We present an experimental setup for laser-based angle-resolved time-of-flight photoemission. Using a picosecond pulsed laser, photons of energy 10.5 eV are generated through higher harmonic generation in xenon. The high repetition rate of the light source, variable between 0.2 and 8 MHz, enables high photoelectron count rates and short acquisition times. By using a time-of-flight analyzer with angle-resolving capabilities, electrons emitted from the sample within a circular cone of up to +/- 15 degrees can be collected. Hence, simultaneous acquisition of photoemission data for a complete area of the Brillouin zone is possible. The current photon energy enables bulk sensitive measurements, high angular resolution, and the resulting covered momentum space is large enough to enclose the entire Brillouin zone in cuprate high-T(c) superconductors. Fermi edge measurements on polycrystalline Au shows an energy resolution better than 5 meV. Data from a test measurement of the Au(111) surface state are presented along with measurements of the Fermi surface of the high-T(c) superconductor Bi(2)Sr(2)CaCu(2)O(8+delta) (Bi2212).
Several proposed applications and exotic effects in topological insulators rely on the presence of helical Dirac states at the interface between a topological insulator and a normal insulator. In the present work, we have used low-energy angle-resolved photoelectron spectroscopy to uncover and characterize the interface states of Bi2Se3 thin films and Bi2Te3/Bi2Se3 heterostructures grown on Si(111). The results establish that Dirac fermions are indeed present at the topological-normal-insulator boundary and absent at the topological-topological-insulator interface. Moreover, it is demonstrated that band bending present within the topological-insulator films leads to a substantial separation of the interface and surface states in energy. These results pave the way for further studies and the realization of interface-related phenomena in topological-insulator thin-film heterostructures.
A new type of hemispherical electron energy analyzer that permits angle and spin resolved photoelectron spectroscopy has been developed. The analyzer permits standard angle resolved spectra to be recorded with a two-dimensional detector in parallel with spin detection using a mini-Mott polarimeter. General design considerations as well as technical solutions are discussed and test results from the Au(111) surface state are presented.
From a spin-resolved photoemission study on the Bi2Sr2CaCu2O8+delta superconductor, we show experimentally that the first ionization state is of nearly pure singlet character. This is true both above and below the superconducting transition and in the presence of doping and band formation. This provides direct support for the existence and stability of Zhang-Rice singlets in high-temperature superconductors, justifying the ansatz of single-band models. Moreover, we establish this technique as an important probe for a wide range of cuprates and strongly correlated materials.
High-temperature superconductivity emerges from an un-conventional metallic state. This has stimulated strong efforts to understand exactly how Fermi liquids breakdown and evolve into an un-conventional metal. A fundamental question is how Fermi liquid quasiparticle excitations break down in momentum space. Here we show, using angle-resolved photoemission spectroscopy, that the Fermi liquid quasiparticle excitations of the overdoped superconducting cuprate La1.77Sr0.23CuO4 is highly anisotropic in momentum space. The quasiparticle scattering and residue behave differently along the Fermi surface and hence the Kadowaki-Wood's relation is not obeyed. This kind of Fermi liquid breakdown may apply to a wide range of strongly correlated metal systems where spin fluctuations are present.
We report an angle-resolved photoemission study of the electronic structure of the pseudogap state in La1.48Nd0.4Sr0.12CuO4 (T-c < 7 K). Two opposite dispersing Fermi arcs are the main result of this study. Several scenarios that can explain this observation are discussed.
The existence of coherent quasiparticles near the Fermi energy in the low-temperature state of high-temperature superconductors has been well established by angle-resolved photoemission spectroscopy (ARPES). We present a study of La1.83Sr0.17CuO4 in the superconducting state and report an abrupt change in the quasiparticle spectral function, as we follow the dispersion of the ARPES signal from the Fermi energy to 0.6 eV. The interruption in the quasiparticle dispersion separates coherent quasiparticle peaks at low energies from broad incoherent excitations at high energies. We find that the boundary between these low-energy and high-energy features exhibits a cosine-shaped momentum dependence, reminiscent of the superconducting d-wave gap. Further intriguing similarities between characteristics of the incoherent excitations and quasiparticle properties suggest a close relation between the electronic response at high and low energies in cuprate superconductors.
