality of the retrieved profile is strongly dependent upon the exact determination of each photoemission peak intensity. Also it demonstrates that, while favorable for chemical identification, very high resolution spectra may lead to larger errors in profile reconstruction due to larger statistical errors in the intensities, though this is true mainly for deeper layers. Finally, it points out the importance of the physical parameters used in the final obtained results.

Silicene: Compelling Experimental Evidence for Graphenelike Two-Dimensional Silicon

Because of its unique physical properties, graphene, a 2D honeycomb arrangement of carbon atoms, has attracted tremendous attention. Silicene, the graphene equivalent for silicon, could follow this trend, opening new perspectives for applications, especially due to its compatibility with Si-based electronics. Silicene has been theoretically predicted as a buckled honeycomb arrangement of Si atoms and having an electronic dispersion resembling that of relativistic Dirac fermions. Here we provide compelling evidence, from both structural and electronic properties, for the synthesis of epitaxial silicene sheets on a silver (111) substrate, through the combination of scanning tunneling microscopy and angular-resolved photoemission spectroscopy in conjunction with calculations based on density functional theory.

Effect of gadolinium doping on the electronic band structure of europium oxide

High quality films of EuO and Eu${}_{0.96}$Gd${}_{0.04}$O were grown on $p$-type Si(100) via pulsed laser deposition. X-ray-diffraction results show that the addition of Gd changes the growth texture from [001] to [111]. Angular-resolved photoemission spectroscopy reveals electron pockets around the $X$ points in Gd-doped EuO, indicating that the band gap in EuO is indirect. Combined photoemission and inverse photoemission measurements show an apparent transition from $n$-type to $p$-type behavior, which is likely due to band bending near the polar (111) surface.

Reactive Chemical Doping of theBi2Se3Topological Insulator

Using angular resolved photoemission spectroscopy we studied the evolution of the surface electronic structure of the topological insulator Bi(2)Se(3) as a function of water vapor exposure. We find that a surface reaction with water induces a band bending, which shifts the Dirac point deep into the occupied states and creates quantum well states with a strong Rashba-type splitting. The surface is thus not chemically inert, but the topological state remains protected. The band bending is traced back to Se abstraction, leaving positively charged vacancies at the surface. Because of the presence of water vapor, a similar effect takes place when Bi(2)Se(3) crystals are left in vacuum or cleaved in air, which likely explains the aging effect observed in the Bi(2)Se(3) band structure.

Tuning the spin texture in binary and ternary surface alloys on Ag(111)

A giant spin splitting has been observed in surface alloys on noble metal (111) surfaces as a result of a strong structural modification at the surface as well as the large atomic spin-orbit interaction (SOI) of the alloy atoms. These surface alloys are an ideal playground to manipulate both the size of the spin splitting as well as the position of the Fermi level, as it is possible to change the atomic SOI as well as the relaxation by varying alloy atoms and substrates. Using (spin- and) angular-resolved photoemission spectroscopy in combination with quantitative low-energy electron diffraction, we have studied the mixed binary Bi${}_{x}$Sb${}_{1\ensuremath{-}x}$/Ag(111) surface alloy where we observed a continuous evolution of the band structure with $x$ and the mixed ternary Bi${}_{0.3}$Pb${}_{0.35}$Sb${}_{0.35}$/Ag(111) surface alloy.

Illuminating the dark corridor in graphene: Polarization dependence of angle-resolved photoemission spectroscopy on graphene

We have used s- and p-polarized synchrotron radiation to image the electronic structure of epitaxial graphene near the K-point by angular resolved photoemission spectroscopy (ARPES). Part of the experimental Fermi surface is suppressed due to the interference of photoelectrons emitted from the two equivalent carbon atoms per unit cell of graphene's honeycomb lattice. Here we show that by rotating the polarization vector, we are able to illuminate this 'dark corridor' indicating that the present theoretical understanding is oversimplified. Our measurements are supported by first-principles photoemission calculations, which reveal that the observed effect persists in the low photon energy regime.

Photoemission spectroscopy at MOVPE-prepared InGaAs(100) surface reconstructions

Abstract Angular resolved ultraviolet photoemission spectroscopy at BESSY was employed to study the electronic structure of the three different, (4 × 3)-, (2 × 4)-, and (4 × 2)-surface reconstructions of In 0.53 Ga 0.47 As, which was grown lattice-matched to InP(100). The surfaces have been prepared using metal organic vapor phase epitaxy (MOVPE). For spectroscopy, a dedicated transfer system was employed and samples were transferred contamination-free from the MOVPE reactor to UHV-based analysis tools. For the different surface reconstructions, the Γ − Δ − X direction was scanned while varying the photon energy between 10 eV and 28 eV. We observed two surface states in the photoelectron spectra on all of these surface reconstructions in addition to the bulk derived valence band emissions. Different binding energies of the surface states originating from different surface band bending were detected and described.