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Sample records for core-level photoemission study

  1. A study of angle-resolved photoemission extended fine structure as applied to the Ni 3p, Cu 3s, and Cu 3p core levels of the respective clean (111) surfaces

    SciTech Connect

    Huff, W.R.A.; Moler, E.J.; Kellar, S.A.

    1997-04-01

    The first non-s initial state angle-resolved photoemission extended fine structure (ARPEFS) study of clean surfaces for the purpose of further understanding the technique is reported. The surface structure sensitivity of ARPEFS applied to clean surfaces and to arbitrary initial states is studied using normal photoemission data taken from the Ni 3p core levels of a Ni(111) single crystal and the Cu 3s and the Cu 3p core-levels of a Cu(111) single crystal. The Fourier transforms of these clean surface data are dominated by backscattering. Unlike the s initial state data, the p initial state data show a peak in the Fourier transform corresponding to in-plane scattering from the six nearest-neighbors to the emitter. Evidence was seen for single-scattering events from in the same plane as the emitters and double-scattering events. Using a newly developed, multiple-scattering calculation program, ARPEFS data from clean surfaces and from p initial states can be modeled to high precision. Although there are many layers of emitters when measuring photoemission from a clean surface, test calculations show that the ARPEFS signal is dominated by photoemission from atoms in the first two crystal layers. Thus, ARPEFS applied to clean surfaces is sensitive to surface reconstruction. The known contraction of the first two Cu(111) layers is confirmed. The best-fit calculation for clean Ni(111) indicates an expansion of the first two layers. To better understand the ARPEFS technique, the authors studied s and non-s initial state photoemission from clean metal surfaces.

  2. Alkaline Earth Core Level Photoemission Spectroscopy of High-Temperature Superconductors

    NASA Technical Reports Server (NTRS)

    Vasquez, R.

    1993-01-01

    This paper examines photoemission measurements of the alkaline Earth core levels of high-temperature superconductors and related materials, models that seek to explain the large negative shifts observed relative to the corresponding alkaline Earth metals, and the effect of lattice site disorder on the core level spectra and the presence or absence of intrinsic surface peaks.

  3. Core-level x-ray photoemission: Deviations from threshold behavior

    NASA Astrophysics Data System (ADS)

    Cox, D. L.; Frota, H. O.; Oliveira, L. N.; Wilkins, J. W.

    1985-07-01

    We present a systematic numerical study of core-level x-ray photoemission intensity in metals, with emphasis upon studying the deviations from behavior asymptotically close to threshold. For a model with a contact potential and linear conduction-electron dispersion, we have evaluated the photoemission intensity for core-hole phase shifts δ(0) between 0.05π and 0.5π. We find the following results. (i) The asymptotic regime extends out to 0.01 to 0.1 times the conduction bandwidth (D) from threshold. The range of the asymptotic regime decreases with increasing (absolute) phase shift. (ii) The linear relation between the integrated photoemission intensity and the asymptotic form holds for all phase shifts above ~0.1D. Due to our normalization procedure we cannot say whether it holds below this value. (iii) Discrepancies exist between numerical estimates of the deviations from asymptotic behavior and approximate analytic estimates. (iv) A definition of the frequency-dependent threshold singularity exponent α(ω) in terms of a moment of the photoemission intensity is stable out to the conduction-band edge and may prove useful to experimentalists attempting to extract exponents from their data.

  4. Spin polarization and magnetic dichroism in core-level photoemission from ferromagnets

    SciTech Connect

    Menchero, J G

    1997-05-01

    In this thesis we present a theoretical investigation of angle- and spin-resolved core-level photoemission from ferromagnetic Fe and Ni. We also consider magneto-dichroic effects due to reversal of the photon helicity or reversal of the sample magnetization direction. In chapter 1, we provide a brief outline of the history of photoemission, and show how it has played an important role in the development of modern physics. We then review the basic elements of the theory of core-level photoemission, and discuss the validity of the some of the commonly-used approximations. In chapter 2, we present a one-electron theory to calculate spin- and angle-resolved photoemission spectra for an arbitrary photon polarization. The Hamiltonian includes both spin-orbit and exchange interactions. As test cases for the theory, we calculate the spin polarization and magnetic dichroism for the Fe 2p core level, and find that agreement with experiment is very good.

  5. Spin-Orbit Effects in Spin-Resolved L2,3 Core Level Photoemission of 3d Ferromagnetic Thin Films

    SciTech Connect

    Komesu, T; Waddill, G D; Yu, S W; Butterfield, M; Tobin, J G

    2007-10-02

    We present spin-resolved 2p core level photoemission for the 3d transition metal films of Fe and Co grown on Cu(100). We observe clear spin asymmetry in the main 2p core level photoemission peaks of Fe and Co films consistent with trends in the bulk magnetic moments. The spin polarization can be strongly enhanced, by variation of the experimental geometry, when the photoemission is undertaken with circularly polarized light, indicating that spin-orbit interaction can have a profound in spin polarized photoemission. Further spin polarized photoemission studies using variable circularly polarized light at high photon energies, high flux are indicated, underscoring the value of synchrotron measurements at facilities with increased beam stability.

  6. Evidence of the nature of core-level photoemission satellites using angle-resolved photoemission extended fine structure

    SciTech Connect

    Moler, E.J.; Kellar, S.A.; Huff, W.R.A.

    1997-04-01

    The authors present a unique method of experimentally determining the angular momentum and intrinsic/extrinsic origin of core-level photoemission satellites by examining the satellite diffraction pattern in the Angle Resolved Photoemission Extended Fine Structure (ARPEFS) mode. They show for the first time that satellite peaks not associated with chemically differentiated atomic species display an ARPEFS intensity oscillation. They present ARPEFS data for the carbon 1s from ({radical}3x{radical}3)R30 CO/Cu(111) and p2mg(2xl)CO/Ni(110), nitrogen 1s from c(2x2) N{sub 2}/Ni(100), cobalt 1s from p(1x1)Co/Cu(100), and nickel 3p from clean nickel (111). The satellite peaks and tails of the Doniach-Sunjic line shapes in all cases exhibit ARPEFS curves which indicate an angular momentum identical to the main peak and are of an intrinsic nature.

  7. Angle-resolved photoemission extended fine structure of the Ni 3p, Cu 3s, and Cu 3p core levels of the respective clean (111) surfaces

    SciTech Connect

    Huff, W.R. |; Chen, Y.; Kellar, S.A.; Moler, E.J. |; Hussain, Z.; Huang, Z.Q.; Zheng, Y.; Shirley, D.A.

    1997-07-01

    We report a non-s initial-state angle-resolved photoemission extended fine-structure (ARPEFS) study of clean surfaces for the purpose of further understanding the technique. The surface structure sensitivity of ARPEFS applied to clean surfaces and to arbitrary initial states is studied using normal photoemission data taken from the Ni 3p core levels of a Ni(111) single crystal and the Cu 3s and the Cu 3p core levels of a Cu(111) single crystal. The Fourier transforms of these clean surface data are dominated by backscattering. Unlike the s initial-state data, the p initial-state data show a peak in the Fourier transform corresponding to in-plane scattering from the six nearest neighbors to the emitter. Evidence was seen for single-scattering events from the same plane as the emitters and double-scattering events. Using a recently developed, multiple-scattering calculation program, ARPEFS data from clean surfaces and from p initial states can be modeled to high precision. Although there are many layers of emitters when measuring photoemission from a clean surface, test calculations show that the ARPEFS signal is dominated by photoemission from atoms in the first two crystal layers. Thus ARPEFS applied to clean surfaces is sensitive to surface reconstruction. The best-fit calculation for clean Ni(111) indicates an expansion of the first two layers. {copyright} {ital 1997} {ital The American Physical Society}

  8. Detection of subsurface core-level shifts in Si 2p core-level photoemission from Si(111)-(1x1):As

    SciTech Connect

    Paggel, J.J.; Hasselblatt, M.; Horn, K.

    1997-04-01

    The (7 x 7) reconstruction of the Si(111) surface arises from a lowering energy through the reduction of the number of dangling bonds. This reconstruction can be removed by the adsorption of atoms such as hydrogen which saturate the dangling bonds, or by the incorporation of atoms, such as arsenic which, because of the additional electron it possesses, can form three bonds and a nonreactive lone pair orbital from the remaining two electrons. Core and valence level photoemission and ion scattering data have shown that the As atoms replace the top silicon atoms. Previous core level spectra were interpreted in terms of a bulk and a single surface doublet. The authors present results demonstrate that the core level spectrum contains two more lines. The authors assign these to subsurface silicon layers which also experience changes in the charge distribution when a silicon atom is replaced by an arsenic atom. Subsurface core level shifts are not unexpected since the modifications of the electronic structure and/or of photohole screening are likely to decay into the bulk and not just to affect the top-most substrate atoms. The detection of subsurface components suggests that the adsorption of arsenic leads to charge flow also in the second double layer of the Si(111) surface. In view of the difference in atomic radius between As and Si, it was suggested that the (1 x 1): As surface is strained. The presence of charge rearrangement up to the second double layer implies that the atomic coordinates also exhibit deviations from their ideal Si(111) counterparts, which might be detected through a LEED I/V or photoelectron diffraction analysis.

  9. Angle and temperature dependence of magnetic circular dichroism in core-level photoemission from Gd(0001)

    SciTech Connect

    Denecke, R.; Morais, J.; Ynzunza, R. X.; Menchero, J. G.; Liesegang, J.; Rice, M.; Kortright, J.; Hussain, Z.; Fadley, C. S.

    1997-04-01

    Magnetic dichroism in core-level photoelectron emission from solids represents a promising new element-specific probe of surface and interface atomic structure and magnetic order. One way of measuring such effects is by using photoelectrons excited by circular polarized radiation, thus leading to magnetic circular dichroism (MCD) if the intensity with right-circular polarized (RCP) light is not equal to that with left-circular polarized (LCP) light. The spin-integrated photoelectron intensity in a certain emission direction also in general depends on the direction of the magnetization in a magnetic material. In fact, if the magnetization lies in a surface mirror plane, then inverting its direction can provide a second way of measuring MCD. Purely atomic theoretical models have been successful in explaining many aspects of such data. By varying the emission direction one also probes the geometric structure of the sample. But such MCD in photoelectron angular distributions (MCDAD) then has to be interpreted also in terms of photoelectron diffraction. Measuring the temperature dependence of such MCD effects also provides a useful tool for studying magnetic transition temperatures. The authors have here studied such effects in core-level emission from Gd(0001).

  10. Photoemission core-level shifts reveal the thiolate-Au(111) interface

    SciTech Connect

    Groenbeck, Henrik; Odelius, Michael

    2010-08-15

    The nature of the thiolate/Au(111) interface is a long-standing puzzle. It has been suggested that thiolates drive surface reconstruction, however, a consensus regarding the adsorption configuration is missing. Herein, the density-functional theory is used to evaluate surface core-level shifts (SCLSs) for methyl thiolates on Au(111) assuming a representative set of different surface reconstructions. The SCLSs are found to provide sensitive fingerprints of the anchoring configuration, and it is only thiolate adsorption in the form of MeS-Au-SMe complexes that can be reconciled with experimental data.

  11. A photoemission study of the diamond and the single crystal C{sub 60}

    SciTech Connect

    Wu, Jin

    1994-03-01

    This report studied the elctronic structure of diamond (100) and diamond/metal interface and C{sub 60}, using angle-resolved and core level photoemission. The C(100)-(2X1) surface electronic structure was studied using both core level and angle resolved valence band photoemission spectroscopy. The surface component of the C 1s core level spectrum agrees with theoretical existence of only symmetrical dimers. In the case of metal/diamond interfaces, core level and valence photoelectron spectroscopy and LEED studies WERE MADE OF B and Sb on diamond (100) and (111) surfaces. In the case of single-crystal C{sub 60}, photoemission spectra show sharp molecular features, indicating that the molecular orbitals are relatively undisturbed in solid C{sub 60}.

  12. Study of Photoemissive Dusty Plasma

    SciTech Connect

    Gavrikov, A. V.; Fortov, V. E.; Petrov, O. F.; Babichev, V. N.; Filippov, A. V.; Pal', A. F.; Starostin, A. N.

    2008-09-07

    The present work deals with the experimental and theoretical investigation of photoemissive charging of polydisperse dust particles. The characteristic size of dust particles under consideration was 0.1-25 mkm. The experimental part of this work was devoted to the study of positive charging of macroparticles under UV-radiation that acted on dusty formations. Investigations were carried out in argon at normal pressure with particles of different materials. Dust structure was subjected to radiation. The power and frequency spectrum of this radiation was close to corresponding parameters of sun radiation near the top layers of Earth atmosphere. Owing to electron photoemission the macroparticles became positively charged. On the basis of experimental data the estimation of this charge was performed. It was about 500 elementary charges for micron particles. The theoretical part of present work included the numerical simulation of photoemissive dusty plasma decay in a drift-diffusion approximation. The model included equilibrium equation for positively charged macroparticles (in experiment, the percent of these particles was about 90), negatively charged dust particles (about 10%), positive ions (those were born by electron strike of buffered gas atoms) and electrons. Also the model included the Poisson equation for determination of potential distribution in the discharge region. The results of numerical calculations were in a satisfactory correspondence with experimental data both for time dependences of positively and negatively charged macroparticles concentrations and for their velocities.

  13. Photoemission studies of wurtzite zinc oxide.

    NASA Technical Reports Server (NTRS)

    Powell, R. A.; Spicer, W. E.; Mcmenamin, J. C.

    1972-01-01

    The electronic structure of wurtzite zinc oxide, investigated over the widest possible photon energy range by means of photoemission techniques, is described. Of particular interest among the results of the photoemission study are the location of the Zn 3rd core states, the width of the upper valence bands, and structure in the conduction-band and valence-band density of states.

  14. High-resolution core-level photoemission measurements on the pentacene single crystal surface assisted by photoconduction

    NASA Astrophysics Data System (ADS)

    Nakayama, Yasuo; Uragami, Yuki; Yamamoto, Masayuki; Yonezawa, Keiichirou; Mase, Kazuhiko; Kera, Satoshi; Ishii, Hisao; Ueno, Nobuo

    2016-03-01

    Upon charge carrier transport behaviors of high-mobility organic field effect transistors of pentacene single crystal, effects of ambient gases and resultant probable ‘impurities’ at the crystal surface have been controversial. Definite knowledge on the surface stoichiometry and chemical composites is indispensable to solve this question. In the present study, high-resolution x-ray photoelectron spectroscopy (XPS) measurements on the pentacene single crystal samples successfully demonstrated a presence of a few atomic-percent of (photo-)oxidized species at the first molecular layer of the crystal surface through accurate analyses of the excitation energy (i.e. probing depth) dependence of the C1s peak profiles. Particular methodologies to conduct XPS on organic single crystal samples, without any charging nor damage of the sample in spite of its electric insulating character and fragility against x-ray irradiation, is also described in detail.

  15. Photoemission studies of semiconductor nanocrystals

    SciTech Connect

    Hamad, K. S.; Roth, R.; Alivisatos, A. P.

    1997-04-01

    Semiconductor nanocrystals have been the focus of much attention in the last ten years due predominantly to their size dependent optical properties. Namely, the band gap of nanocrystals exhibits a shift to higher energy with decreasing size due to quantum confinement effects. Research in this field has employed primarily optical techniques to study nanocrystals, and in this respect this system has been investigated extensively. In addition, one is able to synthesize monodisperse, crystalline particles of CdS, CdSe, Si, InP, InAs, as well as CdS/HgS/CdS and CdSe/CdS composites. However, optical spectroscopies have proven ambiguous in determining the degree to which electronic excitations are interior or surface admixtures or giving a complete picture of the density of states. Photoemission is a useful technique for understanding the electronic structure of nanocrystals and the effects of quantum confinement, chemical environments of the nanocrystals, and surface coverages. Of particular interest to the authors is the surface composition and structure of these particles, for they have found that much of the behavior of nanocrystals is governed by their surface. Previously, the authors had performed x-ray photoelectron spectroscopy (XPS) on CdSe nanocrystals. XPS has proven to be a powerful tool in that it allows one to determine the composition of the nanocrystal surface.

  16. Hidden relationship between the electrical conductivity and the Mn 2p core-level photoemission spectra in La{sub 1-x}Sr{sub x}MnO{sub 3}

    SciTech Connect

    Hishida, T.; Ohbayashi, K.; Saitoh, T.

    2013-01-28

    Core-level electronic structure of La{sub 1-x}Sr{sub x}MnO{sub 3} has been studied by x-ray photoemission spectroscopy (XPS). We first report, by the conventional XPS, the well-screened shoulder structure in Mn 2p{sub 3/2} peak, which had been observed only by hard x-ray photoemission spectroscopy so far. Multiple-peak analysis revealed that the Mn{sup 4+} spectral weight was not proportional to the nominal hole concentration x, indicating that a simple Mn{sup 3+}/Mn{sup 4+} intensity ratio analysis may result in a wrong quantitative elemental analysis. Considerable weight of the shoulder at x = 0.0 and the fact that the shoulder weight was even slightly going down from x = 0.2 to 0.4 were not compatible with the idea that this weight simply represents the metallic behavior. Further analysis found that the whole Mn 2p{sub 3/2} peak can be decomposed into four portions, the Mn{sup 4+}, the (nominal) Mn{sup 3+}, the shoulder, and the other spectral weight located almost at the Mn{sup 3+} location. We concluded that this weight represents the well-screened final state at Mn{sup 4+} sites, whereas the shoulder is known as that of the Mn{sup 3+} states. We found that the sum of these two spectral weight has an empirical relationship to the conductivity evolution with x.

  17. Photoemission study of SmCo2

    NASA Astrophysics Data System (ADS)

    Kang, J.-S.; Yang, C. J.; Lee, Y. P.; Olson, C. G.; Cho, E.-J.; Oh, S.-J.; Anderson, R. O.; Liu, L. Z.; Park, J.-H.; Allen, J. W.; Ellis, W. P.

    1993-10-01

    The electronic structure of SmCo2 is investigated with photoemission spectroscopy (PES). All the PES spectra are consistent in showing that the bulk Sm ions are trivalent, but that the surface has divalent Sm ions and is probably inhomogeneously mixed valent. Both the Sm 4f valence band and Sm 3d core level PES spectra are found to be substantially broader than those of Sm metal. The observed larger linewidths for SmCo2, as compared to those of pure Sm metal, suggest a larger lifetime broadening, probably due to an increased number of valence-band electrons, and a larger 4f hybridization, mainly to Co 3d states. Weak satellite structures are observed in the Co 3d valence band and Co 2p core level PES spectra, indicating Co 3d correlation effects. The comparison of the experimental valence-band PES spectrum with the theoretical Co 3d projected local density of states also suggests that Co 3d correlation effects in SmCo2 are non-negligible.

  18. Photoemission study of the Cs$z.urule;GaP(110) interface at low temperatures

    NASA Astrophysics Data System (ADS)

    Chassé, Th.; Paggel, J.; Neuhold, G.; Theis, W.; Horn, K.

    1994-04-01

    The formation of the Cs⧸GaP(110) interface at low temperature has been studied using core and valence level photoemission. It is found that a nonmetallic first adsorption layer is followed by a transition to a metallic film. Valence level spectra show that Cs induces a new peak above the valence band maximum, which from the appearance of the core level spectra is assigned to adsorbate-substrate charge transfer. At higher coverages an intermediate species is identified on the basis of Cs 5p core level spectra. The metallic layer of Cs is characterised by metallic surface and bulk core level emission, the occurrence of plasmon satellites, and the emergence of a metallic Fermi edge. The relative separation of the different Cs core level line contributions are analysed through a Born-Haber cycle and qualitative arguments based on final state screening.

  19. HIGH RESOLUTION PHOTOEMISSION STUDIES OF COMPLEX MATERIALS.

    SciTech Connect

    JOHNSON,P.D.; VALLA,T.; FEDOROV,A.; REISFELD,G.; HULBERT,S.L.

    1999-10-13

    Recent instrumentation developments in photoemission are providing new insights into the physics of complex materials. With increased energy and momentum resolution, it has become possible to examine in detail different contributions to the self-energy or inverse lifetime of the photohole created in the photoexcitation process. Employing momentum distribution and energy distribution curves, a detailed study of the optimally doped cuprate, Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8+{delta}}, shows that the material behaves like a non-Fermi liquid with no evidence for the quasi-particles characteristic of a Fermi liquid.

  20. Photoemission studies of a clean and oxidized niobium-aluminum alloy using synchrotron radiation

    NASA Astrophysics Data System (ADS)

    Oshima, M.; Pate, B. B.; Lu, Z. M.; Jupiter, P. J.; Lindau, I.; Spicer, W. E.

    1983-06-01

    The alloy formation and oxidation of a Nb-rich Nb-Al alloy has been studied using core level photoemission in combination with synchroton radiation as a surface sensitive probe. Exactly the same chemical shifts were observed from both the Nb-Al alloy and an Al-evaporated Nb surface, indicating similar structural arrangements. It is found that the oxidation rate of Nb in these structures is drastically decreased in comparison to either pure Nb metal or Nb 3Sn. Two stages in the oxidation of the Nb-Al alloy are clearly distinguished by chemical shifts of the Al 2 p, Nb 4 p and O 2 p levels.

  1. Alkyl-terminated Si(111) surfaces: A high-resolution, core level photoelectron spectroscopy study

    SciTech Connect

    Terry, J.; Linford, M.R.; Wigren, C.; Cao, R.; Pianetta, P.; Chidsey, C.E.

    1999-01-01

    The bonding of alkyl monolayers to Si(111) surfaces has been studied with high-resolution core level photoelectron spectroscopy (PES). Two very different wet-chemical methods have been used to prepare the alkyl monolayers: (i) Olefin insertion into the H{endash}Si bond of the H{endash}Si(111) surface, and (ii) replacement of Cl on the Cl{endash}Si(111) surface by an alkyl group from an alkyllithium reagent. In both cases, PES has revealed a C 1s component shifted to lower binding energy and a Si 2p component shifted to higher binding energy. Both components are attributed to the presence of a C{endash}Si bond at the interface. Along with photoelectron diffraction data [Appl. Phys. Lett. {bold 71}, 1056, (1997)], these data are used to show that these two synthetic methods can be used to functionalize the Si(111) surface. {copyright} {ital 1999 American Institute of Physics.}

  2. Structural origin of Si-2p core-level shifts from Si(100)-c[4x2] surface: A spectral x-ray photoelectron diffraction study

    SciTech Connect

    Chen, X.; Tonner, B.P.; Denlinger, J.

    1997-04-01

    The authors have performed angle-resolved x-ray photoelectron diffraction (XPD) from a Si(100)-c(4x2) surface to study the structural origin of Si-2p core-level shifts. In the experiment, the highly resolved surface Si-2p core-level spectra were measured as a fine grid of hemisphere and photon energies, using the SpectroMicroscopy Facility {open_quotes}ultraESCA{close_quotes} instrument. By carefully decomposing the spectra into several surface peaks, the authors are able to obtain surface-atom resolved XPD patterns. Using a multiple scattering analysis, they derived a detailed atomic model for the Si(100)-c(4x2) surface. In this model, the asymmetric dimers were found tilted by 11.5 plus/minus 2.0 degrees with bond length of 2.32 plus/minus 0.05{angstrom}. By matching model XPD patterns to experiment, the authors can identify which atoms in the reconstructed surface are responsible for specific photoemission lines in the 2p spectrum.