An angle-resolved photoemission study of the scattering rate in the superconducting phase of the high-temperature superconductor La2-xSrxCuO4 with x=0.145 and x=0.17, as a function of binding energy and momentum, is presented. We observe that the scattering rate scales linearly with binding energy up to the high-energy scale E-1 similar to 0.4 eV. The scattering rate is found to be strongly anisotropic, with a minimum along the (0,0)-(pi,pi) direction. A possible connection to a quantum-critical point is discussed.
We have performed an angle resolved photoemission study on a single crystal of the optimally electron doped (n-type) cuprate superconductor Nd2-xCexCuO4 (x=0.15) at a photon energy of 400 eV. The Fermi surface is mapped out and is, in agreement with earlier measurements, of hole-type with the expected Luttinger volume. However, comparing with previous low energy measurements, we observe a different Fermi surface shape and a different distribution of spectral intensity around the Fermi surface contour. The observed Fermi surface shape indicates a stronger electron correlation in the bulk as compared to the surface.
We present angle-resolved photoelectron spectroscopy data probing the electronic structure of the Nd-substituted high-T-c cuprate La1.48Nd0.4Sr0.12CuO4. Data have been acquired at low and high photon energies, h nu=55 and 500 eV, respectively. The two extracted Fermi surfaces show significant differences. The differences can be attributed to either the change in probing depth suggesting dissimilarity of the intrinsic electronic structure between surface and bulk regions, or a considerable c-axis dispersion signaling a strong interlayer coupling. At both photon energies, considerable spectral weight is observed at all points along the Fermi surface and the intensity distribution as well as Fermi-surface shape observed at low as well as high photon energy is markedly different from what has been previously reported for La1.28Nd0.6Sr0.12CuO4 by Zhou [Science 286, 268 (1999)]. Document Type: Article
We use high-resolution angle-resolved photoemission spectroscopy to investigate the electronic structure of the antiferromagnetic heavy fermion compound CePt2In7, which is amember of the CeIn3-derived heavy fermion material family. Weak hybridization among 4f electron states and conduction bands was identified in CePt2In7 at low temperature much weaker than that in the other heavy fermion compounds like CeIrIn5 and CeRhIn5. The Ce 4f spectrum shows fine structures near the Fermi energy, reflecting the crystal electric field splitting of the 4f(5/2)(1) and 4f(7/2)(1) states. Also, we find that the Fermi surface has a strongly three-dimensional topology, in agreement with density-functional theory calculations.
Topological insulators are a class of quantum materials in which time-reversal symmetry, relativistic effects and an inverted band structure result in the occurrence of electronic metallic states on the surfaces of insulating bulk crystals. These helical states exhibit a Dirac-like energy dispersion across the bulk bandgap, and they are topologically protected. Recent theoretical results have suggested the existence of topological crystalline insulators (TCIs), a class of topological insulators in which crystalline symmetry replaces the role of time-reversal symmetry in ensuring topological protection(1,2). In this study we show that the narrow-gap semiconductor Pb1-xSnxSe is a TCI for x = 0.23. Temperature-dependent angle-resolved photoelectron spectroscopy demonstrates that the material undergoes a temperature-driven topological phase transition from a trivial insulator to a TCI. These experimental findings add a new class to the family of topological insulators, and we anticipate that they will lead to a considerable body of further research as well as detailed studies of topological phase transitions.
The effect of capping a dilute assembly of nanoscale mass-selected Fe clusters with a Co thin film has been studied using X-ray magnetic circular dichroism (XMCD). The clusters, containing around 400 atoms, were deposited in situ from a gas-aggregation source onto highly oriented pyrolytic graphite. The exposed clusters possess magnetic moments that are enhanced compared to the bulk, by around 4% for m(spin) and around 75% for m(orb). In addition, a surface core level shifted component is observed in the L-3.2 XMCD spectrum. Upon adding the Co layer, the surface component disappears, m(orb) is decreased for the Fe clusters, and m(spin) increases. The exposed clusters are magnetically isotropic but a strong in-plans anisotropy is observed after depositing the Co overlayer. We attribute this to the shape of the Co islands in which the Fe clusters are embedded.
The magnetic moments in exposed, mass-selected, nanoscale Fe clusters in the size range 1.89-2.20 nm (300-475 atoms), deposited onto graphic in situ have been measured by X-ray magnetic circular dichroism. The smallest clusters possess moments that are enhanced by around 4% for m(spin) and 80% for m(orb) and decrease towards the bulk value with increasing size. The larger clusters show an in-plane anisotropy that is consistent with the anisotropy in the orbital moment. The smallest clusters are, within experimental error, magnetically isotropic. The anisotropy constant in the 475-atom clusters is significantly higher than the bulk value.
Nodal angle-resolved photoemission spectra taken on overdoped La1.77Sr0.23CuO4 are presented and analyzed. It is proven that the low-energy excitations are true Landau Fermi-liquid quasiparticles. We show that momentum and energy distribution curves can be analyzed self-consistently without quantitative knowledge of the bare band dispersion. Finally, by imposing Kramers-Kronig consistency on the self-energy Sigma, insight into the quasiparticle residue is gained. We conclude by comparing our results to quasiparticle properties extracted from thermodynamic, magnetoresistance, and high-field quantum oscillation experiments on overdoped Tl2Ba2CuO6+delta.
The magnetic circular dichroism in the perpendicular geometry of the resonant 2p3p3p photoemission (PE) spectroscopy has been investigated in metallic Ni as a function of the photon energy across the Ni Lj absorption edge. Within the experimental error bars, the photon energy dependence of the PE dichroism signal is the same as the one shown by the magnetic circular dichroism of the corresponding x-ray absorption (XMCD), obtained in the collinear geometry. This is attributed to the fact that, in metal Ni, the orbital [L-z] and dipolar [T-z] moments are smaller than the spin angular moment [S-z]. The latter is the dominating term in both the expressions that give the integrated values of the PE dichroism or XMCD intensities, Although the respective photon energy dependence is very similar, the normalized PE dichroism intensity is a factor similar to 5.6 smaller than the normalized XMCD signal, while only a factor similar to 1.6 is expected from theoretical considerations. This factor is observed even below the L-3 threshold, thus we exclude that the small intensity of the perpendicular geometry dichroism in the Ni 2p3p3p resonant photoemission is due to fast relaxation processes in the intermediate state.
The intensity of the O 1s core photoemission peak has been measured for CuO and NiO as the photon energy is scanned across the L-3 absorption edge of the metal ion. In CuO, the O 1s peak shows a typical antiresonant behavior, with a sizable decrease of its cross section at photon energies below the Cu L-3 threshold. No detectable effect is observed for NiO. The CuO data are well reproduced by a multiatom resonant photoemission model based on resonant light scattering.
We have investigated the behavior of the 2p3p3p and 2p3s3p Anger lines of CuO and Cu2O scanning the photon energy across the Cu L-3 resonance. For both samples, when the excitation energy is below the L-3 resonance, we observe the 2p3p3p and 2p3s3p peaks at constant binding energy. This behavior is typical of nonradiative resonant Raman scattering. If the photon energy is raised above the L-3 maximum, the two samples behave in different ways. In CuO, the Auger peaks are always observed at constant binding energy, while in Cu2O their kinetic energy first reaches a maximum at correspondence with the absorption threshold, and then stabilizes at a value slightly higher than the off-resonance Auger peaks. These differences are interpreted in terms of the different electronic structure of the Auger intermediate state at resonance. In CuO, the intermediate state corresponds to a single 2p(3/2) core hole, with the Cu 3d band completely filled. On the contrary, in Cu2O the intermediate state is represented by the combination of a 2p(3/2) hole with a 4sp electron in strong interaction with the O-2sp valence band. In CuO, for photon energies higher than 1.5 eV above the L-3-edge maximum, the constant binding energy radiationless Raman peaks are accompanied by constant kinetic energy replicas. These are attributed to the relaxation of the Auger intermediate state through electron-hole pair generation across the band gap of the material. Satellites that could be associated to relaxation precesses involving energies smaller than the band gap are not resolved. No variation of the lineshape of the Anger peaks is observed as a function of the sample temperature, indicating that different densities of thermally accessible excitations do not have a strong influence on the recombination process of the core hole.
Using spin-resolved resonant photoemission we have probed the singlet vs. triplet character of the two-hole state in the layered cuprates Bi2Sr2CaCu2O8+delta La2-xSrxCuO4 and Sr2CuO2Cl2. The combination of the photon circular polarization with the photoelectron spin detection gives access to the character of the photoemission final states, which correspond to the two-hole configurations localized at a (CuO4) site. In particular, the lowest energy state is found to have a very high singlet character in all the measured compounds. This can be considered as a strong indication of the existence and stability of the so-called Zhang-Rice singlets in the layered cuprates.