  3. A first-principles core-level XPS study on the boron impurities in germanium crystal

    SciTech Connect

    Yamauchi, Jun; Yoshimoto, Yoshihide; Suwa, Yuji

    2013-12-04

    We systematically investigated the x-ray photoelectron spectroscopy (XPS) core-level shifts and formation energies of boron defects in germanium crystals and compared the results to those in silicon crystals. Both for XPS core-level shifts and formation energies, relationship between defects in Si and Ge is roughly linear. From the similarity in the formation energy, it is expected that the exotic clusters like icosahedral B12 exist in Ge as well as in Si.

  4. Magneto-optical and photoemission studies of ultrathin wedges

    SciTech Connect

    Bader, S.D.; Li, Dongqi

    1995-12-01

    Magnetic phase transitions of Fe wedges grown epitaxially on Cu(100) are detected via the surface magneto-optical Kerr effect and used to construct a phase diagram for face centered Fe. Also, the confinement of Cu sp- and d-quantum-well states is studied for Cu/Co(wedge)/Cu(100) utilizing undulator-based photoemission experiments.

  5. Fingerprints of the hydrogen bond in the photoemission spectra of croconic acid condensed phase: An x-ray photoelectron spectroscopy and ab-initio study

    SciTech Connect

    Bisti, F.; Stroppa, A.; Picozzi, S.; Ottaviano, L.

    2011-05-07

    The electronic structure of Croconic Acid in the condensed phase has been studied by comparing core level and valence band x-ray photoelectron spectroscopy experiments and first principles density functional theory calculations using the Heyd-Scuseria-Ernzerhof screened hybrid functional and the GW approximation. By exploring the photoemission spectra for different deposition thicknesses, we show how the formation of the hydrogen bond network modifies the O 1s core level lineshape. Moreover, the valence band can be explained only if the intermolecular interactions are taken into account in the theoretical approach.

  6. Photoemission Study of the Rare Earth Intermetallic Compounds: RNi2Ge2 (R=Eu, Gd)

    SciTech Connect

    Jongik Park

    2004-12-19

    EuNi{sub 2}Ge{sub 2} and GdNi{sub 2}Ge{sub 2} are two members of the RT{sub 2}X{sub 2} (R = rare earth, T = transition metal and X = Si, Ge) family of intermetallic compounds, which has been studied since the early 1980s. These ternary rare-earth intermetallic compounds with the tetragonal ThCr{sub 2}Si{sub 2} structure are known for their wide variety of magnetic properties, Extensive studies of the RT{sub 2}X{sub 2} series can be found in Refs [ 1,2,3]. The magnetic properties of the rare-earth nickel germanides RNi{sub 2}Ge{sub 2} were recently studied in more detail [4]. The purpose of this dissertation is to investigate the electronic structure (both valence band and shallow core levels) of single crystals of EuNi{sub 2}Ge{sub 2} and GdNi{sub 2}Ge{sub 2} and to check the assumptions that the f electrons are non-interacting and, consequently, the rigid-band model for these crystals would work [11], using synchrotron radiation because, to the best of our knowledge, no photoemission measurements on those have been reported. Photoemission spectroscopy has been widely used to study the detailed electronic structure of metals and alloys, and especially angle-resolved photoemission spectroscopy (ARPES) has proven to be a powerful technique for investigating Fermi surfaces (FSs) of single-crystal compounds.

  7. Near-field focused photoemission from polystyrene microspheres studied with photoemission electron microscopy

    SciTech Connect

    Peppernick, Samuel J.; Joly, Alan G.; Beck, Kenneth M.; Hess, Wayne P.

    2012-07-07

    We use photoemission electron microscopy(PEEM) to image 3 μm diameter polystyrene spheres supported on a metalthin film illuminated by 400 nm (~3.1 eV) and 800 nm (~1.5 eV) femtosecond (fs) laser pulses. Intense photoemission is generated by microspheres even though polystyrene is an insulator and its ionization threshold is well above the photon energies employed. We observe intense photoemission from the far side (the side opposite the incident light) of the illuminated microsphere that is attributed to light focusing within the microsphere. For the case of p-polarized, 800 nm fs laser pulses, we observe photoemission exclusively from the far side of the microsphere and additionally resolve sub-50 nm hot spots in the supporting Pt/Pd thin film that are located only within the focal region of the microsphere. We compare the PEEM images with finite difference time domain(FDTD) electrodynamic simulations to model our experimental results. Finally, the FDTD simulations predict light focusing in the microsphere and subsequent interaction with the supporting metal surface that is consistent with the experimental observations.

  8. Spin polarized photoemission studies of interfacial and thin film magnetism

    SciTech Connect

    Johnson, P.D.; Brookes, N.B.; Chang, Y.; Garrison, K.

    1993-01-01

    Spin polarized photoemission is used to study the electronic structure of noble metals deposited on ferromagnetic substrates. Studies of Ag deposited on an Fe(001) substrate reveal a series of minority spin interface or quantum well states with binding energies dependent on the thickness of the silver. Similar behavior is observed for Cu films deposited on a fct Co(001) substrate. Tight-binding modeling reproduces many of the observations and shows that hybridization of the sp-bands with the noble metal d-bands cannot be ignored.

  9. Spin polarized photoemission studies of interfacial and thin film magnetism

    SciTech Connect

    Johnson, P.D.; Brookes, N.B.; Chang, Y.; Garrison, K.

    1993-06-01

    Spin polarized photoemission is used to study the electronic structure of noble metals deposited on ferromagnetic substrates. Studies of Ag deposited on an Fe(001) substrate reveal a series of minority spin interface or quantum well states with binding energies dependent on the thickness of the silver. Similar behavior is observed for Cu films deposited on a fct Co(001) substrate. Tight-binding modeling reproduces many of the observations and shows that hybridization of the sp-bands with the noble metal d-bands cannot be ignored.

  10. Comparative Photoemission Study of Actinide (Am, Pu, Np and U) Metals, Nitrides, and Hydrides

    SciTech Connect

    Gouder, Thomas; Seibert, Alice; Rebizant, Jean; Huber, Frank; Havela, Ladislav

    2007-07-01

    Core-level and valence-band spectra of Pu and the other early actinide compounds show remarkable systematics, which can be understood in the framework of final state screening. We compare the early actinide (U, Np, Pu and Am) metals, nitrides and hydrides and a few other specific compounds (PuSe, PuS, PuCx, PuSix) prepared as thin films by sputter deposition. In choosing these systems, we combine inherent 5f band narrowing, due to 5f orbital contraction throughout the actinide series, with variations of the chemical environment in the compounds. Goal of this work was to learn more on the electronic structure of the early actinide systems and to achieve the correct interpretation of their photoemission spectra. The highly correlated nature of the 5f states in systems, which are on the verge to localization, makes this a challenging task, because of the peculiar interplay between ground state DOS and final-state effects. Their influence can be estimated by doing systematic studies on systems with different (5f) bandwidths. We conclude on the basis of such systematic experiments that final-state effects due to strong e-e correlations in narrow 5f-band systems lead to multiplet like structures, analogous to those observed in the case of systems with localized electron states. Such observations in essentially band-like 5f-systems was first surprising, but the astonishing similarity of photoemission spectra of very different chemical systems (e.g. PuSe, Pu{sub 2}C{sub 3}..) points to a common origin, relating them to atomic features rather than material dependent density of states (DOS) features. (authors)

  11. Core-level photoabsorption study of defects and metastable bonding configurations in boron nitride

    SciTech Connect

    Jimenez, I.; Jankowski, A.F.; Terminello, L.J.

    1997-04-01

    Boron nitride is an interesting material for technological applications and for fundamental solid state physics investigations. It is a compound isoelectronic with carbon and, like carbon can possess sp{sup 2} and sp{sup 3} bonded phases resembling graphite and diamond. BN crystallizes in the sp{sup 2}-bonded hexagonal (h-BN), rhombohedral (r-BN) and turbostratic phases, and in the sp{sup 3}-bonded cubic (c-BN) and wurtzite (w-BN) phases. A new family of materials is obtained when replacing C-C pairs in graphite with isoelectronic B-N pairs, resulting in C{sub 2}BN compounds. Regarding other boron compounds, BN is exceptional in the sense that it has standard two-center bonds with conventional coordination numbers, while other boron compounds (e.g. B{sub 4}C) are based on the boron icosahedron unit with three-center bonds and high coordination numbers. The existence of several allotropic forms and fullerene-like structures for BN suggests a rich variety of local bonding and poses the questions of how this affects the local electronic structure and how the material accommodates the stress induced in the transition regions between different phases. One would expect point defects to play a crucial role in stress accommodation, but these must also have a strong influence in the electronic structure, since the B-N bond is polar and a point defect will thus be a charged structure. The study of point defects in relationship to the electronic structure is of fundamental interest in these materials. Recently, the authors have shown that Near-Edge X-ray Absorption Fine Structure (NEXAFS) is sensitive to point defects in h-BN, and to the formation of metastable phases even in amorphous materials. This is significant since other phase identification techniques like vibrational spectroscopies or x-ray diffraction yield ambiguous results for nanocrystalline and amorphous samples. Serendipitously, NEXAFS also combines chemical selectivity with point defect sensitivity.

  12. Preparation of clean InP(100) surfaces studied by synchrotron radiation photoemission

    NASA Astrophysics Data System (ADS)

    Sun, Yun; Liu, Zhi; Machuca, Francisco; Pianetta, Piero; Spicer, William E.

    2003-01-01

    The chemical cleaning of indium phosphide (InP),(100) surfaces is studied systematically by using photoemission electron spectroscopy. In order to achieve the necessary surface sensitivity and spectral resolution, synchrotron radiation with photon energies ranging from 60 to 600 eV are used to study the indium 4d, phosphorus 2p, carbon 1s, and oxygen 1s core levels, and the valence band. Typical H2SO4:H2O2:H2O solutions used to etch GaAs(100) surfaces are applied to InP(100) surfaces. It is found that the resulting surface species are significantly different from those found on GaAs(100) surfaces and that a second chemical cleaning step using a strong acid is required to remove residual surface oxide. This two-step cleaning process leaves the surface oxide free and with approximately 0.4 ML of elemental phosphorus, which is removed by vacuum annealing. The carbon coverage is also reduced dramatically from approximately 1 to about 0.05 ML. The chemical reactions are investigated, the resulting InP surface species at different cleaning stages are determined, and the optimum cleaning procedure is presented.

  13. Band Structure of SnTe Studied by Photoemission Spectroscopy

    NASA Astrophysics Data System (ADS)

    Littlewood, P. B.; Mihaila, B.; Schulze, R. K.; Safarik, D. J.; Gubernatis, J. E.; Bostwick, A.; Rotenberg, E.; Opeil, C. P.; Durakiewicz, T.; Smith, J. L.; Lashley, J. C.

    2010-08-01

    We present an angle-resolved photoemission spectroscopy study of the electronic structure of SnTe and compare the experimental results to ab initio band structure calculations as well as a simplified tight-binding model of the p bands. Our study reveals the conjectured complex Fermi surface structure near the L points showing topological changes in the bands from disconnected pockets, to open tubes, and then to cuboids as the binding energy increases, resolving lingering issues about the electronic structure. The chemical potential at the crystal surface is found to be 0.5 eV below the gap, corresponding to a carrier density of p=1.14×1021cm-3 or 7.2×10-2 holes per unit cell. At a temperature below the cubic-rhombohedral structural transition a small shift in spectral energy of the valance band is found, in agreement with model predictions.

  14. Band structure of SnTe studied by photoemission spectroscopy.

    PubMed

    Littlewood, P B; Mihaila, B; Schulze, R K; Safarik, D J; Gubernatis, J E; Bostwick, A; Rotenberg, E; Opeil, C P; Durakiewicz, T; Smith, J L; Lashley, J C

    2010-08-20

    We present an angle-resolved photoemission spectroscopy study of the electronic structure of SnTe and compare the experimental results to ab initio band structure calculations as well as a simplified tight-binding model of the p bands. Our study reveals the conjectured complex Fermi surface structure near the L points showing topological changes in the bands from disconnected pockets, to open tubes, and then to cuboids as the binding energy increases, resolving lingering issues about the electronic structure. The chemical potential at the crystal surface is found to be 0.5 eV below the gap, corresponding to a carrier density of p=1.14 × 10(21)  cm(-3) or 7.2 × 10(-2) holes per unit cell. At a temperature below the cubic-rhombohedral structural transition a small shift in spectral energy of the valance band is found, in agreement with model predictions. PMID:20868120

  15. Angle-resolved photoemission study of Ag(1 1 1)

    NASA Astrophysics Data System (ADS)

    Edamoto, K.; Miyazaki, E.; Shimokoshi, K.; Kato, H.

    1990-01-01

    The (1 1 1) face of Ag has been studied by angle-resolved photoemission spectroscopy utilizing synchrotron radiation as the excitation source (25 <= hv <= 50eV). The overlapping Ag 4d bands were deconvolved by the modified FIRO method. The peak positions thus determined are used to map the dispersion curves along the lang1 1 1rang (Γ-L) direction. The results show general agreement with calculated band structure, so far as the energy levels and symmetries are concerned. However, it is found that the density of state effect is dominant in the spectra obtained in the present photon energy region. The emission from the Ag 5s, p bands is observed to be broadened due to the indirect transition process.

  16. Photoemission optogalvanic studies with copper as target electrode

    NASA Astrophysics Data System (ADS)

    Ajithprasad, K. C.; Nampoori, V. P. N.; Vallabhan, C. P. G.

    1996-12-01

    Photoemission optogalvanaic (POG) effect has been observed by irradiating copper target electrode, in a nitrogen discharge cell using 1.06 μm and frequency doubled 532 nm Nd:YAG laser pulse. Measurement of the nature of the variation of POG signal strength with 532 nm laser fluence confirms the two photon induced photoelectric emission from copper. However, using 1.06 μm laser pulses thermally assisted photoemission is observed.

  17. Photoemission and magnetic circular dichroism studies of magnetic semiconductors

    NASA Astrophysics Data System (ADS)

    Fujimori, Atsushi

    2005-03-01

    Recently, a series of novel ferromagnetic semiconductors have been synthesized using MBE and related techniques and have attracted much attention because of unknown mechanisms of carrier-induced ferromagnetism and potential applications as "spin electronics" devices. Some new materials show ferromagnetism even well above room temperature. Photoemission spectroscopy has been used to study the d orbitals of the dilute transition-metal atoms, mostly Mn, and their hybridization with the host band states [1]. Soft x-ray absorption spectroscopy (XAS) and magnetic circular dichroism (MCD) at the transition-metal 2p-3d absorption edges are useful techniques to study the valence and spin states of the transition-metal atoms. Furthermore, since MCD has different sensitivities to the ferromagnetic and paramagnetic components at different temperatures and magnetic fileds, if the sample is a mixture of ferromagnetic and non-ferromagnetic transition- metal atoms, it can be used to separate the two components and to study their electronic structures. In this talk, results are presented for the prototypical diluted ferromagnetic semiconductor Ga1-xMnxAs [2] and the room-temperature ferromagnets Zn1-xCoxO and Ti1-xCoxO2.I acknowledge collaboration with Y. Ishida, J.-I. Hwang, M. Kobayashi, Y. Takeda, Y. Saitoh, J. Okamoto, T. Okane, Y. Muramatsu, K. Mamiya, T. Koide, A. Tanaka, M. Tanaka, Hayashi, S. Ohya, T. Kondo, H. Munekata, H. Saeki, H. Tabata, T. Kawai, Y. Matsumoto, H. Koinuma, T. Fukumura and M. Kawasaki. This work was supported by a Grant-in-Aid for Scientific Research in Priority Area "Semiconductor nano-spintronics" (14076209) from MEXT, Japan.1. J. Okabayashi et al., Phys. Rev. B 64, 125304 (2001).2. A. Fujimori et al., J. Electron Spectrosc. Relat. Phenom., in press.

  18. Surface Optimization of RBa2Cu3O7-δ (R=Y, Nd) Epitaxial High Tc Films for In Situ Photoemission Studies

    NASA Astrophysics Data System (ADS)

    Abrecht, M.; Schmauder, T.; Ariosa, D.; Touzelet, O.; Rast, S.; Onellion, M.; Pavuna, D.

    One of the intrinsic difficulties for in situ photoemission studies of high Tc oxide films is the surface volatility, especially the oxygen loss. In order to solve this problem, we have constructed a dedicated system for high Tc film surface studies, in particular for ARPES measurements. Here we briefly describe our pulsed laser deposition (PLD) system that is linked to the photoemission chamber at the Synchrotron Radiation Center (SRC) in Wisconsin, and discuss crystallographic and electronic properties measured on epitaxial YBa2Cu3O7-δ (YBCO) and NdBa2Cu3O7-δ (NBCO) films. Resistivity and XRD studies show that the best c axis epitaxial films, with Tc (onset)=92 K (Tc0=90.5 K), are monophase and single crystalline with crystal coherence up to almost 1 µm. Initial core level photoemission study indicates that, for YBCO on SrTiO3 (without any buffer layer), the Ba oxide layer tends to be the dominant surface layer. Further experiments are underway to reproducibly detect sharp Fermi edge and perform ARPES study on optimally doped film surfaces.

  19. Angle-resolved photoemission spectroscopy (ARPES) studies of cuprate superconductors

    SciTech Connect

    Palczewski, Ari Deibert

    2010-01-01

    This dissertation is comprised of three different angle-resolved photoemission spectroscopy (ARPES) studies on cuprate superconductors. The first study compares the band structure from two different single layer cuprates Tl2Ba2CuO6+δ (Tl2201) Tc, max ≈ 95 K and (Bi 1.35Pb0.85)(Sr1.47La0.38)CuO6+δ (Bi2201) Tc, max ≈ 35 K. The aim of the study was to provide some insight into the reasons why single layer cuprate's maximum transition temperatures are so different. The study found two major differences in the band structure. First, the Fermi surface segments close to (π,0) are more parallel in Tl2201 than in Bi2201. Second, the shadow band usually related to crystal structure is only present in Bi2201, but absent in higher Tc Tl2201. The second study looks at the different ways of doping Bi2Sr2CaCu2O8+δ (Bi2212) in-situ by only changing the post bake-out vacuum conditions and temperature. The aim of the study is to systematically look into the generally overlooked experimental conditions that change the doping of a cleaved sample in ultra high vacuum (UHV) experiments. The study found two major experimental facts. First, in inadequate UHV conditions the carrier concentration of Bi2212 increases with time, due to the absorption of oxygen from CO2/CO molecules, prime contaminants present in UHV systems. Second, in a very clean UHV system at elevated temperatures (above about 200 K), the carrier concentration decreases due to the loss of oxygen atoms from the Bi-O layer. The final study probed the particle-hole symmetry of the pseudogap phase in high temperature superconducting cuprates by looking at the thermally excited bands above the Fermi level. The data showed a particle-hole symmetric pseudogap which symmetrically closes away from the nested FS before the node. The data is consistent

  20. Soft X-ray photoemission studies of Hf oxidation

    SciTech Connect

    Suzer, S.; Sayan, S.; Banaszak Holl, M.M.; Garfunkel, E.; Hussain, Z.; Hamdan, N.M.

    2002-02-01

    Soft X-Ray Photoemission Spectroscopy using surface sensitive Synchrotron Radiation has been applied to accurately determine the binding energy shifts and the valence band offset of the HfO2 grown on Hf metal. Charging of oxide films under x-rays (or other irradiation) is circumvented by controlled and sequential in-situ oxidation. Photoemission results show the presence of metallic Hf (from the substrate) with the 4f7/2 binding energy of 14.22 eV, fully oxidized Hf (from HfO2) with the 4f7/2 binding energy of 18.16 eV, and at least one clear suboxide peak. The position of the valence band of HfO2 with respect to the Hf(m) Fermi level is determined as 4.05 eV.

  1. On sulfur core level binding energies in thiol self-assembly and alternative adsorption sites: An experimental and theoretical study

    SciTech Connect

    Jia, Juanjuan; Kara, Abdelkader E-mail: vladimir.esaulov@u-psud.fr; Pasquali, Luca; Bendounan, Azzedine; Sirotti, Fausto; Esaulov, Vladimir A. E-mail: vladimir.esaulov@u-psud.fr

    2015-09-14

    Characteristic core level binding energies (CLBEs) are regularly used to infer the modes of molecular adsorption: orientation, organization, and dissociation processes. Here, we focus on a largely debated situation regarding CLBEs in the case of chalcogen atom bearing molecules. For a thiol, this concerns the case when the CLBE of a thiolate sulfur at an adsorption site can be interpreted alternatively as due to atomic adsorption of a S atom, resulting from dissociation. Results of an investigation of the characteristics of thiol self-assembled monolayers (SAMs) obtained by vacuum evaporative adsorption are presented along with core level binding energy calculations. Thiol ended SAMs of 1,4-benzenedimethanethiol (BDMT) obtained by evaporation on Au display an unconventional CLBE structure at about 161.25 eV, which is close to a known CLBE of a S atom on Au. Adsorption and CLBE calculations for sulfur atoms and BDMT molecules are reported and allow delineating trends as a function of chemisorption on hollow, bridge, and atop sites and including the presence of adatoms. These calculations suggest that the 161.25 eV peak is due to an alternative adsorption site, which could be associated to an atop configuration. Therefore, this may be an alternative interpretation, different from the one involving the adsorption of atomic sulfur resulting from the dissociation process of the S–C bond. Calculated differences in S(2p) CLBEs for free BDMT molecules, SH group sulfur on top of the SAM, and disulfide are also reported to clarify possible errors in assignments.

  2. Photoemission spectroscopy studies of new topological insulator materials

    NASA Astrophysics Data System (ADS)

    Weber, Andrew Patton

    As the size of a solid shrinks, the ratio of surface area to bulk volume grows and surface effects become more important. In a world where technologies advance with the shrinking size of electronic devices, one phase of matter has emerged which is fit for the near future of surface-dominated performance. Moreover, it has brought a new set of ideas to solid-state physics and chemistry, especially the understanding that the discipline of topology can be applied to classify the electron band structures. The topological insulator phase yields an exotic metal surface state in which the orientation of the electron's spin is locked perpendicular to its momentum. This property suppresses backscattering (making it possible to pass spin-polarized currents through the material without loss), offers a crucial ingredient for innovative approaches to quantum computation, and provides the basis for observing unique magnetoelectric effects. However, the surface states of materials in the topological insulator phase can wildly differ, so it is of interest to systematically characterize new materials to understand how the structure in position-space is related to the spin-resolved structure of electrons in energy- and momentum-space. We will discuss this relationship as it is probed through spin- and angle-resolved photoemission spectroscopy experiments on three topological (Bi2)m(Bi2Se3)n superlattices: (a) Bi2Se3 (m = 0, n = 1), (b) Bi4Se3 (m = 1, n = 1), and (c) BiSe (m = 1, n = 2). Our studies have not only proven the topological nature of these materials, but also demonstrate how bulk band structure and polar chemical bonding control the surface metal's concentration, dispersion, and spin-orbital character. Case (a) is considered to provide an ideal model of the topological surface metal. Case (b) provides the three important findings: (1) the chemical identity of the surface-termination controls the orbital composition and energy distribution of the surface states, (2) there

  3. A photoemission study of Pd ultrathin films on Pt(111)

    SciTech Connect

    Mun, Bongjin Simon; Lee, Choongman; Stamenkovic, Vojislav; Markovic, Nenad M.; Ross Jr., Philip N.