The x-ray photoemission spectrum of the valence states of 3d transition-metal systems is spin polarized when using circularly polarized photons. The integral of the spin-orbit spectrum is proportional to the expectation value of the angular part of the 3d spin-orbit operator in the initial state. We show that this quantity can be used to get an estimate of the atomic orbital moment. While the measurement is sensitive to the magnetization axis, it does not require a net macroscopic magnetization nor the presence of a long-range magnetic order, and is therefore suitable for any transition-metal systems being antiferromagnetic or paramagnetic or magnetically disordered. In the case of full 3d shell the integral of the spin-orbit spectrum is zero, but the spectral shape can give a direct estimate of the 3d spin-orbit energy splitting DeltaE(SO). We have used Cu and CoO to experimentally test this technique. As expected Cu provides a vanishing result for , whereas for Co2+ in CoO we find =1.36h at 0 K. On the other hand we find DeltaE(SO)similar or equal to280 meV for Cu.
The electronic structure and the electron dynamics of the clean InAs(111)A 2 x 2 and the InAs(111)B 1 x 1 surfaces have been studied by laser pump-and-probe photoemission spectroscopy. Normally unpopulated electron states above the valence band maximum (VBM) are filled on the InAs(111)A surface due to the conduction band pinning above the Fermi level (E-F). Accompanied by the downward band banding alignment, a charge accumulation layer is confined to the surface region creating a two dimensional electron gas (2DEG). The decay of the photoexcited carriers above the conduction band minimum (CBM) is originated by bulk states affected by the presence of the surface. No occupied states were found on the InAs(111)B 1 x 1 surface. This fact is suggested to be due to the surface stabilisation by the charge removal from the surface into the bulk. The weak photoemission intensity above the VBM on the (111)B surface is attributed to electron states trapped by surface defects. The fast decay of the photoexcited electron states on the (111)A and the (111)B surfaces was found to be tau(111A) less than or equal to 5 ps and tau(111B) less than or equal to 4ps, respectively. We suggest the diffusion of the hot electrons into the bulk is the decay mechanism. (
We present a soft x-ray angle-resolved photoemission spectroscopy study of overdoped high-temperature superconductors. In-plane and out-of-plane components of the Fermi surface are mapped by varying the photoemission angle and the incident photon energy. No k(z) dispersion is observed along the nodal direction, whereas a significant antinodal k(z) dispersion is identified for La-based cuprates. Based on a tight-binding parametrization, we discuss the implications for the density of states near the van Hove singularity. Our results suggest that the large electronic specific heat found in overdoped La2-xSrxCuO4 cannot be assigned to the van Hove singularity alone. We therefore propose quantum criticality induced by a collapsing pseudogap phase as a plausible explanation for observed enhancement of electronic specific heat.
Room temperature deposition of Sn on the Pt(110)(1 x 2) surface has been studied by scanning tunnelling microscopy and core level photoelectron spectroscopy. At low coverage Sri is found in three different configurations; as mobile adatoms in the valley of the missing-row reconstruction, as 1D-Pt-Sn-Pt- alloy chains forming local Pt3Sn(110)2 x 2 regions and finally as 3D alloy islands. At higher coverage these islands form a platinum rich alloy film, which is dissolved in the crystal upon annealing to 600 degreesC.
We present a detailed study of the valence and conduction bands of VO2 across the metal-insulator transition using bulk-sensitive photoelectron and O K x-ray absorption spectroscopies. We observe a giant transfer of spectral weight with distinct features that require an explanation which goes beyond the Peierls transition model as well as the standard single-band Hubbard model. Analysis of the symmetry and energies of the bands reveals the decisive role of the V 3d orbital degrees of freedom. Comparison to recent realistic many body calculations shows that much of the k dependence of the self-energy correction can be cast within a dimer model.
The charge density in solids is a fundamental parameter. Here we demonstrate that the charge density can be determined by the use of angle resolved photoelectron spectroscopy. The method, which involves a Fourier-like transform from momentum space to real space, is demonstrated by utilizing soft x-ray angle resolved photoelectron spectroscopy to sample the complete three-dimensional Brillouin zone of copper. It is also shown that this can be done in an energy resolved way as to extract the charge density contribution from states of a particular energy.
We report an angle-resolved photoemission study of the charge stripe ordered La1.6-xNd0.4SrxCuO4 (Nd-LSCO) system. A comparative and quantitative line-shape analysis is presented as the system evolves from the overdoped regime into the charge ordered phase. On the overdoped side (x = 0.20), a normal-state antinodal spectral gap opens upon cooling below 80 K. In this process, spectral weight is preserved but redistributed to larger energies. A correlation between this spectral gap and electron scattering is found. A different line shape is observed in the antinodal region of charge ordered Nd-LSCO x = 1/8. Significant low-energy spectral weight appears to be lost. These observations are discussed in terms of spectral-weight redistribution and gapping originating from charge stripe ordering.
The minimal ingredients to explain the essential physics of layered copper-oxide (cuprates) materials remains heavily debated. Effective low-energy single-band models of the copper-oxygen orbitals are widely used because there exists no strong experimental evidence supporting multi-band structures. Here, we report angle-resolved photoelectron spectroscopy experiments on La-based cuprates that provide direct observation of a two-band structure. This electronic structure, qualitatively consistent with density functional theory, is parametrised by a two-orbital (d(x2-y2) and d(z2)) tight-binding model. We quantify the orbital hybridisation which provides an explanation for the Fermi surface topology and the proximity of the van-Hove singularity to the Fermi level. Our analysis leads to a unification of electronic hopping parameters for single-layer cuprates and we conclude that hybridisation, restraining d-wave pairing, is an important optimisation element for superconductivity.
LaCoO3 displays two broad anomalies in the DC magnetic susceptibility chi(DC), occurring, respectively, around 50 K and 500 K. We have investigated the first of them within the 10 K < T < RT temperature range using Co K alpha(1) x-ray absorption spectroscopy (XAS) in the partial fluorescence yield mode. In contrast with previous O K-edge XAS reports, our data show the existence of abrupt changes around 50 K which can be nicely correlated with the anomaly in chi(DC). To our knowledge, this is the first time that a clear, quantitative relationship between the temperature dependence of the magnetic susceptibility and that of the XAS spectra is reported. The intensity changes in the preedge region, which are consistent with a transition from a lower to a higher spin state, have been analyzed using a minimal model including the Co 3d and O 2p hybridization in the initial state. The temperature dependence of the Co magnetic moment obtained from the estimated e(g) and t(2g) occupations could be satisfactorily reproduced. Also, the decrease of the Co 3d and O 2p hybridization by increasing temperature obtained from this simple model compares favorably with the values estimated from thermal evolution of the crystallographic structure.
A theoretical description of the Fano effect in the angle-integrated valence-band photoemission of paramagnetic solids is presented that is based on the one-step model of photoemission and relativistic multiple-scattering theory. Applications to fcc-Cu led to a very satisfying agreement with recent experimental data that show the Fano effect, i.e., a finite spin-polarization for the spectra is found for excitation with circularly polarized radiation. As can be demonstrated by model calculations. this finding is caused by the presence of spin-orbit coupling. To allow for a more detailed discussion of the spectra a simplified description of the Fano effect is presented that treats spin-orbit coupling as a perturbation.
A theoretical description of the Fano-effect in the angle-integrated valence-band photoemission (VB XPS) of paramagnetic solids is presented that is based on the one-step model of photoemission and relativistic multiple scattering theory. Applications to fcc-Cu and fcc-Ag led to a very satisfying agreement with recent experimental data that show the Fano-effect, i.e., a finite spin polarisation of the photoelectrons is found for excitation with circularly polarised radiation. As can be demonstrated by model calculations, this finding is caused by the presence of spin-orbit coupling. To allow for a more detailed discussion of the spectra, a simplified description of the Fano-effect is presented that treats spin-orbit coupling as a perturbation.
O 1s x-ray absorption study of the Mott insulator Ca2RuO4 shows that the orbital population of the 4d t(2g) band dramatically changes with temperature. In addition, spin-resolved circularly polarized photoemission study of Ca2RuO4 shows that a substantial orbital angular momentum is induced in the Ru 4d t(2g) band. Based on the experimental results and model Hartree-Fock calculations, we argue that the cooperation between the strong spin-orbit coupling in the Ru 4d t(2g) band and the small distortion of the RuO6 octahedra causes the interesting changeover of the spin and orbital anisotropy as a function of temperature.