    2005-05-11

    The origin of surface core-level shift (SCLS) of Pd thin films on Pt(111) substrate is investigated. At sub-monolayer coverage of Pd thin films, the splitting of Pd 3d core level peaks indicate the contribution of both initial and final-state of photo-ionization processes while there is almost no change on valence band (VB) spectra. When the coverage of Pd reaches to single monolayer, the final-state relaxation effect on the Pd 3d vanishes and only the initial-state effect, a negative SCLS, is present. Also, the VB spectrum at Pd monolayer films shows a clear band narrowing, that is the origin of the negative SCLS at monolayer coverage. As the Pd coverage is increased to more than monolayer thickness, the Pd 3d peaks start to show the surface layer contribution from second and third layers, positive SCLS, and the VB spectrum shows even narrower band width, possibly due to the formation of surface states and strained effect of Pd adlayers on top of the first pseudomorphic layer.

  4. High-resolution photoemission study of MgB2.

    PubMed

    Takahashi, T; Sato, T; Souma, S; Muranaka, T; Akimitsu, J

    2001-05-21

    We have performed high-resolution photoemission spectroscopy on MgB2 and observed opening of a superconducting gap with a narrow coherent peak. We found that the superconducting gap is s like with the gap value ( Delta) of 4.5+/-0.3 meV at 15 K. The temperature dependence (15-40 K) of the gap value follows well the BCS form, suggesting that 2Delta/k(B)T(c) at T = 0 is about 3. No pseudogap behavior is observed in the normal state. The present results strongly suggest that MgB2 is categorized into a phonon-mediated BCS superconductor in the weak-coupling regime.

  5. Soft-x-ray resonant-photoemission study of mixed-valence TmSe

    NASA Astrophysics Data System (ADS)

    Oh, S.-J.; Allen, J. W.; Lindau, I.

    1984-08-01

    A single crystal of mixed-valence TmSe was studied by a resonant-photoemission technique with use of synchrotron radiation in the soft-x-ray region (hν=70-200 eV). The two Tm 4f emissions, one corresponding to the divalent Tm ion (4f13-->4f12) and the other to the trivalent Tm ion (4f12-->4f11), are both resonantly enhanced at photon energies close to the Tm 4d binding energy (170 to 180 eV), but their resonance behaviors differ from each other in that the former structure follows the multiplet structure of the 4d94f14 intermediate-state configuration whereas the latter shows multiplets of the 4d94f13 configuration. This can serve as a direct spectroscopic identification of the 4f occupation number of each component of the 4f emissions. Because the correlation energies between Tm 4d and 4f electrons and those between two 4f electrons are similar, these resonance thresholds come at about the same energy for both configurations. The bulk-sensitive constant-final-state (CFS) spectra show a superposition of both resonance features, confirming bulk mixed valency of TmSe. The bulk valence deduced from this CFS measurement is 2.62+/-0.15. The Tm 5p core-level emissions show two sets of spin-orbit peaks corresponding to two different Tm valences, and they also resonate in the same way as 4f emissions. The apparent spin-orbit splittings between 5p12 and 5p32 peaks differ by 1.4 eV for two Tm valences, most probably because of the exchange interaction between the 5p hole and 4f electrons. The variation of the relative intensity of the divalent peak to the trivalent peak as a function of photon energy clearly supports the existence of divalent surface layer(s), as recently reported. The electron escape depth has been calculated from this intensity ratio, and the results are compared with various theoretical models.

  6. Pulsed laser deposition for in-situ photoemission studies on YBa2Cu3O7-δ and related oxide films

    NASA Astrophysics Data System (ADS)

    Schmauder, T.; Frazer, B.; Gatt, R.; Xi, Xiaoxing; Onellion, Marshall; Ariosa, Daniel; Grioni, M.; Margaritondo, Giorgio; Pavuna, Davor

    1998-12-01

    We describe a new pled laser deposition (PLD) system that is linked to an angle-resolved photoemission (ARPES) chamber at the Synchrotron Radiation Center (SRC) in Wisconsin, USA. We also discuss our first results on epitaxially grown YBa2Cu3O7-(delta ) (YBCO) films. The core level photoemission data indicate that a Ba-oxide layer is the dominant surface layer. We were not able to reproducibly detect a sharp fermi edge in the photoemission spectra and thus conclude that the surface layer is non-metallic, probably due to oxygen loss at the surface. The absence of screening of the Y and Ba core levels is a further argument for this conclusion. Further experiments with ozone treated film surfaces are currently under way.

  7. GaAs clean up studied with synchrotron radiation photoemission

    NASA Astrophysics Data System (ADS)

    Tallarida, Massimo; Adelmann, Christoph; Delabie, Annelies; van Elshocht, Sven; Caymax, Matty; Schmeisser, Dieter

    2012-12-01

    In this contribution we describe the chemical changes at the surface of GaAs upon adsorption of tri-methyl-aluminum (TMA). TMA is used to grow Al2O3 with atomic layer deposition (ALD) usually using H2O as oxygen source. Recently, it was pointed out that the adsorption of TMA on various III-V surfaces reduces the native oxide, allowing the growth of an abrupt III-V/High-K interface with reduced density of defects. Synchrotron radiation photoemission spectroscopy (SR-PES) is a powerful method to characterize surfaces and interfaces of many materials, as it is capable to determine their chemical composition as well as the electronic properties. We performed in-situ SR-PES measurements after exposing a GaAs surface to TMA pulses at about 250°C. Upon using the possibility of tuning the incident photon energy we compared the Ga3d spectra at 41 eV, 71 eV, 91 eV and 121 eV, as well as the As3d at 71 eV and 91 eV. Finally, we show that using SR-PES allows a further understanding of the surface composition, which is usually not accessible with other techniques.

  8. Angle-resolved photoemission study of thin molecular-beam-epitaxy-grown α-Sn1-xGex films with x~0.5

    NASA Astrophysics Data System (ADS)

    Höchst, Hartmut; Engelhardt, Michael A.; Hernández-Calderón, Isaac

    1989-11-01

    Angle-resolved synchrotron-radiation photoemission spectroscopy is used to study the electronic structure of metastable epitaxial films of α-Sn1-xGex alloys. Homogeneous crystalline alloy films were grown by molecular-beam epitaxy on Ge(100) substrates at ~400 °C up to a thickness of ~300 Å. Photoemission core-level analysis indicates a strong tendency to form a compound with a composition close to x~0.5. Angle-resolved spectra show a shift of the Γ8 valence band from ~0.6 eV in Ge(100) to ~0.16 eV below EF in the α-Sn0.48Ge0.52 alloy. The experimental information of a constant alloy Fermi level locates the top of the Γ8 valence band ~0.16 eV below EF. Assuming a linear band model, the direct band gap of Eg~0.2 eV for x~0.5 will then locate the bottom of the Γ7 conduction band ~0.04 eV above EF.

  9. Dopamine adsorption on anatase TiO2(101): a photoemission and NEXAFS spectroscopy study.

    PubMed

    Syres, K; Thomas, A; Bondino, F; Malvestuto, M; Grätzel, M

    2010-09-21

    The adsorption of dopamine onto an anatase TiO(2)(101) single crystal has been studied using photoemission and NEXAFS techniques. Photoemission results suggest that the dopamine molecule adsorbs on the surface in a bidentate geometry, resulting in the removal of band gap states in the TiO(2) valence band. Using the searchlight effect, carbon K-edge NEXAFS spectra indicate that the phenyl rings in the dopamine molecules are orientated normal to the surface. A combination of experimental and computational results indicates the appearance of new unoccupied states arising following adsorption. The possible role of these states in the charge-transfer mechanism of the dopamine-TiO(2) system is discussed.

  10. Dopamine adsorption on anatase TiO2(101): a photoemission and NEXAFS spectroscopy study.

    PubMed

    Syres, K; Thomas, A; Bondino, F; Malvestuto, M; Grätzel, M

    2010-09-21

    The adsorption of dopamine onto an anatase TiO(2)(101) single crystal has been studied using photoemission and NEXAFS techniques. Photoemission results suggest that the dopamine molecule adsorbs on the surface in a bidentate geometry, resulting in the removal of band gap states in the TiO(2) valence band. Using the searchlight effect, carbon K-edge NEXAFS spectra indicate that the phenyl rings in the dopamine molecules are orientated normal to the surface. A combination of experimental and computational results indicates the appearance of new unoccupied states arising following adsorption. The possible role of these states in the charge-transfer mechanism of the dopamine-TiO(2) system is discussed. PMID:20735026

  11. Nitrogen Doping and Thermal Stability in HfSiOxNy Studied by Photoemission and X-ray Absorption Spectroscopy

    SciTech Connect

    Toyoda, Satoshi; Okabayashi, Jun; Takahashi, Haruhiko; Oshima, Masaharu; Lee, Dong-Ick; Sun, Shiyu; sun, Steven; Pianetta, Piero A.; Ando, Takashi; Fukuda, Seiichi; /SONY, Atsugi

    2005-12-14

    We have investigated nitrogen-doping effects into HfSiO{sub x} films on Si and their thermal stability using synchrotron-radiation photoemission and x-ray absorption spectroscopy. N 1s core-level photoemission and N K-edge absorption spectra have revealed that chemical-bonding states of N-Si{sub 3-x}O{sub x} and interstitial N{sub 2}-gas-like features are clearly observed in as-grown HfSiO{sub x}N{sub y} film and they decrease upon ultrahigh vacuum (UHV) annealing due to a thermal instability, which can be related to the device performance. Annealing-temperature dependence in Hf 4f and Si 2p photoemission spectra suggests that the Hf-silicidation temperature is effectively increased by nitrogen doping into the HfSiO{sub x} although the interfacial SiO{sub 2} layer is selectively reduced. No change in valence-band spectra upon UHV annealing suggests that crystallization of the HfSiO{sub x}N{sub y} films is also hindered by nitrogen doping into the HfSiO{sub x}.

  12. Electronic properties of atomic layer deposition films, anatase and rutile TiO2 studied by resonant photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Das, C.; Richter, M.; Tallarida, M.; Schmeisser, D.

    2016-07-01

    The TiO2 films are prepared by atomic layer deposition (ALD) method using titanium isopropoxide precursors at 250 °C and analyzed using resonant photoemission spectroscopy (resPES). We report on the Ti2p and O1s core levels, on the valence band (VB) spectra and x-ray absorption spectroscopy (XAS) data, and on the resonant photoelectron spectroscopy (resPES) profiles at the O1s and the Ti3p absorption edges. We determine the elemental abundance, the position of the VB maxima, the partial density of states (PDOS) in the VB and in the conduction band (CB) and collect these data in a band scheme. In addition, we analyze the band-gap states as well as the intrinsic states due to polarons and charge-transfer excitations. These states are found to cause multiple Auger decay processes upon resonant excitation. We identify several of these processes and determine their relative contribution to the Auger signal quantitatively. As our resPES data allow a quantitative analysis of these defect states, we determine the relative abundance of the PDOS in the VB and in CB and also the charge neutrality level. The anatase and rutile polymorphs of TiO2 are analyzed in the same way as the TiO2 ALD layer. The electronic properties of the TiO2 ALD layer are compared with the anatase and rutile polymorphs of TiO2. In our comparative study, we find that ALD has its own characteristic electronic structure that is distinct from that of anatase and rutile. However, many details of the electronic structure are comparable and we benefit from our spectroscopic data and our careful analysis to find these differences. These can be attributed to a stronger hybridization of the O2p and Ti3d4s states for the ALD films when compared to the anatase and rutile polymorphs.

  13. Resonant Photoemission in f Electron Systems: Pu& Gd

    SciTech Connect

    Tobin, J G; Chung, B W; Schulze, R K; Terry, J; Farr, J D; Shuh, D K; Heinzelman, K; Rotenberg, E; Waddill, G D; van der Laan, G

    2003-03-07

    Resonant photoemission in the Pu5f and Pu6p states is compared to that in the Gd4f and Gd5p states. Spectral simulations, based upon and atomic model with angular momentum coupling, are compared to the Gd and Pu results. Additional spectroscopic measurements of Pu, including core level photoemission and x-ray absorption are also presented.

  14. The evolution of Ga and As core levels in the formation of Fe/GaAs (001): A high resolution soft x-ray photoelectron spectroscopic study

    SciTech Connect

    Thompson, Jamie D. W.; Neal, James R.; Shen, Tiehan H.; Morton, Simon A.; Tobin, James G.; Dan Waddill, G.; Matthew, Jim A. D.; Greig, Denis; Hopkinson, Mark

    2008-07-15

    A high resolution soft x-ray photoelectron spectroscopic study of Ga and As 3d core levels has been conducted for Fe/GaAs (001) as a function of Fe thickness. This work has provided unambiguous evidence of substrate disrupting chemical reactions induced by the Fe overlayer--a quantitative analysis of the acquired spectra indicates significantly differing behavior of Ga and As during Fe growth, and our observations have been compared with existing theoretical models. Our results demonstrate that the outdiffusing Ga and As remain largely confined to the interface region, forming a thin intermixed layer. Whereas at low coverages Fe has little influence on the underlying GaAs substrate, the onset of substrate disruption when the Fe thickness reaches 3.5 A results in major changes in the energy distribution curves (EDCs) of both As and Ga 3d cores. Our quantitative analysis suggests the presence of two additional As environments of metallic character: one bound to the interfacial region and another which, as confirmed by in situ oxidation experiments, surface segregates and persists over a wide range of overlayer thickness. Analysis of the corresponding Ga 3d EDCs found not two, but three additional environments--also metallic in nature. Two of the three are interface resident whereas the third undergoes outdiffusion at low Fe coverages. Based on the variations of the integrated intensities of each component, we present a schematic of the proposed chemical makeup of the Fe/GaAs (001) system.

  15. The evolution of Ga and As core levels in the formation of Fe/GaAs (001):A high resolution soft x-ray photoelectron spectroscopic study

    SciTech Connect

    Thompson, Jamie; Neal, James; Shen, Tiehan; Morton, Simon; Tobin, James; Waddill, George Dan; Matthew, Jim; Greig, Denis; Hopkinson, Mark

    2008-07-14

    A high resolution soft x-ray photoelectron spectroscopic study of Ga and As 3d core levels has been conducted for Fe/GaAs (001) as a function of Fe thickness. This work has provided unambiguous evidence of substrate disrupting chemical reactions induced by the Fe overlayer--a quantitative analysis of the acquired spectra indicates significantly differing behavior of Ga and As during Fe growth, and our observations have been compared with existing theoretical models. Our results demonstrate that the outdiffusing Ga and As remain largely confined to the interface region, forming a thin intermixed layer. Whereas at low coverages Fe has little influence on the underlying GaAs substrate, the onset of substrate disruption when the Fe thickness reaches 3.5 Angstrom results in major changes in the energy distribution curves (EDCs) of both As and Ga 3d cores. Our quantitative analysis suggests the presence of two additional As environments of metallic character: one bound to the interfacial region and another which, as confirmed by in situ oxidation experiments, surface segregates and persists over a wide range of overlayer thickness. Analysis of the corresponding Ga 3d EDCs found not two, but three additional environments--also metallic in nature. Two of the three are interface resident whereas the third undergoes outdiffusion at low Fe coverages. Based on the variations of the integrated intensities of each component, we present a schematic of the proposed chemical makeup of the Fe/GaAs (001) system.

  16. The Evolution of Ga and As Core Levels in the Formation of Fe/GaAs(001): A High Resolution Soft X-ray Photoelectron Spectroscopic Study

    SciTech Connect

    Thompson, J W; Neal, J R; Shen, T H; Morton, S A; Tobin, J G; Waddill, G D; Matthew, J D; Greig, D; Hopkinson, M

    2006-12-08

    A high resolution soft x-ray photoelectron spectroscopic study of Ga and As 3d core levels has been conducted for Fe/GaAs (001) as a function of Fe thickness. This work has provided unambiguous evidence of substrate disrupting chemical reactions induced by the Fe overlayer--a quantitative analysis of the acquired spectra indicates significantly differing behavior of Ga and As during Fe growth, and our observations have been compared with existing theoretical models. Our results demonstrate that the outdiffusing Ga and As remain largely confined to the interface region, forming a thin intermixed layer. Whereas at low coverages Fe has little influence on the underlying GaAs substrate, the onset of substrate disruption when the Fe thickness reaches 3.5 {angstrom} results in major changes in the energy distribution curves (EDCs) of both As and Ga 3d cores. Our quantitative analysis suggests the presence of two new As environments of metallic character; one bound to the interfacial region and another which, as confirmed by in-situ oxidation experiments, surface segregates and persists over a wide range of overlayer thickness. Analysis of the corresponding Ga 3d EDCs found not two, but three new environments--also metallic in nature. Two of the three are interface-resident whereas the third undergoes outdiffusion at low Fe coverages. Based on the variations of the integrated intensities of each component, we present a schematic of the proposed chemical make-up of the Fe/GaAs (001) system.

  17. Pronounced Surface Band Bending of Thin-Film Silicon Revealed by Modeling Core Levels Probed with Hard X-rays.

    PubMed

    Wippler, David; Wilks, Regan G; Pieters, Bart E; van Albada, Sacha J; Gerlach, Dominic; Hüpkes, Jürgen; Bär, Marcus; Rau, Uwe

    2016-07-13

    Enhancing the probing depth of photoemission studies by using hard X-rays allows the investigation of buried interfaces of real-world device structures. However, it also requires the consideration of photoelectron-signal attenuation when evaluating surface effects. Here, we employ a computational model incorporating surface band bending and exponential photoelectron-signal attenuation to model depth-dependent spectral changes of Si 1s and Si 2s core level lines. The data were acquired from hydrogenated boron-doped microcrystalline thin-film silicon, which is applied in silicon-based solar cells. The core level spectra, measured by hard X-ray photoelectron spectroscopy using different excitation energies, reveal the presence of a 0.29 nm thick surface oxide layer. In the silicon film a downward surface band bending of eVbb = -0.65 eV over ∼6 nm obtained via inverse modeling explains the observed core level shifts and line broadening. Moreover, the computational model allows the extraction of the "real" Si 1s and Si 2s bulk core level binding energies as 1839.13 and 150.39 eV, and their natural Lorentzian line widths as 496 and 859 meV, respectively. These values significantly differ from those directly extracted from the measured spectra. Because band bending usually occurs at material surfaces we highly recommend the detailed consideration of signal integration over depth for quantitative statements from depth-dependent measurements.

  18. Photoemission studies of classic and novel thermoelectric materials

    NASA Astrophysics Data System (ADS)

    Greanya, Viktoria Augusta

    Thermoelectric materials have been studied vigorously since the 1950s. Recent advances in materials synthesis and theory have rejuvinated the field in the last decade. The thermoelectric properties of materials are related to their electronic structure. In addition, many of these materials behave quasi-low-dimensionally, making them ideal candidates for study using angle resolved and angle integrated photoelectron spectroscopy (ARPES and AIPES). We report the first detailed study of the valence band electronic structure of Bi2Te3, Bi2Se3 and CsBi 4Te6 using ARPES and AIPES. Experimental results are compared with local density approximation (LDA) band structure calculations and (when available) with de Haas-van Alphen and Shubnikov-de Haas experiments. Bi2Te3 is currently the best room temperature thermoelectric material known. Dispersions of the valence bands were determined using ARPES. A six-fold k-space degeneracy in the valence band maximum is found. The quasi-two-dimensional nature of the electronic structure was demonstrated by the weakly dispersive bands along the Gamma-Z direction. The density of states (DOS) for this material was also studied using AIPES. Spectra were taken at multiple photon energies. Six valence band peaks were found. Good correspondence with the calculated DOS was found. Bi2Se3 is isostructural to Bi2Te 3 but its thermoelectric performance is significantly worse. The valence band dispersions for this material have been determined, as well as the DOS. We find the valence band maximum to be located at Gamma. Ten easily identifiable bands are seen within 4 eV of the Fermi level. The energy bands in the Gamma-Z direction are found to be flatter than those predicted by theory. The APES measurements revealed a total of nine bands, which correspond well to the calculated DOS. CsBi4Te6 is a novel thermoelectric material, recently discovered in the chemistry department of Michigan State University. This material exhibits quasi

  19. Photoemission studies of fluorine functionalized porous graphitic carbon

    NASA Astrophysics Data System (ADS)

    Ganegoda, Hasitha; Jensen, David S.; Olive, Daniel; Cheng, Lidens; Segre, Carlo U.; Linford, Matthew R.; Terry, Jeff

    2012-03-01

    Porous graphitic carbon (PGC) has unique properties desirable for liquid chromatography applications when used as a stationary phase. The polar retention effect on graphite (PREG) allows efficient separation of polar and non-polar solutes. Perfluorinated hydrocarbons however lack polarizabilty and display strong lipo- and hydrophobicity, hence common lipophilic and hydrophilic analytes have low partition coefficiency in fluorinated stationary phases. Attractive interaction between fluorinated stationary phase and fluorinated analytes results in strong retention compared to non-fluorinated analytes. In order to change the selectivities of PGC, it is necessary to develop a bonded PGC stationary phase. In this study, we have synthesized perfluorinated, PGC using hepatadecafluoro-1-iodooctane, under different temperature conditions. Surface functionalization of the raw material was studied using photoelectron spectroscopy (PES). Results indicate the existence of fluorine containing functional groups, -CF, -CF2 along with an intercalated electron donor species. Multiple oxygen functional groups were also observed, likely due to the presence of oxygen in the starting material. These oxygen species may be responsible for significant modifications to planer and tetrahedral carbon ratios.

  20. Photoemission studies of fluorine functionalized porous graphitic carbon

    SciTech Connect

    Ganegoda, Hasitha; Olive, Daniel; Cheng, Lidens; Segre, Carlo U.; Terry, Jeff; Jensen, David S.; Linford, Matthew R.

    2012-03-01

    Porous graphitic carbon (PGC) has unique properties desirable for liquid chromatography applications when used as a stationary phase. The polar retention effect on graphite (PREG) allows efficient separation of polar and non-polar solutes. Perfluorinated hydrocarbons however lack polarizabilty and display strong lipo- and hydrophobicity, hence common lipophilic and hydrophilic analytes have low partition coefficiency in fluorinated stationary phases. Attractive interaction between fluorinated stationary phase and fluorinated analytes results in strong retention compared to non-fluorinated analytes. In order to change the selectivities of PGC, it is necessary to develop a bonded PGC stationary phase. In this study, we have synthesized perfluorinated, PGC using hepatadecafluoro-1-iodooctane, under different temperature conditions. Surface functionalization of the raw material was studied using photoelectron spectroscopy (PES). Results indicate the existence of fluorine containing functional groups, -CF, -CF{sub 2} along with an intercalated electron donor species. Multiple oxygen functional groups were also observed, likely due to the presence of oxygen in the starting material. These oxygen species may be responsible for significant modifications to planer and tetrahedral carbon ratios.

  1. First-principles and angle-resolved photoemission study of lithium doped metallic black phosphorous

    NASA Astrophysics Data System (ADS)

    Sanna, A.; Fedorov, A. V.; Verbitskiy, N. I.; Fink, J.; Krellner, C.; Petaccia, L.; Chikina, A.; Usachov, D. Yu; Grüneis, A.; Profeta, G.

    2016-06-01

    First principles calculations demonstrate the metallization of phosphorene by means of Li doping filling the unoccupied antibonding p z states. The electron–phonon coupling in the metallic phase is strong enough to eventually lead to a superconducting phase at T c = 17 K for LiP8 stoichiometry. Using angle-resolved photoemission spectroscopy we confirm that the surface of black phosphorus can be chemically functionalized using Li atoms which donate their 2s electron to the conduction band. The combined theoretical and experimental study demonstrates the semiconductor-metal transition indicating a feasible way to induce a superconducting phase in phosphorene and few-layer black phosphorus.