The low-temperature microscopic magnetic properties of the quasi-2D heavy- fermion compound, CePt2In7 are investigated by using a positive muon-spin rotation and relaxation (μ+SR) technique. Clear evidence for the formation of a commensurate antiferromagnetic order below TN 5.40 K is presented. The magnetic order parameter is shown to fit well to a modified BCS gap-energy function in a strong-coupling scenario.
An on-board sample cleaver has been developed in order to cleave small and hard-to-cleave samples. To acquire good cleaves from rigid samples the alignment of the cleaving blade with respect to the internal crystallographic planes is crucial. To have the opportunity to mount the sample and align it to the blade ex situ has many advantages. The design presented has allowed us to cleave very tiny and rigid samples, e.g., the high-temperature superconductor La(2-x)SrxCuO4. Further, in this design the sample and the cleaver will have the same temperature, allowing us to cleave and keep the sample at low temperature. This is a big advantage over prior cleaver systems. As a result, better surfaces and alignments can be realized, which considerably simplifies and improves the experiments.
Transiently excited electron states at the GaSb(001) surface have been studied by means of time- and angle-resolved photoemission spectroscopy based on a femtosecond laser system. A normally unpopulated surface electron state has been found at similar to 250 meV above the valence band maximum with a strong confinement at the center of the surface Brillouin zone. The lifetime of transiently excited carriers at the intergap surface states has been found to be similar to 11 ps, associated with rapid carrier diffusion.
We present the first study revealing the electronic structure and electron dynamics of the excited adatom state at the Ge(111): Sn(root 3 x root 3)R30 degrees surface. By the use of time- and angle-resolved photoemission spectroscopy, the normally unoccupied electronic structure of the partly empty Sn adatom can be probed. From the angle-resolved data we conclude that the adatom electrons at the Ge:Sn surface are more delocalized than at the clean Ge(111)c(2 x 8) surface. A unique pump-and-probe technique, based on a pulsed femtosecond laser-system, has also allowed us to study the recombination process of the excited state. We connect the recombination process of the excited electrons to the coherent fluctuations of the Sn adatoms. As a result we present an estimate for the time between each collective and coherent adatom flip Delta t = 9 ps, i.e. an adatom switching frequency nu(SW) approximate to 0.1 THz. We find that our results, contrary to scanning tunneling microscopy measurements [F. Ronci, S. Colonna, S.D. Thorpe, A. Cricenti, G. Le Lay, Phys. Rev. Lett. 95 (2005) 156101], agree very well with values extracted from molecular dynamics simulations found in the literature [J. Avila, A. Mascaraque, E.G. Michel, M.C. Asensio, G. Le Lay, J. Ortega, R. Perez, F. Flores, Phys. Rev. Lett. 82 (1999) 442; D. Farias, W. Kaminski, J. Lobo, J. Ortega, E. Hulpke, R. Perez, F. Flores, E.G. Michel, Phys. Rev. Lett. 91 (2003) 16103].
Epitaxial growth of Fe on a stepped Cu(111) surface leads to the formation of fee Fe stripes along the step edges for coverages lower than 1.5 monolayer (ML). Using the sensitivity of the x-ray magnetic circular dichroism and sum-rule analysis, the changes in the magnetic properties in the low thickness range from similar to 5% of a monolayer to 4 ML, covering the one-dimensional (1D) coalescence (similar to 0.8 ML) and the 2D percolation limit (similar to 1.5 ML), have been determined. The determination of the spin moment (m(spin)) indicates significant features which can be correlated to the morphological transition. In particular, the m(spin) decreases at the 1D coalescence limit, but increases as the film reaches the 2D percolation limit and starts to transform into the bcc phase. This behavior is tentatively ascribed to the decrease in the Fe atomic volume, as it is well known that such changes can dramatically modify the magnetic properties of gamma-Fe.
We have investigated the initial stages of titanyl phthalocyanine (TiOPc) growth on single crystalline ZnO(0 0 0 1). This organic-semiconductor interface is self-organizing as a 2 x 1 pattern appears in a low energy electron diffraction upon deposition of the molecules. To achieve this pattern, the TiOPc is suggested to adsorb standing with the edge of the molecule along the substrate atomic rows. Photoelectron spectroscopy is used to further analyze the interface; a relatively large upwards band bending amounting to 0.5 eV is found and a splitting of the molecules highest occupied molecular orbital occurs after thermal treatment, indicating that the molecules are lying down.
We report a study of the initial interface formation of Co on InAs(1 1 1)A and B surfaces using high resolution photoelectron spectroscopy and scanning tunneling microscopy. We observe a strong chemical interaction between Co and, in particular, surface indium forming a metallic overlayer already below monolayer coverage. On annealed surfaces this overlayer agglomerates into islands, with a narrow size distribution. Furthermore, no two-dimensional electron gas is formed on InAs(1 1 1)A-Co in contrast to the clean surface.
We have measured hard x-ray photoemission spectra of pure vanadium sesquioxide (V2O3) across its metal-insulator transition. We show that, in the metallic phase, a clear correlation exists between the shakedown satellites observed in the vanadium 2p and 3p core-level spectra and the coherent peak measured at the Fermi level. Comparing experimental results and dynamical mean-field theory calculations, we estimate the Hubbard energy U in V2O3 (4.20 +/- 0.05 eV). From our bulk-sensitive photoemission spectra we infer the existence of a critical probing depth for investigating electronic properties in strongly correlated solids.
We report core level and valence band photoemission results obtained for Nd2-xCexCuO4 (x = 0.15) single crystals and films by using both soft and hard x rays, hence, with tunable depth sensitivity. When using hard x rays only, we observe distinct and energy separated structures in the main 2p(5)3d(9)L peak of Cu 2p(3/2) and 2p(1/2) core levels, including the well screened features located at the high kinetic energy side, which were recently reported by Taguchi et al. [Phys. Rev. Lett. 95, 177002 (2005)]. By varying the photoelectron takeoff angle, we analyze the difference in the screening properties between surface and bulk, and we demonstrate the depth dependence of the electronic properties by following the evolution of the bulk-related peak. The possible influence of the surface conditions on the Cu 2p spectral features is also discussed.
We present a comprehensive study of the photon energy dependence of the valence band photoemission yield in the prototype Mott-Hubbard oxide V2O3. The analysis of our experimental results, covering an extended photon energy range (20-6000 eV) and combined with GW calculations, allows us to identify the nature of the orbitals contributing to the total spectral weight at different binding energies, and in particular to locate the V 4s states at about 8 eV binding energy. From this comparative analysis, we conclude that the intensity of the quasiparticle photoemission peak, observed close to the Fermi level in the paramagnetic metallic phase upon increasing photon energy, does not have a significant correlation with the intensity variation in the O 2p and V 3d yield, thus, confirming that bulk sensitivity is an essential requirement for the detection of this coherent low-energy excitation.
We present angle-resolved photoemission spectroscopy measurements of the surface states on in-situ grown (111) oriented films of Pb1-xSnxSe, a three-dimensional topological crystalline insulator. We observe surface states with Dirac-like dispersion at (Gamma) over bar and (M) over bar in the surface Brillouin zone, supporting recent theoretical predictions for this family of materials. We study the parallel dispersion isotropy and Dirac-point binding energy of the surface states, and perform tight-binding calculations to support our findings. The relative simplicity of the growth technique is encouraging, and suggests a clear path for future investigations into the role of strain, vicinality, and alternative surface orientations in (Pb,Sn)Se solid solutions.
The "double Dirac cone" 2D topological interface states found on the (001) faces of topological crystalline insulators such as Pb1-xSnxSe feature degeneracies located away from time reversal invariant momenta and are a manifestation of both mirror symmetry protection and valley interactions. Similar shifted degeneracies in 1D interface states have been highlighted as a potential basis for a topological transistor, but realizing such a device will require a detailed understanding of the intervalley physics involved. In addition, the operation of this or similar devices outside of ultrahigh vacuum will require encapsulation, and the consequences of this for the topological interface state must be understood. Here we address both topics for the case of 2D surface states using angle-resolved photoemission spectroscopy. We examine bulk Pb1-xSnxSe(001) crystals overgrown with PbSe, realizing trivial/topological heterostructures. We demonstrate that the valley interaction that splits the two Dirac cones at each (X) over bar is extremely sensitive to atomic-scale details of the surface, exhibiting non-monotonic changes as PbSe deposition proceeds. This includes an apparent total collapse of the splitting for sub-monolayer coverage, eliminating the Lifshitz transition. For a large overlayer thickness we observe quantized PbSe states, possibly reflecting a symmetry confinement mechanism at the buried topological interface.
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