  2. Optical study of HgCdTe infrared photodetectors using internal photoemission spectroscopy

    SciTech Connect

    Lao, Yan-Feng; Unil Perera, A. G.; Wijewarnasuriya, Priyalal S.

    2014-03-31

    We report a study of internal photoemission spectroscopy (IPE) applied to a n-type Hg{sub 1−x}Cd{sub x}Te/Hg{sub 1−y}Cd{sub y}Te heterojunction. An exponential line-shape of the absorption tail in HgCdTe is identified by IPE fittings of the near-threshold quantum yield spectra. The reduction of quantum yield (at higher photon energy) below the fitting value is explained as a result of carrier-phonon scatterings. In addition, the obtained bias independence of the IPE threshold indicates a negligible electron barrier at the heterojunction interface.

  3. First-principles and angle-resolved photoemission study of lithium doped metallic black phosphorous

    NASA Astrophysics Data System (ADS)

    Sanna, A.; Fedorov, A. V.; Verbitskiy, N. I.; Fink, J.; Krellner, C.; Petaccia, L.; Chikina, A.; Usachov, D. Yu; Grüneis, A.; Profeta, G.

    2016-06-01

    First principles calculations demonstrate the metallization of phosphorene by means of Li doping filling the unoccupied antibonding p z states. The electron-phonon coupling in the metallic phase is strong enough to eventually lead to a superconducting phase at T c = 17 K for LiP8 stoichiometry. Using angle-resolved photoemission spectroscopy we confirm that the surface of black phosphorus can be chemically functionalized using Li atoms which donate their 2s electron to the conduction band. The combined theoretical and experimental study demonstrates the semiconductor-metal transition indicating a feasible way to induce a superconducting phase in phosphorene and few-layer black phosphorus.

  4. Interfacial electronic structure of Na deposited on rubrene thin film studied by synchrotron radiation photoemission

    NASA Astrophysics Data System (ADS)

    Wei, Ching-Hsuan; Cheng, Chiu-Ping; Lin, Hong-Cheu; Pi, Tun-Wen

    2015-12-01

    The electronic structure of rubrene doped with various concentrations of Na was studied by synchrotron-radiation photoemission. Three stages of development were found with increasing Na concentration; Na penetrating deep into the organic film, followed by development of gap states, and ended with a metallic Na film. The charge transfer from Na to rubrene resulted in a vacuum-level shift. By doping Na into rubrene, we could control the IP of the organic molecule, which is favorable for application in organic semiconductor devices.

  5. Crystal structure and X-ray photoemission spectroscopic study of A{sub 2}LaMO{sub 6} [A=Ba, Ca; M=Nb, Ta

    SciTech Connect

    Dutta, Alo; Saha, Sujoy; Sinha, T.P.

    2015-09-15

    The X-ray photoemission spectroscopic (XPS) study of the double perovskite oxides A{sub 2}LaMO{sub 6} [A=Ba, Ca; M=Nb, Ta] synthesized by the solid-state reaction technique has been carried out to investigate the nature of the chemical state of the constituent ions and the bonding between them. The Rietveld refinement of the X-ray diffraction patterns suggests the monoclinic crystal structure of all the materials at room temperature. The negative and positive chemical shifts of the core level XPS spectrum of O-1s and Nb-3d{sub 3/2}/Ta-4f{sub 5/2} respectively suggest the covalent bonding between Nb/Ta cations and O ion. The change of the bonding strength between the anion and the cations from one material to another has been analyzed. The vibrational property of the materials is investigated using the room temperature Raman spectra. A large covalency of Ta-based compound than Nb compound is confirmed from the relative shifting of the Raman modes of the materials. - Graphical abstract: Crystal structure of two perovskite oxides CLN and CLT is investigated. XPS study confirms the two different co-ordination environments of Ca and covalent bonding between B-site cations and O-ion. - Highlights: • Ordered perovskite structure obtained by Rietveld refinement of XRD patterns. • Study of nature of chemical bonding by X-ray photoemission spectroscopy. • Opposite chemical shift of d-states of Nb/Ta with respect to O. • Covalent bonding between d-states of Nb/Ta and O. • Relative Raman shifts of CLN and CLT substantiate the more covalent character of Ta than Nb.

  6. Electronic structure of Mo1-x Re x alloys studied through resonant photoemission spectroscopy.

    PubMed

    Sundar, Shyam; Banik, Soma; Sharath Chandra, L S; Chattopadhyay, M K; Ganguli, Tapas; Lodha, G S; Pandey, Sudhir K; Phase, D M; Roy, S B

    2016-08-10

    We studied the electronic structure of Mo-rich Mo1-x Re x alloys ([Formula: see text]) using valence band photoemission spectroscopy in the photon energy range 23-70 eV and density of states calculations. Comparison of the photoemission spectra with the density of states calculations suggests that, with respect to the Fermi level E F, the d states lie mostly in the binding energy range 0 to  -6 eV, whereas s states lie in the binding energy range  -4 to  -10 eV. We observed two resonances in the photoemission spectra of each sample, one at about 35 eV photon energy and the other at about 45 eV photon energy. Our analysis suggests that the resonance at 35 eV photon energy is related to the Mo 4p-5s transition and the resonance at 45 eV photon energy is related to the contribution from both the Mo 4p-4d transition (threshold: 42 eV) and the Re 5p-5d transition (threshold: 46 eV). In the constant initial state plot, the resonance at 35 eV incident photon energy for binding energy features in the range E F (BE  =  0) to  -5 eV becomes progressively less prominent with increasing Re concentration x and vanishes for x  >  0.2. The difference plots obtained by subtracting the valence band photoemission spectrum of Mo from that of Mo1-x Re x alloys, measured at 47 eV photon energy, reveal that the Re d-like states appear near E F when Re is alloyed with Mo. These results indicate that interband s-d interaction, which is weak in Mo, increases with increasing x and influences the nature of the superconductivity in alloys with higher x. PMID:27301550

  7. Electronic structure of Mo1-x Re x alloys studied through resonant photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Sundar, Shyam; Banik, Soma; Sharath Chandra, L. S.; Chattopadhyay, M. K.; Ganguli, Tapas; Lodha, G. S.; Pandey, Sudhir K.; Phase, D. M.; Roy, S. B.

    2016-08-01

    We studied the electronic structure of Mo-rich Mo1-x Re x alloys (0≤slant x≤slant 0.4 ) using valence band photoemission spectroscopy in the photon energy range 23-70 eV and density of states calculations. Comparison of the photoemission spectra with the density of states calculations suggests that, with respect to the Fermi level E F, the d states lie mostly in the binding energy range 0 to  -6 eV, whereas s states lie in the binding energy range  -4 to  -10 eV. We observed two resonances in the photoemission spectra of each sample, one at about 35 eV photon energy and the other at about 45 eV photon energy. Our analysis suggests that the resonance at 35 eV photon energy is related to the Mo 4p-5s transition and the resonance at 45 eV photon energy is related to the contribution from both the Mo 4p-4d transition (threshold: 42 eV) and the Re 5p-5d transition (threshold: 46 eV). In the constant initial state plot, the resonance at 35 eV incident photon energy for binding energy features in the range E F (BE  =  0) to  -5 eV becomes progressively less prominent with increasing Re concentration x and vanishes for x  >  0.2. The difference plots obtained by subtracting the valence band photoemission spectrum of Mo from that of Mo1-x Re x alloys, measured at 47 eV photon energy, reveal that the Re d-like states appear near E F when Re is alloyed with Mo. These results indicate that interband s-d interaction, which is weak in Mo, increases with increasing x and influences the nature of the superconductivity in alloys with higher x.

  8. Electronic structure of Mo1‑x Re x alloys studied through resonant photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Sundar, Shyam; Banik, Soma; Sharath Chandra, L. S.; Chattopadhyay, M. K.; Ganguli, Tapas; Lodha, G. S.; Pandey, Sudhir K.; Phase, D. M.; Roy, S. B.

    2016-08-01

    We studied the electronic structure of Mo-rich Mo1‑x Re x alloys (0≤slant x≤slant 0.4 ) using valence band photoemission spectroscopy in the photon energy range 23–70 eV and density of states calculations. Comparison of the photoemission spectra with the density of states calculations suggests that, with respect to the Fermi level E F, the d states lie mostly in the binding energy range 0 to  ‑6 eV, whereas s states lie in the binding energy range  ‑4 to  ‑10 eV. We observed two resonances in the photoemission spectra of each sample, one at about 35 eV photon energy and the other at about 45 eV photon energy. Our analysis suggests that the resonance at 35 eV photon energy is related to the Mo 4p–5s transition and the resonance at 45 eV photon energy is related to the contribution from both the Mo 4p–4d transition (threshold: 42 eV) and the Re 5p–5d transition (threshold: 46 eV). In the constant initial state plot, the resonance at 35 eV incident photon energy for binding energy features in the range E F (BE  =  0) to  ‑5 eV becomes progressively less prominent with increasing Re concentration x and vanishes for x  >  0.2. The difference plots obtained by subtracting the valence band photoemission spectrum of Mo from that of Mo1‑x Re x alloys, measured at 47 eV photon energy, reveal that the Re d-like states appear near E F when Re is alloyed with Mo. These results indicate that interband s–d interaction, which is weak in Mo, increases with increasing x and influences the nature of the superconductivity in alloys with higher x.

  9. Photoemissive coating

    NASA Technical Reports Server (NTRS)

    Gange, R. A.

    1972-01-01

    Polystyrene coating is applied to holographic storage tube substrate via glow discharge polymerization in an inert environment. After deposition of styrene coating, antimony and then cesium are added to produce photoemissive layer. Technique is utilized in preparing perfectly organized polymeric films useful as single-crystal membranes.

  10. Study on the long wavelength SiGe/Si heterojunction internal photoemission infrared photodetectors

    NASA Astrophysics Data System (ADS)

    Aslan, B.; Turan, R.; Liu, H. C.

    2005-10-01

    The theory of internal photoemission in semiconductor heterojunctions has been investigated and the existing model has been extended by incorporating the effect of different effective masses in the active region and the substrate, nonspherical-nonparabolic bands, and the energy loss per collision. Photoresponse measurements on Si 1- xGe x/Si heterojunction internal photoemission (HIP) infrared photodetectors (IP) have shown that they are fit well by the theory. Qualitative model describing the mechanisms of photocurrent generation in our structures are presented. We also study the effect of a double barrier on the photoresponse spectrum of a SiGe/Si HIP IP. It has been shown that the performance of our devices depends significantly on the applied bias and the operating temperature; therefore, their cut-off wavelengths can be tuned to the desired region by changing the potential difference across the device and/or changing the device temperature. The barrier heights (correspondingly the cut-off wavelengths) of the samples have been determined from their IP spectra by using the extended model which has the wavelength and doping concentration dependent free carrier absorption parameters.

  11. Angle resolved photoemission study of the c(2 × 2)Si overlayer on Fe(100)

    NASA Astrophysics Data System (ADS)

    Egert, B.; Grabke, H. J.; Sakisaka, Y.; Rhodin, T. N.

    1984-06-01

    Angle resolved photoemission experiments utilizing polarized synchrotron radiation were performed to study the electronic structure of valence levels of Si segregated in a c(2 × 2) overlayer on the α-Fe(100) surface. The spectra were taken at varying photon energies (14 ⩽ ω ⩽ 40 eV), in dependence on the polarization of the incoming light, and as a function of the photoelectron emission angle in the symmetry directions T¯M¯' and T¯X¯' of the surface Brillouin zone. Evaluation of the photoemission data shows that the Si 3p levels form energy bands for the ordered c(2 × 2) overlayer on Fe(100). The initial state energy of the Si 3p states depends on k∥ being measured. At T¯ a bonding Si 3p z state (a 1 symmetry) and an antibonding Si 3p xp y state (e symmetry) is analyzed, which are separated by 0.8 eV in binding energy. In going from T¯ to M¯' the Si 3p z induced level disperses ~ 0.8 eV to lower initial state energies. In the T¯X¯' direction the overall Si 3p band width is approximate 1.3 eV. Though the interaction between silicon and iron surface atoms are relatively weak compared to Fe(100)-c(2 × 2)S, modifications in the Fe derived valence band states occur, including the formation of a hybridization state located 1.4 eV below EF.

  12. Interaction between adsorbed hydrogen and potassium on a carbon nanocone containing material as studied by photoemission

    SciTech Connect

    Yu, Xiaofeng; Raaen, Steinar

    2015-09-14

    Hydrogen adsorption on a potassium doped carbon nanocone containing material was studied by photoelectron spectroscopy and work function measurement. The valence band spectra indicate that there is charge transfer from potassium to carbon. Upon deposition on carbon potassium is in its ionic state for lower doping and shows both ionic and metallic behavior at higher doping. Adsorption of hydrogen facilitates diffusion of potassium on the carbon material as seen by changes in the K{sub 2p} core level spectrum. Variations in the measured sample work function indicate that hydrogen initially adsorb on the K dopants and subsequently adsorb on the carbon cone containing material.

  13. Density Functional Theory Study of the Energetics, Electronic Structure, and Core-Level Shifts of NO Adsorption on the Pt(111) Surface

    SciTech Connect

    Zeng, Z. H.; Da Silva, J. L. F.; Deng, H. Q.; Li, W. X.

    2009-01-01

    In this work, we report a first-principles investigation of the energetics, structures, electronic properties, and core-level shifts of NO adsorption on the Pt(111) surface. Our calculations are based on density functional theory within the framework of the ultrasoft pseudopotential plane-wave and the all-electron projected augmented-wave methods. We found that at 0.25, 0.50, and 0.75 monolayer, NO adsorbs preferentially in the fcc, fcc+top, and fcc+top+hcp sites, respectively. The geometric parameters, adsorption energies, vibrational frequencies, and work-function changes are in good agreement with the experimental data. The interaction between NO and Pt(111) was found to follow a donation-back-donation process, in which the NO {sigma} states donate electrons to the substrate Pt d states, while the substrate Pt d states back donate to the NO {pi} states. Though there is an overall net charge transfer from the substrate to the NO adsorbate regardless of the adsorption sites and coverages, the spatial redistribution of the transferred electron is site dependent. The charge accumulation for NO in the top sites occurs closer to the surface than NO in the hollow sites, which results in the reduction of the Pt(111) surface work function for the top NO but an increase for the hollow NO. The core-level shifts of the topmost surface Pt atoms coordinated with top and hollow NO molecules at different coverages are in excellent agreement with experiments. In contrast, the N 1s core-level shifts between top and hollow NO ({approx}0.7 eV) deviated significantly from the zero shift found in experiments. Our analysis indicates that the difference may come from the thermal vibration and rotation of adsorbed NO on the Pt(111) surface.

  14. Angle Resolved Photoemission Study of a Mott Insulator and Its Evolution to a High Temperature Superconductor

    NASA Astrophysics Data System (ADS)

    Ronning, F.

    2002-03-01

    One of the most remarkable facts about the high temperature superconductors is their close proximity to an antiferromagnetically ordered Mott insulating phase. This fact suggests that to understand superconductivity in the cuprates we must first understand the insulating regime. Due to material properties the technique of angle resolved photoemission is ideally suited to study the electronic structure in the cuprates. Thus, a natural starting place to unlocking the secrets of high Tc would appears to be with a photoemission investigation of insulating cuprates. This dissertation presents the results of precisely such a study. In particular, we have focused on the compound Ca2-xNaxCuO2Cl2. With increasing Na content this system goes from an antiferromagnetic Mott insulator with a Neel transition of 256K to a superconductor with an optimal transition temperature of 28K. At half filling we have found an asymmetry in the integrated spectral weight, which can be related to the occupation probability, n(k). This has led us to identify a d-wave-like dispersion in the insulator, which in turn implies that the high energy pseudogap as seen by photoemission is a remnant property of the insulator. These results are robust features of the insulator which we found in many different compounds and experimental conditions. By adding Na we were able to study the evolution of the electronic structure across the insulator to metal transition. We found that the chemical potential shifts as holes are doped into the system. This picture is in sharp contrast to the case of La2-xSrxCuO4 where the chemical potential remains fixed and states are created inside the gap. Furthermore, the low energy excitations (ie the Fermi surface) in metallic Ca1.9Na0.1CuO2Cl2 is most well described as a Fermi arc, although the high binding energy features reveal the presence of shadow bands. Thus, the results in this dissertation provide a new avenue for understanding the evolution of the Mott insulator to

  15. Interaction of light and surface plasmon polaritons in Ag islands studied by nonlinear photoemission microscopy.

    PubMed

    Buckanie, N M; Kirschbaum, P; Sindermann, S; Meyer zu Heringdorf, F-J

    2013-07-01

    Two photon photoemission microscopy was used to study the interaction of femtosecond laser pulses with Ag islands prepared using different strategies on Si(111) and SiO₂. The femtosecond laser pulses initiate surface plasmon polariton (SPP) waves at the edges of the island. The superposition of the electrical fields of the femtosecond laser pulses with the electrical fields of the SPP results in a moiré pattern that is comparable despite the rather different methods of preparation and that gives access to the wavelength and direction of the SPP waves. If the SPPs reach edges of the Ag islands, they can be converted back into light waves. The incident and refracted light waves result in an interference pattern that can again be described with a moiré pattern, demonstrating that Ag islands can be used as plasmonic beam deflectors for light.

  16. Photoemission spectroscopy study of the lanthanum lutetium oxide/silicon interface

    SciTech Connect

    Nichau, A.; Schnee, M.; Schubert, J.; Bernardy, P.; Hollaender, B.; Buca, D.; Mantl, S.; Besmehn, A.; Breuer, U.; Rubio-Zuazo, J.; Castro, G. R.; Muecklich, A.; Borany, J. von

    2013-04-21

    Rare earth oxides are promising candidates for future integration into nano-electronics. A key property of these oxides is their ability to form silicates in order to replace the interfacial layer in Si-based complementary metal-oxide field effect transistors. In this work a detailed study of lanthanum lutetium oxide based gate stacks is presented. Special attention is given to the silicate formation at temperatures typical for CMOS processing. The experimental analysis is based on hard x-ray photoemission spectroscopy complemented by standard laboratory experiments as Rutherford backscattering spectrometry and high-resolution transmission electron microscopy. Homogenously distributed La silicate and Lu silicate at the Si interface are proven to form already during gate oxide deposition. During the thermal treatment Si atoms diffuse through the oxide layer towards the TiN metal gate. This mechanism is identified to be promoted via Lu-O bonds, whereby the diffusion of La was found to be less important.

  17. Photoemission study of the electronic structure and charge density waves of Na₂Ti₂Sb₂O

    SciTech Connect

    Tan, S. Y.; Jiang, J.; Ye, Z. R.; Niu, X. H.; Song, Y.; Zhang, C. L.; Dai, P. C.; Xie, B. P.; Lai, X. C.; Feng, D. L.

    2015-04-30

    The electronic structure of Na₂Ti₂Sb₂O single crystal is studied by photon energy and polarization dependent angle-resolved photoemission spectroscopy (ARPES). The obtained band structure and Fermi surface agree well with the band structure calculation of Na₂Ti₂Sb₂O in the non-magnetic state, which indicates that there is no magnetic order in Na₂Ti₂Sb₂O and the electronic correlation is weak. Polarization dependent ARPES results suggest the multi-band and multi-orbital nature of Na₂Ti₂Sb₂O. Photon energy dependent ARPES results suggest that the electronic structure of Na₂Ti₂Sb₂O is rather two-dimensional. Moreover, we find a density wave energy gap forms below the transition temperature and reaches 65 meV at 7 K, indicating that Na₂Ti₂Sb₂O is likely a weakly correlated CDW material in the strong electron-phonon interaction regime. (author)

  18. Synchrotron-Radiation Photoemission Study of Electronic Structures of a Cs-Doped Rubrene Surface

    NASA Astrophysics Data System (ADS)

    Cheng, Chiu-Ping; Lu, Meng-Han; Chu, Yu-Ya; Pi, Tun-Wen

    Using synchrotron-radiation photoemission spectroscopy, we have studied the electronic structure of a cesium-doped rubrene thin film. The addition of cesium atoms causes the movement of the valence-band spectra and the change in line shapes at different concentration that can be separated into four different stages. In the first stage, the cesium atoms continuously diffuse into the substrate, and the Fermi level moves in the energy gap as a result of an electron transferred from the cesium to the rubrene. The second stage, in which the shifts of the spectra are interrupted, is characterized by the introduction of two in-gap states. When increasing doping of cesium into the third stage, the spectra move again; whereas, the line shapes maintain at the stoichiometric ratio of one. In the fourth stage, new in-gap states appear, which are the highest occupied molecular orbital (HOMO) and HOMO+1 states of (rubrene)2- anion.

  19. Multi-Atom Resonant Photoemission

    NASA Astrophysics Data System (ADS)

    Kay, Alex; Yang, See-Hun; Garcia de Abajo, F. J.; Elke, Arenholz; Mun, Bongjin S.; Mannella, Norman; Zhao, Limin; Hussain, Zahid; van Hove, Michel; Fadley, Charles S.

    2001-03-01

    We will present experimental and theoretical results related to multi-atom resonant photoemission (MARPE) [1], in which the photoelectron intensity from a core level on one atom is influenced by a core-level absorption resonance on another. We will first point out that some prior experimental data [1-3] has been strongly influenced by non-linearities in the detector utilized [2], and that the effects seen in new corrected data are smaller, have a different form, and are strongly dependent on x-ray incidence angle. Data for the specific case of O 1s photoemission from MnO in resonance with Mn 2p excitations that are properly corrected for detector non-linearities data are found to be well described by an extension of resonant photoemission theory to the interatomic case [4], provided that interactions beyond the usual second-order Kramers-Heisenberg treatment are included. These higher-order interactions represent the equivalent of multiple resonant elastic scattering of the radiation. This microscopic theory is also found to simplify so as to yield results equivalent to a classical macroscopic x-ray optical approach, with the latter providing an alternative, although less detailed and general, physical picture of these effects. The relationship of these core-core resonant effects to similar effects seen in valence-core resonances [5-7], as well as in photoelectron angular distributions from a free molecule [8], and to x-ray fluorescence holography, will be discussed. Possible future applications of MARPE to studies of near-neighbor identities and bonding will also be suggested. [1] A. Kay, E. Arenholz, S. Mun, J. Garcia de Abajo, C.S. Fadley, R. Denecke, Z. Hussain, and M.A. Van Hove, Science 281, 679 (1998). [2] M.G. Garnier, N. Witkowski, R. Denecke, D. Nordlund, A. Nilsson, M. Nagasono, N. Mårtensson, and A. Föhlisch, Maxlab Annual Report for 1999 and private communication correcting this data for detector non-linearities. [3] A. Kikas, E. Nommiste, R. Ruus, A

  20. Thermal stability of the HfO2/SiO2 interface for sub-0.1 μm complementary metal-oxide-semiconductor gate oxide stacks: A valence band and quantitative core-level study by soft x-ray photoelectron spectroscopy

    NASA Astrophysics Data System (ADS)

    Barrett, N.; Renault, O.; Damlencourt, J.-F.; Martin, F.

    2004-12-01

    Synchrotron-radiation photoelectron spectroscopy is used to study the valence-band structure and the core-level photoemission spectra of HfO2 ultrathin films grown onto SiO2/Si substrates by atomic layer deposition (ALD). We determine the band offsets (valence and conduction) of HfO2 to Si as a function of postdeposition annealing treatments (under an inert N2 atmosphere or in situ in ultrahigh vacuum) and find a significant evolution, the conduction-band offset remaining larger than 1.5eV. The Si2p and the Hf4f core-level spectra give detailed information on the composition and the spatial extent of the interfacial Hf silicate layer formed between the SiO2 bottom oxide and the HfO2 ALD thin film. By a quantitative treatment of the Si2p core-level intensities, we examine the thermal stability of the interface silicate after postdeposition annealing under N2 and in situ annealing in ultrahigh vacuum (UHV), both at 800°C. The as-deposited layer gives rise to a HfO2/Hf0.35Si0.65O2/SiO2 stack with corresponding thicknesses of 0.74/0.51/0.73nm. After postdeposition annealing at 800°C in a N2 atmosphere, this becomes a HfO2/Hf0.31Si0.69O2/SiO2 stack with corresponding thicknesses of 0.71:0.58:0.91nm. In situ annealing in UHV, on the other hand, gives a HfO2/Hf0.35Si0.65O2/SiO2 stack with corresponding thicknesses of 0.65:0.70:0.76nm. The former favors an extension of both the silicate and the SiO2 interface layers, whereas the latter develops only the silicate layer.

  1. Epitaxy of CoSix (1studied by photoemission and extended x-ray-absorption fine-structure techniques

    NASA Astrophysics Data System (ADS)

    Pirri, C.; Hong, S.; Tuilier, M. H.; Wetzel, P.; Gewinner, G.; Cortès, R.

    1996-01-01

    Electronic and structural properties of epitaxial CoSix layers have been investigated by means of core-level and valence-band photoemission, x-ray photoelectron diffraction, and extended x-ray-absorption fine-structure (EXAFS) experiments. CoSix layers of various x compositions have been grown on silicon by low rate Co and Si co-deposition onto room-temperature Si(111) substrates, with film thicknesses ranging from 30 to 100 Å. Photoemission shows substantial differences in valence and core-level spectra with respect to those of stable fluorite-type CoSi2 and ɛ-CoSi and indicate that well-defined metastable phases are formed. In particular, core-level photoemission experiments performed with a monochromatized x-ray source show large Si 2p binding-energy shifts (~0.4 eV) in the room-temperature deposited CoSix (1

  2. Trends in adsorbate induced core level shifts

    NASA Astrophysics Data System (ADS)

    Nilsson, Viktor; Van den Bossche, Maxime; Hellman, Anders; Grönbeck, Henrik

    2015-10-01

    Photoelectron core level spectroscopy is commonly used to monitor atomic and molecular adsorption on metal surfaces. As changes in the electron binding energies are convoluted measures with different origins, calculations are often used to facilitate the decoding of experimental signatures. The interpretation could in this sense benefit from knowledge on trends in surface core level shifts for different metals and adsorbates. Here, density functional theory calculations have been used to systematically evaluate core level shifts for (111) and (100) surfaces of 3d, 4d, and 5d transition metals upon CO, H, O and S adsorption. The results reveal trends and several non-intuitive cases. Moreover, the difficulties correlating core level shifts with charging and d-band shifts are underlined.

  3. Electronic Properties of Layered Oxides:. Pulsed Laser Deposition of YBCO Films for In-Situ Studies by Photoemission Spectroscopy

    NASA Astrophysics Data System (ADS)

    Pavuna, D.; Ariosa, D.; Berger, H.; Christensen, S.; Frazer, B.; Gatt, R.; Grioni, M.; Margaritondo, G.; Misra, S.; Onellion, M.; Schmauder, T.; Vobornik, I.; Xi, X.; Zacchigna, M.; Zwick, F.

    Due to imperfect surfaces of most cuprate samples, almost all Photoemission studies in the past decade were performed on Bi2Sr2CaCu2O8+x, even though a large fraction of other studies and electronic applications was reported for YBa2Cu3O7-δ (YBCO) family of superconducting compounds. In order to systematically study the gap parameter and the Fermi surface variation in high symmetry directions of YBCO and related oxide films we have constructed a new facility at the Wisconsin Synchrotron Radiation Center. We use the pulsed laser ablation (PLD) system that is directly linked to the photoemission chamber. In our unique approach, the samples never leave the controlled ambient and we oxidize our films, either by molecular oxygen or by ozone. In this paper, we, summarize some of the most relevant recent results on electronic properties of layered oxides and describe our new facility for the study of YBCO and related oxide films.

  4. Structural and electronic properties of V2O3 ultrathin film on Ag(001): LEED and photoemission study

    NASA Astrophysics Data System (ADS)

    Kundu, Asish K.; Menon, Krishnakumar S. R.

    2016-05-01

    V2O3 ultrathin films were grown on Ag(001) substrate by reactive evaporation of vanadium (V) metal in presence of oxygen and their structural and electronic properties were studied by Low Energy Electron Diffraction (LEED), X-ray Photo Electron Spectroscopy (XPS) and Angle Resolved Photoemission Spectroscopic (ARPES) techniques, respectively. On top of square symmetry substrate Ag(001), hexagonal surface of V2O3 (0001) is stabilized in the form of two domain structure, rotated by 30°(or 90°)to each other, has been observed by LEED. Rather than epitaxial flat monolayer, formation of well-ordered V2O3 (0001) island has been confirmed from the LEED and the Photoemission Spectroscopic (PES) study. Stoichiometry of the grown film was confirmed by the XPS study. Evolution of valance band electronic structure of V2O3 (0001) surface has been studied as a function of film thickness by ARPES.

  5. Structural studies of molecular and metallic overlayers using angle- resolved photoemission extended fine structure

    SciTech Connect

    Huang, Z.

    1992-10-01

    Angle-resolved photoemission extended fine structure (ARPEFS) was used to study molecular and metallic overlayers on metal surfaces through analysis of p2mg(2[times]1)CO/Ni(110) and the p(2[times]2)K/Ni(111) adsorption. For the dense p2mg(2[times]1)CO/Ni(110) surface layer, photoemission intensities from C 1s level were measured in three directions at photoelectron kinetic energies 60-400 eV. Using multiple-scattering spherical-wave (MSSW) modeling, it was found that CO molecules are adsorbed on short-bridge sites, with adjacent CO along the [110] direction displaced alternatively in opposite directions towards the [001] azimuths to form a zigzag chain geometry. The tilt angle is 16[plus minus]2[degree] from the surface normal for the direction linking the C atom and the center of the Ni bridge. The carbon C-Ni interatomic distance was determined to be 1.94[plus minus]0.02[Angstrom]. The first- to second-layer spacing of Ni is 1.27[plus minus]0.04[Angstrom], up from 1.10[Angstrom] for the clean Ni(110) surface, but close to the 1.25[Angstrom] Ni interlayer spacing in the bulk. The C-O bond length and tilt angle were varied within small ranges (1.10--1.20[Angstrom] and 15--23[degrees]) in our MSSW simulations. Best agreement between experiment and simulations was achieved at 1.16[Angstrom] and 19[degrees]. This yields an O-O distance of 2.95[Angstrom] for the two nearest CO molecules, (van der Waals' radius [approximately] 1.5 [Angstrom] for oxygen). Two different partial-wave phase-shifts were used in MSSW, and structural results from both are in very good agreement. For the p(2[times]2)K/Ni(111) overlayer, ARPEFS [chi](k) curves from K 1s level measured along [111] and [771] at 130K showed that the K atoms are preferentially adsorbed on the atop sites, in agreement with a LEED study of the same system.

  6. Structural studies of molecular and metallic overlayers using angle- resolved photoemission extended fine structure

    SciTech Connect

    Huang, Z.

    1992-10-01

    Angle-resolved photoemission extended fine structure (ARPEFS) was used to study molecular and metallic overlayers on metal surfaces through analysis of p2mg(2{times}1)CO/Ni(110) and the p(2{times}2)K/Ni(111) adsorption. For the dense p2mg(2{times}1)CO/Ni(110) surface layer, photoemission intensities from C 1s level were measured in three directions at photoelectron kinetic energies 60-400 eV. Using multiple-scattering spherical-wave (MSSW) modeling, it was found that CO molecules are adsorbed on short-bridge sites, with adjacent CO along the [110] direction displaced alternatively in opposite directions towards the [001] azimuths to form a zigzag chain geometry. The tilt angle is 16{plus_minus}2{degree} from the surface normal for the direction linking the C atom and the center of the Ni bridge. The carbon C-Ni interatomic distance was determined to be 1.94{plus_minus}0.02{Angstrom}. The first- to second-layer spacing of Ni is 1.27{plus_minus}0.04{Angstrom}, up from 1.10{Angstrom} for the clean Ni(110) surface, but close to the 1.25{Angstrom} Ni interlayer spacing in the bulk. The C-O bond length and tilt angle were varied within small ranges (1.10--1.20{Angstrom} and 15--23{degrees}) in our MSSW simulations. Best agreement between experiment and simulations was achieved at 1.16{Angstrom} and 19{degrees}. This yields an O-O distance of 2.95{Angstrom} for the two nearest CO molecules, (van der Waals` radius {approximately} 1.5 {Angstrom} for oxygen). Two different partial-wave phase-shifts were used in MSSW, and structural results from both are in very good agreement. For the p(2{times}2)K/Ni(111) overlayer, ARPEFS {chi}(k) curves from K 1s level measured along [111] and [771] at 130K showed that the K atoms are preferentially adsorbed on the atop sites, in agreement with a LEED study of the same system.

  7. Study of the P3HT/PCBM interface using photoemission yield spectroscopy

    NASA Astrophysics Data System (ADS)

    Grzibovskis, Raitis; Vembris, Aivars

    2016-04-01

    Photogeneration efficiency and charge carrier extraction from active layer are the parameters that determine the efficiency of organic photovoltaics (OPVs). Devices made of organic materials often consist of thin (up to 100nm) layers. At this thickness different interface effects become more pronounced. The electron affinity and ionization energy shift can affect the charge carrier transport across metal-organic interface which can affect the performance of the entire device. In the case of multilayer OPVs, energy level compatibility at the organic-organic interface is as important. Photoemission yield spectroscopy was used for organic-organic interface study by ionization energy measurements. In this work we studied "sandwich" type samples of two well-known organic photovoltaic materials- poly(3- hexylthiophene-2,5-diyl) (P3HT) and [6,6]-phenyl C61 butyric acid methyl ester (PCBM). Ionization energy changes at the P3HT/PCBM interface depending on PCBM layer thickness were studied. P3HT layer was obtained by spin-coating while PCBM was deposited on the P3HT by thermal evaporation in vacuum. No ionization energy shift of P3HT was observed. On the contrary, PCBM at the interface with P3HT created additional 0.40eV barrier for hole transport from PCBM to P3HT.

  8. A soft x-ray photoemission study of the chemisorption and reaction of diethylsilane on Si(100)

    SciTech Connect

    Lapiano-Smith, D.A.; Himpsel, F.J.; Terminello, L.J.

    1993-06-01

    Soft x-ray synchrotron radiation was utilized as the excitation source in a high-resolution photoemission experiment on chemisorption and subsequent reaction of diethylsilane on the Si(100) surface. We have found that diethylsilane chemisorbs dissociatively to form Si-CH{sub 2}CH{sub 3} surface species on Si(100) following a room temperature exposure. These species are identified by two very sharp peaks observed in the valence band spectra positioned at 17.9 and 14.3 eV binding energy. In addition, C 1s core level spectra, measured following exposures of Si(100) substrates as a function of surface temperature, show that carbon, in some form, exists on the Si surface following exposures at every temperature from room temperature to about 600C. While only {minus}CH{sub 2}CH{sub 3}, ethyl groups are observed on the surface at room temperature, these species appear to partially dehydrogenate at 300C, producing a mixture of {minus}CH{sub 2}CH{sub 3} groups and other intermediate carbonaceous species. At a growth temperature of about 400C the intermixing of elemental carbon with Si begins. At higher temperatures, we observe the continued degradation of diethylsilane to produce a Si + C alloy on the surface at 600C. Results indicate that diethylsilane has potential as a molecular precursor for SiC formation by chemical vapor deposition techniques.

  9. Unit charge on supported gold clusters in photoemission final state

    NASA Astrophysics Data System (ADS)

    Wertheim, G. K.; Dicenzo, S. B.; Youngquist, S. E.

    1983-12-01

    The large, positive core-level shifts seen in photoemission from Au clusters on poorly conducting substrates result from a unit positive charge left on a cluster during the photoemission final state. The case of clusters supported on a poorly conducting carbon substrate is intermediate between the case of free clusters and that of clusters supported on metallic substrates. The identification of a macroscopic Coulomb effect removes the apparent conflict between positive core-level shifts and the expected initial state band-structure effect, whereby increased localization in small clusters should increase the density in Au and decrease the Au core electron binding energy.

  10. CHEMISTRY OF SO{sub 2} ON MODEL METAL AND OXIDE CATALYSTS: PHOTOEMISSION AND XANES STUDIES

    SciTech Connect

    RODRIGUEZ,J.A.; JIRSAK,T.; CHATURVEDI,S.; HRBEK,J.; FREITAG,A.; LARESE,J.Z.

    2000-07-09

    High-resolution synchrotron based photoemission and x-ray absorption spectroscopy have been used to study the interaction of SO{sub 2} with a series of metals and oxides. The chemistry of SO{sub 2} on metal surfaces is rich. At low coverages, the molecule fully decomposes into atomic S and O. At large coverages, the formation of SO{sub 3} and SO{sub 4} takes place. The following sequence was found for the reactivity of the metals towards SO{sub 2}: Pt {approx} Rh < Ru < Mo << Zn, Sn, Cs. Alloying can be useful for reducing the chemical affinity of a metal for SO{sub 2} and controlling S poisoning. Pd atoms bonded to Rh and Pt atoms bonded to Sn interact weakly with SO{sub 2}. In general, SO{sub 2} mainly reacts with the O centers of metal oxides. SO{sub 4} is formed on CeO{sub 2} and SO{sub 3} on ZnO. On these systems there is no decomposition of SO{sub 2}. Dissociation of the molecule is observed after introducing a large amount of Ce{sup 3+} sites in ceria, or after depositing Cu or alkali metals on the oxide surfaces. These promote the catalytic activity of the oxides during the destruction of SO{sub 2}.

  11. Internal Photoemission and X-Ray Photoelectron Spectroscopic Studies of Sulfur-Passivated GaAs

    NASA Astrophysics Data System (ADS)

    Sato, Kenji; Ikoma, Hideaki

    1993-02-01

    Internal photoemission and X-ray photoelectron spectroscopic (XPS) measurements were performed to investigate the effect of sulfur passivation on the GaAs surface and the degradation of the GaAs surface exposed to air ambient after the passivation. The reverse bias dependence of the Schottky barrier height was very small in the as-sulfur-treated sample and was mainly explained by the image force lowering effect. However, it increased as this sample was exposed to air, indicating an increase in the interface state density. The XPS studies showed that both the Ga and As oxides were hardly observed in the sulfur-passivated samples. This indicates that sulfur passivation strongly suppresses oxidation of GaAs. However, a small amount of elemental arsenic was observed with a trace of the As suboxides (such as AsO) after exposure to air and it increased as the exposure time was increased. These results were probably correlated with the increase in the bias dependence of the Schottky barrier height in samples exposed to air after the passivation. Thermal oxidation of GaAs was found to be retarded by sulfur passivation until oxidation time was about 10 min at 300°C. A possible model of suppression of oxidation by sulfur passivation was also discussed.

  12. Bi2-Bi2Se3 Superlattice Materials Studied by Photoemission Spectroscopy

    NASA Astrophysics Data System (ADS)

    Weber, Andrew; Pletikosic, Ivo; Gibson, Quinn; Ji, Huiwen; Schoop, Leslie; Sadowski, Jurek; Caruso, Anthony; Vescovo, Elio; Fedorov, Alexei; Cava, Robert; Valla, Tonica

    2014-03-01

    Although searches are carried out independently for new 2D quantum spin Hall or 3D topological materials for their robust, spin-polarized edge or surface conduction states, little has been done to experimentally show that both phases can coexist in a single material or explore how they may interact. The superlattice series Bi2m(Bi2Se3)n , featuring stacked layers of Bi2 and Bi2Se3, may contain systems where a combination of 2D and 3D topological phenomena should be at play, the latter of which can be identified by combined computational and spin-and angle-resolved photoemission spectroscopy studies. We find that several members of the series, (m =0, n =1), (m =1, n =1) and (m =2, n =1) have spin-chiral surface states at the center of the surface Brillouin zone, a trait of strong topological insulators. The characterization of the topological surface states will be discussed for these series members.

  13. Synchrotron radiation photoemission study of metal overlayers on hydrogenated amorphous silicon at room temperature

    SciTech Connect

    Pi, J.

    1990-09-21

    In this dissertation, metals deposited on a hydrogenated amorphous silicon (a-Si:H) film at room temperature are studied. The purpose of this work is mainly understanding the electronic properties of the interface, using high-resolution synchrotron radiation photoemission techniques as a probe. Atomic hydrogen plays an important role in passivating dangling bonds of a-Si:H films, thus reducing the gap-state distribution. In addition, singly bonded hydrogen also reduces states at the top of the valence band which are now replaced by deeper Si-H bonding states. The interface is formed by evaporating metal on an a-Si:H film in successive accumulations at room temperature. Au, Ag, and Cr were chosen as the deposited metals. Undoped films were used as substrates. Since some unique features can be found in a-Si:H, such as surface enrichment of hydrogen diffused from the bulk and instability of the free surface, we do not expect the metals/a-Si:H interface to behave exactly as its crystalline counterpart. Metal deposits, at low coverages, are found to gather preferentially around regions deficient in hydrogen. As the thickness is increased, some Si atoms in those regions are likely to leave their sites to intermix with metal overlayers like Au and Cr. 129 refs., 30 figs.

  14. Band alignments in Fe/graphene/Si(001) junctions studied by x-ray photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Le Breton, J.-C.; Tricot, S.; Delhaye, G.; Lépine, B.; Turban, P.; Schieffer, P.

    2016-08-01

    The control of tunnel contact resistance is of primary importance for semiconductor-based spintronic devices. This control is hardly achieved with conventional oxide-based tunnel barriers due to deposition-induced interface states. Manipulation of single 2D atomic crystals (such as graphene sheets) weakly interacting with their substrate might represent an alternative and efficient way to design new heterostructures for a variety of different purposes including spin injection into semiconductors. In the present paper, we study by x-ray photoemission spectroscopy the band alignments and interface chemistry of iron-graphene-hydrogenated passivated silicon (001) surfaces for a low and a high n-doping concentration. We find that the hydrogen passivation of the Si(001) surface remains efficient even with a graphene sheet on the Si(001) surface. For both doping concentrations, the semiconductor is close to flat-band conditions which indicates that the Fermi level is unpinned on the semiconductor side of the Graphene/Si(001):H interface. When iron is deposited on the graphene/Si(001):H structures, the Schottky barrier height remains mainly unaffected by the metallic overlayer with a very low barrier height for electrons, a sought-after property in semiconductor based spintronic devices. Finally, we demonstrate that the graphene layer intercalated between the metal and semiconductor also serves as a protection against iron-silicide formation even at elevated temperatures preventing from the formation of a Si-based magnetic dead layer.

  15. Photoemission study of the electronic structure and charge density waves of Na₂Ti₂Sb₂O

    DOE PAGES

    Tan, S. Y.; Jiang, J.; Ye, Z. R.; Niu, X. H.; Song, Y.; Zhang, C. L.; Dai, P. C.; Xie, B. P.; Lai, X. C.; Feng, D. L.

    2015-04-30

    The electronic structure of Na₂Ti₂Sb₂O single crystal is studied by photon energy and polarization dependent angle-resolved photoemission spectroscopy (ARPES). The obtained band structure and Fermi surface agree well with the band structure calculation of Na₂Ti₂Sb₂O in the non-magnetic state, which indicates that there is no magnetic order in Na₂Ti₂Sb₂O and the electronic correlation is weak. Polarization dependent ARPES results suggest the multi-band and multi-orbital nature of Na₂Ti₂Sb₂O. Photon energy dependent ARPES results suggest that the electronic structure of Na₂Ti₂Sb₂O is rather two-dimensional. Moreover, we find a density wave energy gap forms below the transition temperature and reaches 65 meV atmore » 7 K, indicating that Na₂Ti₂Sb₂O is likely a weakly correlated CDW material in the strong electron-phonon interaction regime. (author)« less

  16. Angle-resolved photoemission studies of lattice polaron formation in the cuprate Ca2CuO2Cl2

    SciTech Connect

    Shen, K.M.

    2010-05-03

    To elucidate the nature of the single-particle excitations in the undoped parent cuprates, we have performed a detailed study of Ca{sub 2}CuO{sub 2}Cl{sub 2} using photoemission spectroscopy. The photoemission lineshapes of the lower Hubbard band are found to be well-described by a polaron model. By comparing the lineshape and temperature dependence of the lower Hubbard band with additional O 2p and Ca 3p states, we conclude that the dominant broadening mechanism arises from the interaction between the photohole and the lattice. The strength of this interaction was observed to be strongly anisotropic and may have important implications for the momentum dependence of the first doped hole states.

  17. PHOTOEMISSION PROPERTIES OF LEAD.

    SciTech Connect

    SMEDLEY,J.; RAO,T.; WARREN,J.; SEKUTOWICZ,J.; LEFFERTS,R.; LIPSKI,A.

    2004-07-05

    In this paper we present a study of the photoemission properties of lead at several UV wavelengths, including a study of the damage threshold of electroplated lead under laser cleaning. A quantum efficiency in excess of 0.1% has been achieved for a laser cleaned, electroplated lead sample with a laser wavelength of 193 nm. Niobium cathodes have been measured for comparison, and lead is found to be a superior photoemitter for all measured wavelengths.

  18. Photoemission study of the adsorption of nitric oxide on gallium arsenide (110) at low temperature

    SciTech Connect

    Bermudez, V.M. ); Williams, R.T. Physics Department, Wake Forest University, Winston-Salem, NC ); Williams, G.P. Jr.; Rowe, M.W.; Liu, H.; Wu, A. ); Sadeghi, H.R.; Rife, J.C. )

    1990-05-01

    Photoelectron spectroscopy with synchrotron radiation has been used to study changes in the region of the valence band and Ga and As 3{ital d} core levels of GaAs (110) resulting from exposure to nitric oxide (NO) at substrate temperatures of 40--140 K. Up to about 60 K, NO physisorbs. Thermal and photochemical effects have been observed during annealing of the adsorbed layer or irradiation by the monochromatized synchrotron radiation beam. At about 70 K, a distinct molecular species forms along with adsorbed O. This species, which desorbs and/or dissociates above about 90 K, is identified as nitrous oxide (N{sub 2}O ) on the basis of comparison with similar data for N{sub 2}O condensed on GaAs. Pre-adsorbed O inhibits N{sub 2}O formation, suggesting that the GaAs surface participates actively in the process. Above about 100 K, only O adsorption is observed, occurring by a mechanism different from that leading to O adsorption at lower temperature.

  19. Hard and soft x-ray standing-wave photoelectron spectroscopy and angle-resolved photoemission spectroscopy study of LaNiO3/SrTiO 3 superlattice and its interfaces

    NASA Astrophysics Data System (ADS)

    Eiteneer, Daria N.

    Abstract Many classes of materials that exhibit interesting characteristics in the modulation of the electronic and magnetic properties when they are made of more than one compound, often arranged in multilayers and superlattices. In such cases, the electronic, electric, and magnetic properties of the multilayer, as well as their densities-of-states, are vastly different from the properties of the constituent materials, with the most important features often located at the interfaces. Specifically, perovskite nickelates are examples of materials that lie at the heart of correlated electron physics. Prior studies have been done on superlattices that contain multilayers of two perovskites. Specifically, it has been shown that LaNiO3 (LNO) undergoes a Mott metal-insulator transition when sandwiched between the layers of SrTiO3 (STO). However, even with prior theoretical simulations and experimental studies, no conclusion has been reached so far as to the exact reason for such a transition. To further the investigation of these ideas, we are undertaking a detailed study of the electronic structure of a LaNiO3/SrTiO3 superlattice with 10 repeats of [4 unit-cell LNO/3 unit-cell STO] bilayer grown on an (LaAlO3)0.3(Sr2AlTaO6)0.7 substrate. To provide a complete characterization of this superlattice, it is crucial to characterize the core levels of the atoms at the interface, as well as to measure the depth-dependent density of states and the element-specific magnetization through the interface. The standing-wave photoemission technique provides a unique capability for characterizing the LNO/STO interfaces by depth-resolving the electronic structure of the superlattice, particularly in its momentum-resolving form of standing-wave angle-resolved photoemission using soft x-rays in the ca. 1 keV regime. The main advantages of SW-XPS are its non-destructiveness, large effective attenuation length, and the enhanced depth resolution for buried interfaces via standing

  20. In Vacuo Photoemission Studies of Platinum Atomic Layer Deposition Using Synchrotron Radiation.

    PubMed

    Geyer, Scott M; Methaapanon, Rungthiwa; Shong, Bonggeun; Pianetta, Piero A; Bent, Stacey F

    2013-01-01

    The mechanism of platinum atomic layer deposition using (methylcyclopentadienyl)trimethylplatinum and oxygen is investigated with in vacuo photoemission spectroscopy at the Stanford Synchrotron Radiation Lightsource. With this surface-sensitive technique, the surface species following the Pt precursor half cycle and the oxygen counter-reactant half cycle can be directly measured. We observed significant amounts of carbonaceous species following the Pt precursor pulse, consistent with dehydrogenation of the precursor ligands. Significantly more carbon is observed when deposition is carried out in the thermal decomposition temperature region. The carbonaceous layer is removed during the oxygen counter reactant pulse, and the photoemission spectrum shows that a layer of adsorbed oxygen remains on the surface as previously predicted. PMID:26291229

  1. Hard and soft x-ray standing-wave photoelectron spectroscopy and angle-resolved photoemission spectroscopy study of LaNiO3/SrTiO 3 superlattice and its interfaces

    NASA Astrophysics Data System (ADS)

    Eiteneer, Daria N.

    Abstract Many classes of materials that exhibit interesting characteristics in the modulation of the electronic and magnetic properties when they are made of more than one compound, often arranged in multilayers and superlattices. In such cases, the electronic, electric, and magnetic properties of the multilayer, as well as their densities-of-states, are vastly different from the properties of the constituent materials, with the most important features often located at the interfaces. Specifically, perovskite nickelates are examples of materials that lie at the heart of correlated electron physics. Prior studies have been done on superlattices that contain multilayers of two perovskites. Specifically, it has been shown that LaNiO3 (LNO) undergoes a Mott metal-insulator transition when sandwiched between the layers of SrTiO3 (STO). However, even with prior theoretical simulations and experimental studies, no conclusion has been reached so far as to the exact reason for such a transition. To further the investigation of these ideas, we are undertaking a detailed study of the electronic structure of a LaNiO3/SrTiO3 superlattice with 10 repeats of [4 unit-cell LNO/3 unit-cell STO] bilayer grown on an (LaAlO3)0.3(Sr2AlTaO6)0.7 substrate. To provide a complete characterization of this superlattice, it is crucial to characterize the core levels of the atoms at the interface, as well as to measure the depth-dependent density of states and the element-specific magnetization through the interface. The standing-wave photoemission technique provides a unique capability for characterizing the LNO/STO interfaces by depth-resolving the electronic structure of the superlattice, particularly in its momentum-resolving form of standing-wave angle-resolved photoemission using soft x-rays in the ca. 1 keV regime. The main advantages of SW-XPS are its non-destructiveness, large effective attenuation length, and the enhanced depth resolution for buried interfaces via standing

  2. Resonant photoemission study of the 4f spectral function of cerium in Ce/Fe(100) interfaces

    SciTech Connect

    Witkowski, N.; Bertran, F.; Gourieux, T.; Kierren, B.; Malterre, D.; Panaccione, G. |

    1997-11-01

    In this paper, we present a resonant photoemission study of the cerium 4f spectral function in Ce/Fe(100) interfaces. By covering cerium ultrathin films with lanthanum, we completely suppress the surface contribution of the spectra. Then we show that the cerium atoms at the interface are in an intermediate valent state, whereas the f{sup 1} configuration is stabilized in the top layer. This method allows us to obtain the genuine 4f spectral function of the interface, and could be extended to a study of Ce-based compounds. {copyright} {ital 1997} {ital The American Physical Society}

  3. Chemical Bonding in Tl Cuprates Studied by X-Ray Photoemission

    SciTech Connect

    Lao, J.Y.; Overmyer, D.L.; Ren, Z.F.; Siegal, M.P.; Vasquez, R.P.; Wang, J.H.

    1999-04-05

    Epitaxial thin films of the Tl cuprate superconductors Tl{sub 2}Ba{sub 2}CaCu{sub 2}O{sub 8}, Tl{sub 2}Ba{sub 2}Ca{sub 2}Cu{sub 3}O{sub 10}, and TL{sub 0.78}Bi{sub 0.22}Ba{sub 0.4}Sr{sub 1.6}Ca{sub 2}Cu{sub 3}O{sub 9{minus}{delta}} are studied with x-ray photoemission spectroscopy. These data, together with previous measurements in this lab of Tl{sub 2}Ba{sub 2}CuO{sub 6+{delta}} and TlBa{sub 2}CaCu{sub 2}O{sub 7{minus}{delta}}, comprise a comprehensive data set for a comparative study of Tl cuprates with a range of chemical and electronic properties. In the Cu 2p spectra, a larger energy separation between the satellite and main peaks (E{sub s}-E{sub m}) and a lower intensity ratio (I{sub s}/I{sub m}) are found to correlate with higher values of T{sub c}. Analysis of these spectra within a simple configuration interaction model suggests that higher values of T{sub c} are related to low values of the O 2p {r_arrow} Cu 3d charge transfer energy. In the O 1s region, a smaller bond length between Ba and Cu-O planar oxygen is found to correlate with a lower binding energy for the signal associated with Cu-O bonding, most likely resulting from the increased polarization screening by Ba{sup 2+} ions. For samples near optimum doping, maximum T{sub c} is observed to occur when the Tl 4f{sub 7/2} binding energy is near 117.9 eV, which is near the middle of the range of values observed for Tl cuprates. Higher Tl 4f{sub 7/2} binding energies, corresponding to formal oxidation states nearer Tl{sup 1+}, are also found to correlate with longer bond lengths between Ba and Tl-O planar oxygen, and with higher binding energies of the O 1s signal associated with Tl-O bonding.

  4. Electronic structure of ultrathin Fe films on TiO[sub 2](110) studied with soft-x-ray photoelectron spectroscopy and resonant photoemission

    SciTech Connect

    Diebold, U. Department of Physics, Tulane University, New Orleans, Louisiana 70118-5698 ); Tao, H. ); Shinn, N.D. ); Madey, T.E. )

    1994-11-15

    We report on soft-x-ray photoelectron spectroscopy (SXPS) of a TiO[sub 2](110) surface during deposition of Fe in the monolayer regime. At low fractional monolayer coverages, the adsorbed Fe atoms are oxidized and Ti cations at the interface become reduced due to Fe adsorption. SXPS from shallow core levels and valence bands show that Fe starts to exhibit metallic character at a coverage of approximately 0.7 equivalent monolayers. Two well separated defect states appear in the band gap of TiO[sub 2] at iron coverages well below one monolayer. We use resonant photoemission to obtain information on the partial density of states, and we assign these defect states as being Fe-derived and Ti-derived states, located at the Fe and Ti sites, respectively. We suggest that a position change of oxygen is involved in the bonding of Fe on the TiO[sub 2](110) surface.

  5. In-situ X-ray Photoemission Spectroscopy Study of Atomic Layer Deposition of TiO2 on Silicon Substrate

    NASA Astrophysics Data System (ADS)

    Youb Lee, Seung; Jeon, Cheolho; Kim, Seok Hwan; Kim, Yooseok; Jung, Woosung; An, Ki-Seok; Park, Chong-Yun

    2012-03-01

    In-situ X-ray photoemission spectroscopy (XPS) has been used to investigate the initial stages of TiO2 growth on a Si(001) substrate by atomic layer deposition (ALD). The core level spectra of Si 2p, C 1s, O 1s, and Ti 2p were measured at every half reaction in the titanium tetra-isopropoxide (TTIP)-H2O ALD process. The ligand exchange reactions were verified using the periodic oscillation of the C 1s concentration, as well as changes in the hydroxyl concentration. XPS analysis revealed that Ti2O3 and Si oxide were formed at the initial stages of TiO2 growth. A stoichiometric TiO2 layer was dominantly formed after two cycles and was chemically saturated after four cycles.

  6. In-situ X-ray Photoemission Spectroscopy Study of Atomic Layer Deposition of TiO2 on Silicon Substrate

    NASA Astrophysics Data System (ADS)

    Lee, Seung Youb; Jeon, Cheolho; Kim, Seok Hwan; Kim, Yooseok; Jung, Woosung; An, Ki-Seok; Park, Chong-Yun

    2012-03-01

    In-situ X-ray photoemission spectroscopy (XPS) has been used to investigate the initial stages of TiO2 growth on a Si(001) substrate by atomic layer deposition (ALD). The core level spectra of Si 2p, C 1s, O 1s, and Ti 2p were measured at every half reaction in the titanium tetra-isopropoxide (TTIP)--H2O ALD process. The ligand exchange reactions were verified using the periodic oscillation of the C 1s concentration, as well as changes in the hydroxyl concentration. XPS analysis revealed that Ti2O3 and Si oxide were formed at the initial stages of TiO2 growth. A stoichiometric TiO2 layer was dominantly formed after two cycles and was chemically saturated after four cycles.

  7. A (4x2) reconstruction of CuInSe{sub 2} (001) studied by low-energy electron diffraction and soft x-ray photoemission spectroscopy

    SciTech Connect

    Deniozou, Th.; Esser, N.; Schulmeyer, Th.; Hunger, R.

    2006-01-30

    Clean and flat (001) surfaces of CuInSe{sub 2}/GaAs grown by molecular-beam epitaxy could be prepared by the combination of a Se capping and decapping process and subsequent Ar{sup +} ion sputtering and annealing. The formation of a (4x2) reconstruction was observed with low-energy electron diffraction. Soft x-ray photoemission spectroscopy was performed on the prepared surfaces and revealed surface core-level binding energy shifts in the Cu 2p{sub 3/2}, Se 3d, and In 4d levels which are associated with surface atoms. The structure model of a combined metal adatom-Se dimer structure is proposed to refer to the (4x2) reconstruction.

  8. Photoemission Studies of Quantum Confinement in Nonmagnetic/Magnetic Film and Wedge Structures

    NASA Astrophysics Data System (ADS)

    Li, Dongqi

    1996-03-01

    The field of giant magnetoresistance (GMR) has generated much excitement. Photoemission provides a powerful tool to address some of the outstanding, yet fundamental issues in this field. It probes the spin-polarized metallic quantum well (QW) states in GMR materials, which underlie the oscillatory exchange coupling.(J. E. Ortega and F. J. Himpsel, Phys. Rev. Lett. 69, 844 (1992).) Angle- and spin-resolved photoemission experiments were performed at NSLS undulator beamline U5. For the Cu/Co system, both sp- and d-band derived minority-spin QW states of Cu overlayers on Co(100) grown on a Cu(100) substrate are identified. Also, the degree of confinement of these states is quantified by inserting a Co wedge to form a barrier between the Cu overlayer and substrate.(Dongqi Li, et al., Phys. Rev. B 51, 7195 (1995).) The characteristic length scale for the quantum confinement coincides with that known to influence the GMR. This provides a glimpse into understanding the importance of spin-dependent interfacial scattering. Another basic issue still under debate is the origin of the "long-period" oscillation in systems such as Fe/Cr. The QW picture is recognized as equivalent to the RKKY description of the coupling periodicity. There are three regions of the Cr Fermi surface whose spanning vectors can explain the periodicity, and thus, where the characteristic QW states might emerge: (i) the nested region (due to aliasing); (ii) the N-centered ellipse; or (iii) the d-derived "lens". Angle- resolved photoemission provides a novel methodology to search k-space for the features responsible for the coupling. Work done in collaboration with S. D. Bader, D.-J. Huang, P. D. Johnson, J. E. Mattson, J. Pearson, E. Vescovo. * Supported by DOE BES-MS under #W-31-109-ENG-38 and ONR under #N-00014- 94-F-0085.

  9. A Mechanistic Study of CO2 Reduction at the Interface of a Gallium Phosphide (GaP) Surface using Core-level Spectroscopy

    SciTech Connect

    Flynn, Kristen

    2015-08-18

    Carbon dioxide (CO2) emission into the atmosphere has increased tremendously through burning of fossil fuels, forestry, etc.. The increased concentration has made CO2 reductions very attractive though the reaction is considered uphill. Utilizing the sun as a potential energy source, CO2 has the possibility to undergo six electron and four proton transfers to produce methanol, a useable resource. This reaction has been shown to occur selectively in an aqueous pyridinium solution with a gallium phosphide (GaP) electrode. Though this reaction has a high faradaic efficiency, it was unclear as to what role the GaP surface played during the reaction. In this work, we aim to address the fundamental role of GaP during the catalytic conversion, by investigating the interaction between a clean GaP surface with the reactants, products, and intermediates of this reaction using X-ray photoelectron spectroscopy. We have determined a procedure to prepare atomically clean GaP and our initial CO2 adsorption studies have shown that there is evidence of chemisorption and reaction to form carbonate on the clean surface at LN2 temperatures (80K), in contrast to previous theoretical calculations. These findings will enable future studies on CO2 catalysis.

  10. A Mechanistic Study of CO2 Reduction at the Interface of a Gallium Phosphide (GaP) Surface using Core-level Spectroscopy - Oral Presentation

    SciTech Connect

    Flynn, Kristen

    2015-08-19

    Carbon dioxide (CO2) emission into the atmosphere has increased tremendously through burning of fossil fuels, forestry, etc.. The increased concentration has made CO2 reductions very attractive though the reaction is considered uphill. Utilizing the sun as a potential energy source, CO2 has the possibility to undergo six electron and four proton transfers to produce methanol, a useable resource. This reaction has been shown to occur selectively in an aqueous pyridinium solution with a gallium phosphide (GaP) electrode. Though this reaction has a high faradaic efficiency, it was unclear as to what role the GaP surface played during the reaction. In this work, we aim to address the fundamental role of GaP during the catalytic conversion, by investigating the interaction between a clean GaP surface with the reactants, products, and intermediates of this reaction using X-ray photoelectron spectroscopy. We have determined a procedure to prepare atomically clean GaP and our initial CO2 adsorption studies have shown that there is evidence of chemisorption and reaction to form carbonate on the clean surface at LN2 temperatures (80K), in contrast to previous theoretical calculations. These findings will enable future studies on CO2 catalysis.

  11. Superconducting Gap Anisotropy and Quasiparticle Interactions: A Doping Dependent Photoemission Study

    SciTech Connect

    Mesot, J.; Norman, M.R.; Campuzano, J.C.; Mesot, J.; Campuzano, J.C.; Fretwell, H.M.; Kaminski, A.; Ding, H.; Randeria, M.; Paramekanti, A.; Takeuchi, T.; Yokoya, T.; Sato, T.; Takahashi, T.; Mochiku, T.; Kadowaki, K.

    1999-07-01

    Comparing photoemission measurements on Bi2212 with penetration depth data, we show that a description of the nodal excitations of the d -wave superconducting state in terms of noninteracting quasiparticles is inadequate, and we estimate the magnitude and doping dependence of the Landau interaction parameter which renormalizes the linear T contribution to the superfluid density. Furthermore, although consistent with d -wave symmetry, the gap with underdoping cannot be fit by the simple cos k{sub x}{minus}cos k{sub y} form, which suggests an increasing importance of long range interactions as the insulator is approached. {copyright} {ital 1999} {ital The American Physical Society }

  12. Reverse-engineering the atomic-scale structure of the TiO2/N3 interface in dye-sensitized solar cells using O1s core-level shifts

    NASA Astrophysics Data System (ADS)

    Patrick, Christopher; Giustino, Feliciano

    2011-03-01

    Dye-sensitized solar cells employing mesoporous titania films sensitized with ruthenium-based dyes have shown consistently good performance over the past two decades. Understanding the process of charge injection in these devices requires accurate atomistic models of the interface between the light-absorbing dye and the semiconducting substrate. Despite considerable efforts devoted to the experimental and theoretical investigation of such interfaces, their atomistic nature remains controversial. In this work we pursue a novel computational approach to the study of the semiconductor/dye interface which does not rely on the calculated adsorption energies. In our approach we reverse-engineer photoemission data through the first-principles calculation of O1s core-level spectra for a number of candidate interface models. Our calculations allow us to discard some of the adsorption geometries previously proposed and point to an interface model which reconciles conflicting assignments based either on photoemission or infrared data.

  13. Synchrotron-radiation photoemission study of CdS/CuInSe2 heterojunction formation

    NASA Astrophysics Data System (ADS)

    Nelson, Art J.; Gebhard, Steve; Rockett, Angus; Colavita, Elio; Engelhardt, Mike; Höchst, Hartmut

    1990-10-01

    Synchrotron-radiation soft-x-ray photoemission spectroscopy was used to investigate the development of the electronic structure at the CdS/CuInSe2 heterojunction interface. CdS overlayers were deposited in steps on single-crystal p- and n-type CuInSe2 at 250 °C. Results indicate that the CdS grows in registry with the substrate, initially in a two-dimensional growth mode followed by three-dimensional island growth as is corroborated by reflection high-energy electron-diffraction analysis. Photoemission measurements were acquired after each growth in order to observe changes in the valence-band electronic structure as well as changes in the In 4d, Se 3d, Cd 4d, and S 2p core lines. The results were used to correlate the interface chemistry with the electronic structure at these interfaces and to directly determine the CdS/CuInSe2 heterojunction valence-band discontinuity and the consequent heterojunction band diagram. These results show that the Katnani-Margaritondo method is unreliable in determining offsets for heterojunctions where significant Fermi-level pinning may occur and where the local structure and chemistry of the interface depends strongly on the specific heterojunction.

  14. Surface core-level shifts and atomic coordination at a stepped W(110) surface

    SciTech Connect

    Riffe, D.M.; Kim, B.; Erskine, J.L. ); Shinn, N.D. )

    1994-11-15

    Core-level 4[ital f][sub 7/2] photoemission spectra have been measured from a single, bifacial W crystal, which has both a flat W(110) and a vicinal, stepped W(110) [W(320)] surface. This procedure reduces uncertainties in the quantitative description of peaks in the spectra from W(320). Various analyses, including nonlinear least-squares curve fitting, show that the average surface core-level shift (SCS) for W(320) is only [similar to][minus]140 meV, compared to [minus]310 meV for W(110) and that, at a maximum, only two of five terrace rows are isoelectronic to W(110) surface atoms. The absence of a large SCS for the step-edge atoms contradicts earlier interpretations of W(320) core-level spectra and departs significantly from expectations based on atomic-coordination models or tight-binding calculations of a bulk truncated surface. We suggest that systematic errors are responsible for the differences in reported core-level shifts for W(320). Implications of possible step-edge-driven atomic rearrangements are discussed.

  15. Electronic structure of LiCoO{sub 2} thin films: A combined photoemission spectroscopy and density functional theory study

    SciTech Connect

    Ensling, David; Thissen, Andreas; Laubach, Stefan; Schmidt, Peter C.; Jaegermann, Wolfram

    2010-11-15

    The electronic properties of LiCoO{sub 2} have been studied by theoretical band-structure calculations (using density functional theory) and experimental methods (photoemission). Synchrotron-induced photoelectron spectroscopy, resonant photoemission spectroscopy (ResPES), and soft x-ray absorption (XAS) have been applied to investigate the electronic structure of both occupied and unoccupied states. High-quality PES spectra were obtained from stoichiometric and highly crystalline LiCoO{sub 2} thin films deposited ''in situ'' by rf magnetron sputtering. An experimental approach of separating oxygen- and cobalt-derived (final) states by ResPES in the valence-band region is presented. The procedure takes advantage of an antiresonant behavior of cobalt-derived states at the 3p-3d excitation threshold. Information about the unoccupied density of states has been obtained by O K XAS. The structure of the Co L absorption edge is compared to semiempirical charge-transfer multiplet calculations. The experimental results are furthermore compared with band-structure calculations considering three different exchange potentials [generalized gradient approximation (GGA), using a nonlocal Hubbard U (GGA+U) and using a hybrid functional (Becke, three-parameter, Lee-Yang-Parr [B3LYP])]. For these different approaches total density of states and partial valence-band density of states have been investigated. The best qualitative agreement with experimental results has been obtained by using a GGA+U functional with U=2.9 eV.

  16. Photoemission and near-edge X-ray absorption fine structure studies of the bacterial surface protein layer of Bacillus sphaericus NCTC 9602.

    PubMed

    Vyalikh, Denis V; Kirchner, Alexander; Danzenbächer, Steffen; Dedkov, Yuriy S; Kade, Andreas; Mertig, Michael; Molodtsov, Serguei L

    2005-10-01

    The electronic structure of the regular, two-dimensional bacterial surface protein layer of Bacillus sphaericus NCTC 9602 has been examined by photoemission (PE) and near-edge X-ray absorption fine structure (NEXAFS) spectroscopy. Both the O 1s and the N 1s core-level PE spectra show a single structure, whereas the C 1s core-level spectrum appears manifold, suggesting similar chemical states for each oxygen atom and also for each nitrogen atom, while carbon atoms exhibit a range of chemical environments in the different functional groups of the amino acids. This result is supported by the element-specific NEXAFS spectra of the unoccupied valence electronic states, which exhibit a series of characteristic NEXAFS peaks that can be assigned to particular molecular orbitals of the amino acids by applying a phenomenological building-block model. The relative contributions of the C-O, C-N, and C-C bond originating signals into the C 1s PE spectrum are in good agreement with the number ratios of the corresponding bonds calculated from the known primary structure of the bacterial surface protein. First interpretation of the PE spectrum of the occupied valence states is achieved on the basis of electronic density-of-states calculations performed for small peptides. It was found that mainly the pi clouds of the aromatic rings contribute to both the lowest unoccupied and the highest occupied molecular orbitals.

  17. Angle-resolved photoemission extended fine structure

    SciTech Connect

    Barton, J.J.

    1985-03-01

    Measurements of the Angle-Resolved Photoemission Extended Fine Structure (ARPEFS) from the S(1s) core level of a c(2 x 2)S/Ni(001) are analyzed to determine the spacing between the S overlayer and the first and second Ni layers. ARPEFS is a type of photoelectron diffraction measurement in which the photoelectron kinetic energy is swept typically from 100 to 600 eV. By using this wide range of intermediate energies we add high precision and theoretical simplification to the advantages of the photoelectron diffraction technique for determining surface structures. We report developments in the theory of photoelectron scattering in the intermediate energy range, measurement of the experimental photoemission spectra, their reduction to ARPEFS, and the surface structure determination from the ARPEFS by combined Fourier and multiple-scattering analyses. 202 refs., 67 figs., 2 tabs.

  18. Angle resolved photoemission study of the strongly correlated metal V2O3

    NASA Astrophysics Data System (ADS)

    Lo Vecchio, Irene; Denlinger, Jonathan D.; Krupin, Oleg; Kim, Bumjoon; Metcalf, Patricia; Lupi, Stefano; Allen, James W.; Lanzara, Alessandra

    V2O3 is often considered as the textbook example for the Mott metal-insulator transition. It has been the playground for multiple theoretical approaches and attempts to describe its metallic ground state for half a century. However, the experimental electronic structure is still unknown because of difficulties related to the three-dimensional character of the Fermi surface and the inhomogeneous cleavage of single crystals. Here we reveal for the first time the band structure of V2O3 using angle resolved photoemission spectroscopy. Direct comparison with theory is presented highlighting the important role of electron correlation for the physics of this material. Experiments at the Advanced Light Source were supported by the U.S. DOE Basic Energy Sciences (DE-AC02-05CH11231).

  19. Photoemission Study of VO2 Above and Below the Transition Temperature

    NASA Astrophysics Data System (ADS)

    Moreschini, Luca; Chang, Young Jun; Innocenti, Davide; Walter, Andrew L.; Denlinger, Jonathan; Bostwick, Aaron; Rotenberg, Eli

    2012-02-01

    Angle-resolved photoemission (ARPES) experiments on VO2 have traditionally been hindered by the quality of cleaved single crystals. The lack of a clear metal-insulator transition (MIT) in low photon energy measurements has even lead to the assumption of a surface region with a different electronic structure. WIth the in situ pulsed-laser-deposition (PLD) system available on beamline 7.0.1 at the Advanced Light Source we have grown VO2(001) films on a TiO2 substrate and measured the band structure above and below the transition temperature. We discuss our results in comparison with the available calculations, and we show that the MIT is clearly visible for photon energies within the UV range.

  20. Oliver E. Buckley Condensed Matter Prize Talk: High-resolution Photoemission Studies of the High Tc Superconductors

    NASA Astrophysics Data System (ADS)

    Johnson, Peter

    2011-03-01

    In the last decade, high resolution angle-resolved photoelectron spectroscopy has evolved into one of the most powerful probes of the electronic structure of condensed matter systems. This development reflects new technological advances coupled to the enormous research effort devoted to the study of strongly correlated systems, particularly the high Tc cuprate superconductors. Two decades after their initial discovery the latter still present some of the biggest challenges for materials science. In this talk we review some of the developments in new instrumentation and analysis techniques in photoemission and include discussion of both self-energy effects and Fermi surface studies. In the latter case, the discussion will focus on the pseudogap phase of the underdoped cuprates with particular reference to an observed particle-hole asymmetry and the possibility of hole pockets. Work at Brookhaven is supported by the U.S. Department of Energy.

  1. X-ray photoemission study of the infinite-layer cuprate superconductor Sr(0.9) La (0.1) CuO(2)

    NASA Technical Reports Server (NTRS)

    Vasquez, R. P.; Jung, C. U.; Kim, J. Y.; Kim, M. S.; Lee, S. Y.; Lee, S. I.

    2001-01-01

    The electron-doped infinite-layer superconductor Sr(0.9)La(0.1) CuO(2) is studied with x-ray photoemission spectroscopy (XPS). A nonaqueous chemical etchant is shown to effectively remove contaminants and to yield surfaces from which signals intrinsic to the superconductor dominate.

  2. High-resolution angle-resolved photoemission study of UN and USb; Dual character of 5f electrons

    NASA Astrophysics Data System (ADS)

    Ito, T.; Kumigashira, H.; Souma, S.; Takahashi, T.; Suzuki, T.

    2001-05-01

    We have performed high-resolution angle-resolved photoemission spectroscopy on UN and USb to study the electronic structure near the Fermi level ( EF) and the nature of U 5f electrons. We found that the pnictogen (N and Sb) p bands are fully occupied in contrast with Ce monopnictides and shows a good qualitative agreement with the band calculation by treating the U 5f states as bands. On the other hand, we have not observed dispersive U 5f bands near EF predicted by the band calculation, instead we found two non-dispersive bands near EF, which are assigned as the 5f 2-final-state multiplet indicative of localized U 5f states. The intensity of multiplet structure is stronger in USb than in UN. These results indicate the dual character of U 5f electrons and its difference between USb and UN.

  3. Electronic structure of rare-earth doped SrFBiS2 superconductors from photoemission spectroscopic studies

    NASA Astrophysics Data System (ADS)

    Mishra, P.; Lohani, H.; Jha, Rajveer; Awana, V. P. S.; Sekhar, B. R.

    2016-06-01

    The electronic structure study of the Rare Earth (La, Ce) doped SrFBiS2 superconductors using valence band photoemission in conjugation with the band structure calculations have been presented. The spectral features shift towards higher binding energy, consistent with the electron doping, for the doped compounds. An enhanced metallicity in addition to the shift in the Fermi level towards the conduction band occurs for the Rare Earth (RE) doped compounds. Further, the degeneracy of bands along X-M direction at valence band maximum (VBM) and conduction band minimum (CBM) is lifted due to RE doping. An enhanced spectral weight near EF accompanied by a decrease in density of states at higher binding energy occurs for the doped compounds. This unusual spectral weight shift is substantiated by the change in Fermi surface topology and reduced distortion of Bi-S plane for the doped compounds.

  4. Valence Electronic Structure of Oxygen-Modified α-Mo2C(0001) Surface:. Angle-Resolved Photoemission Study

    NASA Astrophysics Data System (ADS)

    Kato, M.; Ozawa, K.; Sato, T.; Edamoto, K.

    Adsorption of oxygen on α-Mo2C(0001) is investigated with Auger electron spectroscopy (AES), low-energy electron diffraction (LEED) and angle-resolved photoemission spectroscopy (ARPES) utilizing synchrotron radiation. It is found that C KLL Auger peak intensity does not change during O2 exposure, indicating that the depletion of C atoms does not proceed. It is deduced from ARPES and LEED results that adsorbed oxygen atoms from a well-ordered (1 × 1) lattice on the α-Mo2C(0001) surface. The ARPES study shows that oxygen adsorption induces a peculiar state around Fermi level (EF). Off-normal-emission measurements prove that the state is a half-filled metallic state.

  5. Halide-Substituted Electronic Properties of Organometal Halide Perovskite Films: Direct and Inverse Photoemission Studies.

    PubMed

    Li, Chi; Wei, Jian; Sato, Mikio; Koike, Harunobu; Xie, Zhong-Zhi; Li, Yan-Qing; Kanai, Kaname; Kera, Satoshi; Ueno, Nobuo; Tang, Jian-Xin

    2016-05-11

    Solution-processed perovskite solar cells are attracting increasing interest due to their potential in next-generation hybrid photovoltaic devices. Despite the morphological control over the perovskite films, quantitative information on electronic structures and interface energetics is of paramount importance to the optimal photovoltaic performance. Here, direct and inverse photoemission spectroscopies are used to determine the electronic structures and chemical compositions of various methylammonium lead halide perovskite films (MAPbX3, X = Cl, Br, and I), revealing the strong influence of halide substitution on the electronic properties of perovskite films. Precise control over halide compositions in MAPbX3 films causes the manipulation of the electronic properties, with a qualitatively blue shift along the I → Br → Cl series and showing the increase in ionization potentials from 5.96 to 7.04 eV and the change of transport band gaps in the range from 1.70 to 3.09 eV. The resulting light absorption of MAPbX3 films can cover the entire visible region from 420 to 800 nm. The results presented here provide a quantitative guide for the analysis of perovskite-based solar cell performance and the selection of optimal carrier-extraction materials for photogenerated electrons and holes. PMID:27101940

  6. Electronic structure of Co-Ni-Ga Heusler alloys studied by resonant photoemission

    SciTech Connect

    Baral, Madhusmita Banik, Soma Ganguli, Tapas Chakrabarti, Aparna Deb, S. K.; Thamizhavel, A.; Wadikar, Avinash; Phase, D. M.

    2014-04-24

    The electronic structures of Co{sub 2.01}Ni{sub 1.05}Ga{sub 0.94} and Co{sub 1.76}Ni{sub 1.46}Ga{sub 0.78} Heusler alloys have been investigated by resonant photoemission spectroscopy across the 3p-3d transition of Co and Ni. For the Ni excess composition Co{sub 1.76}Ni{sub 1.46}Ga{sub 0.78}, the valence band peak shows a shift of 0.25 eV as compared to the near stoichiometric composition Co{sub 2.01}N1{sub 1.05}Ga{sub 0.94}. Also an enhancement is observed in the Ni related satellite features in the valence band for the Ni excess composition. Due to hybridization of Co and Ni 3d states in these systems, the Co and Ni 3p-3d resonance energies are found to be higher as compared to Co and Ni metals. Theoretical first principle calculation is performed to understand the features in the valence band and the shape of the resonance profile.

  7. Angle-resolved photoemission study of the Kitaev candidate α -RuCl3

    NASA Astrophysics Data System (ADS)

    Zhou, Xiaoqing; Li, Haoxiang; Waugh, J. A.; Parham, S.; Kim, Heung-Sik; Sears, J. A.; Gomes, A.; Kee, Hae-Young; Kim, Young-June; Dessau, D. S.

    2016-10-01

    α -RuCl3 has been hinted to be a spin-orbital-assisted Mott insulator in proximity to a Kitaev spin liquid state. Here we present angle-resolved photoemission measurements on single-crystal α -RuCl3 in both the pristine and electron-doped states, and combine them with Local Density Approximation (LDA)+Spin Orbital Coupling (SOC)+U calculations performed for several low-energy competing magnetically ordered states as well as the paramagnetic state. A large Mott gap is found in the measured band structure of the pristine compound that persists to more than 30 times beyond the magnetic ordering temperature, though the paramagnetic calculation shows almost no gap. Upon electron doping, spectral weight is transferred into the gap but the new states still maintain a sizable gap from the Fermi edge. These findings are most consistent with a Mott insulator with a somewhat exotic evolution out of the Mott state with both temperature and doping, likely related to unusually strong spin fluctuations.

  8. X-ray photoemission study of manganese thin films deposited on a layered semiconductor

    NASA Astrophysics Data System (ADS)

    Mirabella, F.; Parkinson, B. A.; Ghijsen, J.

    2004-02-01

    Germanium sulphide (GeS) and tin diselenide (SnSe2) present anisotropic properties due to their layered crystal structures. These crystals are composed of atomic layers interacting with each other by van der Waals forces only. Recently these materials have been used to prepare a new diluted magnetic semiconductor (DMS) by substituting some Ge or Sn atoms by manganese in the crystal lattice, forming Ge1-xMnxS and Sn1-xMnxSe2. To compare Mn behaviour within the layered crystals, Mn/GeS and Mn/SnSe2 thin films have been grown and investigated in situ by X-ray induced photoemission. Here is reported the XPS analysis of in situ grown Mn/SnSe2 for coverage ranging from sub-monolayer to thin films. The properties of these films were investigated from the structural and reactivity point of view. XPS measurements suggest that an Mn-Sn alloy is formed at the interface and that Mn atoms first deposit as an atomic netting pattern dictated by the typical structure of the SnSe2 (001) surface.

  9. Annealing effects of in-depth profile and band discontinuity in TiN/LaO/HfSiO/SiO{sub 2}/Si gate stack structure studied by angle-resolved photoemission spectroscopy from backside

    SciTech Connect

    Toyoda, S.; Kumigashira, H.; Oshima, M.; Kamada, H.; Tanimura, T.; Ohtsuka, T.; Hata, Y.; Niwa, M.

    2010-01-25

    We have investigated annealing effects on in-depth profile and band discontinuity for a metal gate/high-k gate stack structure on a Si substrate using backside angle-resolved photoemission spectroscopy with synchrotron radiation. In-depth profiles analyzed from angle-resolved photoemission spectroscopy show that La atoms diffuse through the HfSiO layer and reach interfacial SiO{sub 2} layers by rapid thermal annealing. Chemical shift of Si 2p core-level spectra suggests that there are changes in the band discontinuity at the high-k/SiO{sub 2} interface, which is well related to the V{sub th} shift based on the interface dipole model.

  10. X-ray photoemission analysis of clean and carbon monoxide-chemisorbed platinum(111) stepped surfaces using a curved crystal

    PubMed Central

    Walter, Andrew L.; Schiller, Frederik; Corso, Martina; Merte, Lindsay R.; Bertram, Florian; Lobo-Checa, Jorge; Shipilin, Mikhail; Gustafson, Johan; Lundgren, Edvin; Brión-Ríos, Anto´n X.; Cabrera-Sanfelix, Pepa; Sánchez-Portal, Daniel; Ortega, J. Enrique

    2015-01-01

    Surface chemistry and catalysis studies could significantly gain from the systematic variation of surface active sites, tested under the very same conditions. Curved crystals are excellent platforms to perform such systematics, which may in turn allow to better resolve fundamental properties and reveal new phenomena. This is demonstrated here for the carbon monoxide/platinum system. We curve a platinum crystal around the high-symmetry (111) direction and carry out photoemission scans on top. This renders the spatial core-level imaging of carbon monoxide adsorbed on a ‘tunable' vicinal surface, allowing a straightforward visualization of the rich chemisorption phenomenology at steps and terraces. Through such photoemission images we probe a characteristic elastic strain variation at stepped surfaces, and unveil subtle stress-release effects on clean and covered vicinal surfaces. These results offer the prospect of applying the curved surface approach to rationally investigate the chemical activity of surfaces under real pressure conditions. PMID:26561388

  11. X-ray photoemission analysis of clean and carbon monoxide-chemisorbed platinum(111) stepped surfaces using a curved crystal

    DOE PAGES

    Walter, Andrew L.; Schiller, Frederik; Corso, Martina; Merte, Lindsay R.; Bertram, Florian; Lobo-Checa, Jorge; Shipilin, Mikhail; Gustafson, Johan; Lundgren, Edvin; Brión-Ríos, Anto´n X.; et al

    2015-11-12

    Surface chemistry and catalysis studies could significantly gain from the systematic variation of surface active sites, tested under the very same conditions. Curved crystals are excellent platforms to perform such systematics, which may in turn allow to better resolve fundamental properties and reveal new phenomena. This is demonstrated here for the carbon monoxide/platinum system. We curve a platinum crystal around the high-symmetry (111) direction and carry out photoemission scans on top. This renders the spatial core-level imaging of carbon monoxide adsorbed on a 'tunable' vicinal surface, allowing a straightforward visualization of the rich chemisorption phenomenology at steps and terraces. Throughmore » such photoemission images we probe a characteristic elastic strain variation at stepped surfaces, and unveil subtle stress-release effects on clean and covered vicinal surfaces. Lastly, these results offer the prospect of applying the curved surface approach to rationally investigate the chemical activity of surfaces under real pressure conditions.« less

  12. X-ray photoemission analysis of clean and carbon monoxide-chemisorbed platinum(111) stepped surfaces using a curved crystal

    SciTech Connect

    Walter, Andrew L.; Schiller, Frederik; Merte, Lindsay R.; Bertram, Florian; Lobo-Checa, Jorge; Gustafson, Johan; Lundgren, Edvin; Brión-Ríos, Anto´n X.; Cabrera-Sanfelix, Pepa; Sánchez-Portal, Daniel

    2015-11-12

    Surface chemistry and catalysis studies could significantly gain from the systematic variation of surface active sites, tested under the very same conditions. Curved crystals are excellent platforms to perform such systematics, which may in turn allow to better resolve fundamental properties and reveal new phenomena. This is demonstrated here for the carbon monoxide/platinum system. We curve a platinum crystal around the high-symmetry (111) direction and carry out photoemission scans on top. This renders the spatial core-level imaging of carbon monoxide adsorbed on a 'tunable' vicinal surface, allowing a straightforward visualization of the rich chemisorption phenomenology at steps and terraces. Through such photoemission images we probe a characteristic elastic strain variation at stepped surfaces, and unveil subtle stress-release effects on clean and covered vicinal surfaces. Lastly, these results offer the prospect of applying the curved surface approach to rationally investigate the chemical activity of surfaces under real pressure conditions.

  13. Uranium passivation by C+ implantation: a photoemission and secondary ion mass spectrometry study

    SciTech Connect

    Nelson, A J; Felter, T E; Wu, K J; Evans, C; Ferreira, J; Siekhaus, W; McLean, W

    2005-01-20

    Implantation of 33 keV C{sup +} ions into polycrystalline U{sup 238} with a dose of 4.3 x 10{sup 17} cm{sup -2} produces a physically and chemically modified surface layer that prevents further air oxidation and corrosion. X-ray photoelectron spectroscopy and secondary ion mass spectrometry were used to investigate the surface chemistry and electronic structure of this C{sup +} ion implanted polycrystalline uranium and a non-implanted region of the sample, both regions exposed to air for more than a year. In addition, scanning electron microscopy was used to examine and compare the surface morphology of the two regions. The U 4f, O 1s and C 1s core-level and valence band spectra clearly indicate carbide formation in the modified surface layer. The time-of-flight secondary ion mass spectrometry depth profiling results reveal an oxy-carbide surface layer over an approximately 200 nm thick UC layer with little or no residual oxidation at the carbide layer/U metal transitional interface.

  14. Photoemission and LEED study of the Sn/Rh(111) surface--early oxidation steps and thermal stability.

    PubMed

    Hanyš, Petr; Píš, Igor; Mašek, Karel; Sutara, František; Matolín, Vladimír; Nehasil, Václav

    2012-01-11

    We have deposited two monolayers of Sn onto Rh(111) single crystal. After the deposition, no ordered structure was revealed by low energy electron diffraction (LEED). We oxidized the obtained system in a low-pressure oxygen atmosphere at 420 K. The oxidized sample was then gradually heated to study the thermal stability of the oxide layer. We characterized the system by synchrotron radiation stimulated photoelectron spectroscopy and LEED. Valence band and core level photoelectron spectra of rhodium, tin and oxygen were used to study the oxidation of the Sn-Rh(111) surface and its behaviour upon annealing. A low stoichiometric oxide of Sn was created on the surface. The oxidation process did not continue towards creation of SnO(2) with higher oxygen dose. The annealing at 970 K caused decomposition of the surface oxide of Sn and creation of an ordered (√3 × √3)R30° Sn-Rh(111) surface alloy. PMID:22095587

  15. Vacuum space charge effects in sub-picosecond soft X-ray photoemission on a molecular adsorbate layer

    DOE PAGES

    Dell'Angela, M.; Anniyev, T.; Beye, M.; Coffee, R.; Föhlisch, A.; Gladh, J.; Kaya, S.; Katayama, T.; Krupin, O.; Nilsson, A.; et al

    2015-03-01

    Vacuum space charge-induced kinetic energy shifts of O 1s and Ru 3d core levels in femtosecond soft X-ray photoemission spectra (PES) have been studied at a free electron laser (FEL) for an oxygen layer on Ru(0001). We fully reproduced the measurements by simulating the in-vacuum expansion of the photoelectrons and demonstrate the space charge contribution of the high-order harmonics in the FEL beam. Employing the same analysis for 400 nm pump-X-ray probe PES, we can disentangle the delay dependent Ru 3d energy shifts into effects induced by space charge and by lattice heating from the femtosecond pump pulse.

  16. Core level binding energies of functionalized and defective graphene.

    PubMed

    Susi, Toma; Kaukonen, Markus; Havu, Paula; Ljungberg, Mathias P; Ayala, Paola; Kauppinen, Esko I

    2014-01-01

    X-ray photoelectron spectroscopy (XPS) is a widely used tool for studying the chemical composition of materials and it is a standard technique in surface science and technology. XPS is particularly useful for characterizing nanostructures such as carbon nanomaterials due to their reduced dimensionality. In order to assign the measured binding energies to specific bonding environments, reference energy values need to be known. Experimental measurements of the core level signals of the elements present in novel materials such as graphene have often been compared to values measured for molecules, or calculated for finite clusters. Here we have calculated core level binding energies for variously functionalized or defected graphene by delta Kohn-Sham total energy differences in the real-space grid-based projector-augmented wave density functional theory code (GPAW). To accurately model extended systems, we applied periodic boundary conditions in large unit cells to avoid computational artifacts. In select cases, we compared the results to all-electron calculations using an ab initio molecular simulations (FHI-aims) code. We calculated the carbon and oxygen 1s core level binding energies for oxygen and hydrogen functionalities such as graphane-like hydrogenation, and epoxide, hydroxide and carboxylic functional groups. In all cases, we considered binding energy contributions arising from carbon atoms up to the third nearest neighbor from the functional group, and plotted C 1s line shapes by using experimentally realistic broadenings. Furthermore, we simulated the simplest atomic defects, namely single and double vacancies and the Stone-Thrower-Wales defect. Finally, we studied modifications of a reactive single vacancy with O and H functionalities, and compared the calculated values to data found in the literature.

  17. Nondipole Photoemission from Chiral Enantiomers of Camphor

    NASA Astrophysics Data System (ADS)

    Bowen, K. P.; Stolte, W. C.; Young, J. A.; Demchenko, I. N.; Guillemin, R.; Hemmers, O.; Piancastelli, M. N.; Lindle, D. W.

    2010-03-01

    K-shell photoemission from the carbonyl carbon in the chiral molecule camphor has been studied in the region just above the core-shell ionization threshold. Differences between angular distributions of emitted photoelectrons from the two enantiomers are attributed to the influence of chirality combined with nondipole effects in the photoemission process, despite the fact the measurements were taken using linearly polarized x-rays. The results suggest the possibility of a new form of linear dichroism.

  18. Interlayer-state-driven superconductivity in CaC6 studied by angle-resolved photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Kyung, Wonshik; Kim, Yeongkwan; Han, Garam; Leem, Choonshik; Kim, Chul; Koh, Yoonyoung; Kim, Beomyoung; Kim, Youngwook; Kim, Jun Sung; Kim, Keun Su; Rotenberg, Eli; Denlinger, Jonathan D.; Kim, Changyoung

    2015-12-01

    We performed angle-resolved photoemission experiments on CaC6 and measured kz-dependent electronic structures to investigate the interlayer states. The results reveal a spherical interlayer Fermi surface centered at the Γ point. We also find that the graphene-driven band possesses a weak kz dispersion. The overall electronic structure shows a peculiar single-graphene-layer periodicity in the kz direction although the CaC6 unit cell is supposed to contain three graphene layers. This suggests that the c -axis ordering of Ca has little effect on the electronic structure of CaC6. In addition to CaC6, we also studied the a low-temperature superconductor BaC6. For BaC6, the graphene-band Dirac-point energy is smaller than that of CaC6. Based on data from CaC6 and BaC6, we rule out the Cx y phonon mode as the origin of the superconductivity in CaC6, which strongly suggests interlayer-state-driven superconductivity.

  19. Quanty for core level spectroscopy - excitons, resonances and band excitations in time and frequency domain

    NASA Astrophysics Data System (ADS)

    Haverkort, Maurits W.

    2016-05-01

    Depending on the material and edge under consideration, core level spectra manifest themselves as local excitons with multiplets, edge singularities, resonances, or the local projected density of states. Both extremes, i.e., local excitons and non-interacting delocalized excitations are theoretically well under control. Describing the intermediate regime, where local many body interactions and band-formation are equally important is a challenge. Here we discuss how Quanty, a versatile quantum many body script language, can be used to calculate a variety of different core level spectroscopy types on solids and molecules, both in the frequency as well as the time domain. The flexible nature of Quanty allows one to choose different approximations for different edges and materials. For example, using a newly developed method merging ideas from density renormalization group and quantum chemistry [1-3], Quanty can calculate excitons, resonances and band-excitations in x-ray absorption, photoemission, x-ray emission, fluorescence yield, non-resonant inelastic x-ray scattering, resonant inelastic x-ray scattering and many more spectroscopy types. Quanty can be obtained from: http://www.quanty.org.

  20. Combined Photoemission Spectroscopy and Electrochemical Study of a Mixture of (Oxy)carbides as Potential Innovative Supports and Electrocatalysts.

    PubMed

    Calvillo, Laura; Valero-Vidal, Carlos; Agnoli, Stefano; Sezen, Hikmet; Rüdiger, Celine; Kunze-Liebhäuser, Julia; Granozzi, Gaetano

    2016-08-01

    Active and stable non-noble metal materials, able to substitute Pt as catalyst or to reduce the Pt amount, are vitally important for the extended commercialization of energy conversion technologies, such as fuel cells and electrolyzers. Here, we report a fundamental study of nonstoichiometric tungsten carbide (WxC) and its interaction with titanium oxycarbide (TiOxCy) under electrochemical working conditions. In particular, the electrochemical activity and stability of the WxC/TiOxCy system toward the ethanol electrooxidation reaction (EOR) and hydrogen evolution reaction (HER) are investigated. The chemical changes caused by the applied potential are established by combining photoemission spectroscopy and electrochemistry. WxC is not active toward the ethanol electrooxidation reaction at room temperature but it is highly stable under these conditions thanks to the formation of a passive thin film on the surface, consisting mainly of WO2 and W2O5, which prevents the full oxidation of WxC. In addition, WxC is able to adsorb ethanol, forming ethoxy groups on the surface, which constitutes the first step for the ethanol oxidation. The interaction between WxC and TiOxCy plays an important role in the electrochemical stability of WxC since specific orientations of the substrate are able to stabilize WxC and prevent its corrosion. The beneficial interaction with the substrate and the specific surface chemistry makes tungsten carbide a good electrocatalyst support or cocatalyst for direct ethanol fuel cells. However, WxC is active toward the HER and chemically stable under hydrogen reduction conditions, since no changes in the chemical composition or dissolution of the film are observed. This makes tungsten carbide a good candidate as electrocatalyst support or cocatalyst for the electrochemical production of hydrogen. PMID:27399154

  1. Combined Photoemission Spectroscopy and Electrochemical Study of a Mixture of (Oxy)carbides as Potential Innovative Supports and Electrocatalysts.

    PubMed

    Calvillo, Laura; Valero-Vidal, Carlos; Agnoli, Stefano; Sezen, Hikmet; Rüdiger, Celine; Kunze-Liebhäuser, Julia; Granozzi, Gaetano

    2016-08-01

    Active and stable non-noble metal materials, able to substitute Pt as catalyst or to reduce the Pt amount, are vitally important for the extended commercialization of energy conversion technologies, such as fuel cells and electrolyzers. Here, we report a fundamental study of nonstoichiometric tungsten carbide (WxC) and its interaction with titanium oxycarbide (TiOxCy) under electrochemical working conditions. In particular, the electrochemical activity and stability of the WxC/TiOxCy system toward the ethanol electrooxidation reaction (EOR) and hydrogen evolution reaction (HER) are investigated. The chemical changes caused by the applied potential are established by combining photoemission spectroscopy and electrochemistry. WxC is not active toward the ethanol electrooxidation reaction at room temperature but it is highly stable under these conditions thanks to the formation of a passive thin film on the surface, consisting mainly of WO2 and W2O5, which prevents the full oxidation of WxC. In addition, WxC is able to adsorb ethanol, forming ethoxy groups on the surface, which constitutes the first step for the ethanol oxidation. The interaction between WxC and TiOxCy plays an important role in the electrochemical stability of WxC since specific orientations of the substrate are able to stabilize WxC and prevent its corrosion. The beneficial interaction with the substrate and the specific surface chemistry makes tungsten carbide a good electrocatalyst support or cocatalyst for direct ethanol fuel cells. However, WxC is active toward the HER and chemically stable under hydrogen reduction conditions, since no changes in the chemical composition or dissolution of the film are observed. This makes tungsten carbide a good candidate as electrocatalyst support or cocatalyst for the electrochemical production of hydrogen.

  2. Multiatom Resonant Photoemission: Theory and Systematics

    SciTech Connect

    Garcia de Abajo, F.J.; Fadley, C.S.; Van Hove, M.A.; Garcia de Abajo, F.J.

    1999-05-01

    A first-principles calculation of the recently discovered interatomic multiatom resonant photoemission (MARPE) effect is presented. In this phenomenon, core photoelectron intensities are enhanced when the photon energy is tuned to a core-level absorption edge of nonidentical neighboring atoms, thus enabling direct determination of near-neighbor atomic identities. Both the multiatom character of MARPE and retardation effects in the photon and electron interactions in the resonant channel are shown to be crucial. Measured peak-intensity enhancements of 40{percent} in MnO and spectral shapes similar to the corresponding x-ray absorption profiles are well reproduced by this theory. {copyright} {ital 1999} {ital The American Physical Society}

  3. Magnetic x-ray linear dichroism in resonant and non-resonant Gd 4f photoemission

    SciTech Connect

    Mishra, S.; Gammon, W.J.; Pappas, D.P.

    1997-04-01

    The enhancement of the magnetic linear dichroism in resonant 4f photoemission (MLDRPE) is studied from a 50 monolayer film of Gd/Y(0001). The ALS at beamline 7.0.1 provided the source of linearly polarized x-rays used in this study. The polarized light was incident at an angle of 30 degrees relative to the film plane, and the sample magnetization was perpendicular to the photon polarization. The linear dichroism of the 4f core levels is measured as the photon energy is tuned through the 4d-4f resonance. The authors find that the MLDRPE asymmetry is strongest at the resonance. Near the threshold the asymmetry has several features which are out of phase with the fine structure of the total yield.

  4. Photoemission studies with barium and LaB6 photocathodes and polarized laser light

    NASA Astrophysics Data System (ADS)

    Conde, M. E.; Kwon, S. I.; Young, A. T.; Leung, K. N.; Kim, K.-J.

    1994-11-01

    In this paper, presented is a work on the optimization of the performance of barium photocathodes. Studies on the dependence of the quantum yield on the polarization and angle of incidence of the laser beam are conducted. Moreover, studies on single crystal LaB6 photocathodes are reported. This material possesses a lower quantum yield than barium, but chemically it is much less reactive and have a very good thermionic emission characteristics.

  5. Studies of Dirac and Weyl fermions by angle resolved photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Huang, Lunan

    This dissertation consists of three parts. First, we study magnetic domains in Nd2Fe14 B single crystals using high resolution magnetic force microscopy (MFM). In addition to the elongated, wavy nano-domains reported by a previous MFM study, we found that the micrometer size, star-shaped fractal pattern is constructed of an elongated network of nano-domains about 20 nm in width, with resolution-limited domain walls thinner than 2 nm. Second, we studied extra Dirac cones of multilayer graphene on SiC surface by ARPES and SPA-LEED. We discovered extra Dirac cones on Fermi surface due to SiC 6 x 6 and graphene 6√3 x 6√3 coincidence lattice on both single-layer and three-layer graphene sheets. We interpreted the position and intensity of the Dirac cone replicas, based on the scattering vectors from LEED patterns. We found the positions of replica Dirac cones are determined mostly by the 6 x 6 SiC superlattice even graphene layers grown thicker. Finally, we studied the electronic structure of MoTe2 by ARPES and experimentally confirmed the prediction of type II Weyl state in this material. By combining the result of Density Functional Theory calculations and Berry curvature calculations with out experimental data, we identified Fermi arcs, track states and Weyl points, all features predicted to exist in a type II Weyl semimetal. This material is an excellent playground for studies of exotic Fermions.

  6. X-ray photoemission studies of superficially oxidized cesium antimonide photoemitters

    NASA Technical Reports Server (NTRS)

    Bates, C. W., Jr.; Wertheim, G. K.; Buchanan, D. N. E.; Clements, K. E.; Van Atekum, T. M.

    1981-01-01

    Superficially oxidized cesium antimonide photoemitting surfaces prepared in ultrahigh vacuum were studied by X-ray photoelectron spectroscopy. Oxidation of Cs3Sb to produce a surface with enhanced photosensitivity converts part of the antimony to elemental antimony and part of the cesium to cesium suboxide. The latter is identified on the basis of an O1 s peak at 531.3 eV, characteristic of Cs11O3. The production of Cs2O is not ruled out in this process since its signature at 527.5 eV is masked by an antimony shake-up peak at 527 eV.

  7. Photoemission study of praseodymia in its highest oxidation state: The necessity of in situ plasma treatment

    SciTech Connect

    Schaefer, A.; Zielasek, V.; Baeumer, M.; Gevers, S.; Wollschlaeger, J.; Schroeder, T.; Falta, J.

    2011-02-07

    A cold radio frequency oxygen plasma treatment is demonstrated as a successful route to prepare clean, well-ordered, and stoichiometric PrO{sub 2} layers on silicon. High structural quality of these layers is shown by x-ray diffraction. So far unobserved spectral characteristics in Pr 3d x-ray photoelectron (XP) spectra of PrO{sub 2} are presented as a fingerprint for praseodymia in its highest oxidized state. They provide insight in the electronic ground state and the special role of praseodymia among the rare earth oxides. They also reveal that former XP studies suffered from a significant reduction at the surface.

  8. Resonant photoemission study of multiferroic LuFe{sub 2}O{sub 4} across three-dimensional to two-dimensional charge ordering

    SciTech Connect

    Patankar, S.; Choudhary, R. J.; Phase, D. M.

    2015-04-27

    Electronic structures modification of polycrystalline LuFe{sub 2}O{sub 4} across 3 dimensional to 2 dimensional charge ordering (CO) has been studied by resonance photoemission spectroscopy. Constant-initial-state spectra measured across 3p → 3d resonance energy indicate its charge transfer insulating behavior. Valance band spectra study shows states lying closer to the Fermi level are due to Fe{sup 2+} ions. As the temperature is varied from 3D to 2D CO state, a weight transfer of DOS from low binding energy to higher binding energy is observed which is attributed to the modification in the Fe-O hybridized states.

  9. Metal Interfaces with Cadmium Telluride and Zinc Telluride: a Photoemission Study.

    NASA Astrophysics Data System (ADS)

    Wahi, Anita Kumari

    How a metal overlayer grows and chemically interacts with II-VI semiconductor substrates such as CdTe and ZnTe has practical importance for the electrical characteristics of metal/II-VI contacts. Additionally, studying metal/II -VI interfaces gives insight into the role of weak Hg-bonding in HgCdTe and HgZnTe during metal contact formation, where severe Hg depletion from the HgCdTe surface is typically observed upon metal deposition. This work describes a comparative study of interfacial chemistry and band bending behavior for Al, In, Ag, and Pt overlayers on vacuum-cleaved p-CdTe and p-ZnTe (110) using UPS and XPS. A range of metal-substrate reactivities is considered: Al reacts strongly with Te, Ag moderately, and In minimally, with no evidence seen for In reaction on ZnTe. Pt exhibits strong alloying behavior with both Cd and Zn. Results for the binaries are compared to metal/HgCdTe interface formation. It is found that Hg loss can significantly influence the extent of reaction and/or intermixing for these overlayers relative to the binaries, with stronger reaction seen for Al on the binaries. CdTe and ZnTe band bending behavior is examined, in order to correlate Fermi level movement in the bandgap with interfacial chemistry and morphology. All four metals yield Schottky barriers on CdTe and ZnTe, with a narrow range of final Fermi level positions, E_ {fi} = E_{f} -E_{rm VBM}, observed on CdTe, from 0.9 to 1.05 +/- 0.1 eV, and on ZnTe from 0.65 to 1.0 +/- 0.1 eV. The prediction of the metal-induced gap states (MIGS) model that a difference in barrier height exists for two semiconductors dependent upon their valence band offset is examined and agrees with experiment for Ag, Pt and Al, but not for In. For the highly reactive Al, no evidence for the overlayer metallicity required for MIGS to operate is seen until after band bending has stabilized. Reaction and intermixing for Al, Ag, and Pt overlayers on CdTe and ZnTe indicate these interfaces are not ideal. The

  10. Surface study of metal-containing ionic liquids by means of photoemission and absorption spectroscopies

    NASA Astrophysics Data System (ADS)

    Caporali, Stefano; Pedio, Maddalena; Chiappe, Cinzia; Pomelli, Christian S.; Acres, Robert G.; Bardi, Ugo

    2016-06-01

    The vacuum/liquid interface of different ionic liquids obtained by dissolving bistriflimide salts of Ag, Al, Cu, Ni, and Zn in 1-butyl-3-methylimidazolium bistriflimide ([bmim][Tf2N]) was investigated under vacuum using AR-XPS and NEXAFS. The XPS spectra show chemical shifts of the nitrogen of the bistriflimide anion as a function of the metal type, indicating different strength of the coordination bonds. In silver bearing ILs, silver ions were found to be only weakly coordinated. On the contrary, Ni, Cu, Zn, and especially Al exhibit large chemical shifts attributable to strong interaction with the bistriflimide ions. The outermost surface was enriched with or depleted of metal ions as a function of the nature of the metals. Nickel and zinc tend to slightly concentrate at the surface while copper, silver, and especially aluminum are depleted at the surface. We also observed that the aliphatic alkyl chains of the cations tend to protrude outside the surface in all systems studied. However, the presence of metals generally increases the amount of bistriflimide at the vacuum/liquid interface.

  11. Ultraviolet photoemission study of oligothiophenes: π-band evolution and geometries

    NASA Astrophysics Data System (ADS)

    Fujimoto, H.; Nagashima, U.; Inokuchi, H.; Seki, K.; Cao, Y.; Nakahara, H.; Nakayama, J.; Hoshino, M.; Fukuda, K.

    1990-04-01

    Ultraviolet photoelectron spectroscopy (UPS) has been applied to the investigation of the electronic structure of oligothiophenes with 4-8 thiophene rings. In a series of α-linked oligomers (αn with n being the number of rings), a systematic evolution of the π band is observed. Several peaks which correspond to the π band are observed in the region of 0.7-3 eV below the Fermi level (EF), and the bandwidth becomes broader with increasing n. The nonbonding π band is observed at 3.5 eV below EF and its energy is almost independent of the number of thiophene units. UPS spectra of α7 and α8 are fairly similar to the spectra of polythiophene, showing that these oligomers are good model compounds of the polymer. The ionization threshold energy of α7 and polythiophene was observed to be 5.3 eV. The effect of irregularity on the π-electron system was also studied by using oligomers which contain a β linkage or a vinylene group at the middle of the molecule. The UPS spectra showed that the β linkages significantly affect the electronic structure of polythiophene, while the vinylene group does not. In order to analyze the UPS spectra and to investigate the electronic structures of oligomers, the orbital energies and the geometries of these oligomers are calculated by the semiempirical MNDO-SCF-MO (modified neglect of diatomic overlap self-consistent-field molecular orbital) method. Theoretically simulated spectra of these oligothiophenes derived from the obtained orbital energies by Gaussian broadening are compared with the observed ones. The agreement between the observed and calculated spectra is very good, particularly in the π region. It is shown from the optimized geometry that (1) αn 's have planar structure and π electrons are delocalized, (2) the oligomer with β linkages has nonplanar structure leading to limited delocalization of π electrons, and (3) the oligomers with a vinylene group are almost planar and the disturbance by the vinylene group on the

  12. A photoemission study of the coadsorption of CO 2 and Na on TiO 2(110)-(1 × 1) and -(1 × 2) surfaces: adsorption geometry and reactivity

    NASA Astrophysics Data System (ADS)

    Nerlov, Jesper; Christensen, Søren V.; Weichel, Steen; Pedersen, Eddie H.; Møller, Preben J.

    1997-02-01

    The coadsorption of CO 2 and Na on TiO 2(110)-(1 × 1) and -(1 × 2) surfaces have been investigated by synchrotron-radiation based core-level and valence band photoemission. We find that the initially adsorbed Na exhibits a core-level shift of 1.15 eV when the two surfaces are compared. From a simple adsorption model this binding energy shift is understood in terms of a difference in initial Na adsorption site on these surfaces. While the (1 × 1) surface seems to favor Na adsorption in a hollow site "between" bridging surface oxygen atoms, it is found that the (1 × 2) surface facilitates a chemically more advantageous Na adsorption "adjacent to" the bridging oxygen atoms. Valence band measurements support this model since Na adsorption on the (1 × 2) surface leads to emission characteristic of alkali-oxygen-like compounds while this is not the case for the {Na}/{TiO2(110) }-(1 × 1) system. Finally, the relatively high resolution of the core-level emission allows in a direct way the various features contributing to the Na 2p core-level emission to be determined. With respect to adsorption of CO 2 we find for the (1 × 2) surface that CO 2 uptake saturates around 0.5 ML Na coverage compared to 1 ML for the (1 × 1) surface, indicating that the Na coverage required for saturation of CO 2 uptake is proportional to the density of protruded oxygen rows present at the surface. The CO 2 uptake, however, increases as the density of the oxygen rows decreases. Valence band photoemission data obtained from both interfaces show that a surface carbonate species is formed. At lower coverages/exposures there are, however, indications of the presence of a CO -2 species rather than carbonate, thereby suggesting that the carbonate species is formed through the surface reaction: 2CO -2→CO 2-3 + CO.

  13. Synchronization and Characterization of an Ultra-Short Laser for Photoemission and Electron-Beam Diagnostics Studies at a Radio Frequency Photoinjector

    SciTech Connect

    Maxwell, Timothy; Ruan, Jinhao; Piot, Philippe; Lumpkin, Alex

    2012-03-01

    A commercially-available titanium-sapphire laser system has recently been installed at the Fermilab A0 photoinjector laboratory in support of photoemission and electron beam diagnostics studies. The laser system is synchronized to both the 1.3-GHz master oscillator and a 1-Hz signal use to trigger the radiofrequency system and instrumentation acquisition. The synchronization scheme and performance are detailed. Long-term temporal and intensity drifts are identified and actively suppressed to within 1 ps and 1.5%, respectively. Measurement and optimization of the laser's temporal profile are accomplished using frequency-resolved optical gating.

  14. Direct surface magnetometry with photoemission magnetic x-ray dichroism

    SciTech Connect

    Tobin, J.G.; Goodman, K.W.; Schumann, F.O.

    1997-04-01

    Element specific surface magnetometry remains a central goal of synchrotron radiation based studies of nanomagnetic structures. One appealing possibility is the combination of x-ray absorption dichroism measurements and the theoretical framework provided by the {open_quotes}sum rules.{close_quotes} Unfortunately, sum rule analysis are hampered by several limitations including delocalization of the final state, multi-electronic phenomena and the presence of surface dipoles. An alternative experiment, Magnetic X-Ray Dichroism in Photoelectron Spectroscopy, holds out promise based upon its elemental specificity, surface sensitivity and high resolution. Computational simulations by Tamura et al. demonstrated the relationship between exchange and spin orbit splittings and experimental data of linear and circular dichroisms. Now the authors have developed an analytical framework which allows for the direct extraction of core level exchange splittings from circular and linear dichroic photoemission data. By extending a model initially proposed by Venus, it is possible to show a linear relation between normalized dichroism peaks in the experimental data and the underlying exchange splitting. Since it is reasonable to expect that exchange splittings and magnetic moments track together, this measurement thus becomes a powerful new tool for direct surface magnetometry, without recourse to time consuming and difficult spectral simulations. The theoretical derivation will be supported by high resolution linear and circular dichroism data collected at the Spectromicroscopy Facility of the Advanced Light Source.

  15. Photoemission, Correlation and Superconductivity:

    NASA Astrophysics Data System (ADS)

    Abrecht, M.; Ariosa, D.; Cloëtta, D.; Pavuna, D.; Perfetti, L.; Grioni, M.; Margaritondo, G.

    We review some of the problems still affecting photoemission as a probe of high-temperature superconductivity, as well as important recent results concerning their solution. We show, in particular, some of the first important results on thin epitaxial films grown by laser ablation, which break the monopoly of cleaved BCSCO in this type of experiments. Such results, obtained on thin LSCO, may have general implications on the theory of high-temperature superconductivity.

  16. Relationships Between Complex Core Level Spectra and Materials Properties

    SciTech Connect

    Nelin, Constance J.; Bagus, Paul S.; Ilton, Eugene S.; Chambers, Scott A.; Kuhlenbeck, Helmut; Freund, Hans-Joachim

    2010-12-01

    The XPS of many oxides are quite complex and there may be several peaks of significant intensity for each subshell. These peaks arise from many-electron effects, which normally are treated with configuration interaction (CI) wavefunctions where static correlation effects are taken into account. It is common to use semiempirical methods to determine the matrix elements of the CI Hamiltonian and there are few rigorous CI calculations where parameters are not adjusted to fit experiment. In contrast, we present, in the present work, theoretical XPS spectra obtained with rigorous CI wavefunctions for CeO2 where the XPS are especially complex; several different core levels are studied. This study uses an embedded CeO8 cluster model to represent bulk CeO2 and the relativistic CI wavefunctions are determined using four-component spinors from Dirac-Fock calculations. In particular, we examine the importance of interatomic many-body effects where there is a transfer of electrons from occupied oxygen 2p orbitals into empty cation orbitals as it is common to ascribe the complex XPS to this effect. We also contrast the importance of many-body charge-transfer effects for the isoelectronic cations of Ce4+ and La3+. The long-range goal of this work is to relate the XPS features to the nature of the chemical bonding in CeO2 and we describe our progress toward this goal.

  17. A Dust Grain Photoemission Experiment

    NASA Technical Reports Server (NTRS)

    Venturini, C. C.; Spann, J. F., Jr.; Abbas, M. M.; Comfort, R. H.

    2000-01-01

    A laboratory experiment has been developed at Marshall Space Flight Center to study the interaction of micron-sized particles with plasmas and FUV radiation. The intent is to investigate the conditions under which particles of various compositions and sizes become charged, or discharged, while exposed to an electron beam and/or UV radiation. This experiment uses a unique laboratory where a single charged micron size particle is suspended in a quadrupole trap and then subjected to a controlled environment. Tests are performed using different materials and sizes, ranging from 10 microns to 1 micron, to determine the particle's charge while being subjected to an electron beam and /or UV radiation. The focus of this presentation will be on preliminary results from UV photoemission tests, but past results from electron beam, secondary electron emission tests will also be highlighted. A monochromator is used to spectrally resolve UV in the 120 nm to 300 nm range. This enables photoemission measurements as a function of wavelength. Electron beam tests are conducted using I to 3 micron sized aluminum oxide particles subjected to energies between 100 eV to 3 KeV. It was found that for both positive and negative particles the potential tended toward neutrality over time with possible equilibrium potentials between -0.8 Volts and 0.8 Volts.

  18. CH 3Cl adsorption on a Si(100)2 × 1 surface modified by alkali metal overlayer studied by soft X-ray photoemission using synchrotron radiation

    NASA Astrophysics Data System (ADS)

    Gentle, T. M.; Soukiassian, P.; Schuette, K. P.; Bakshi, M. H.; Hurych, Z.

    1988-08-01

    We present the first study of the effect of an alkali metal overlayer on the adsorption of an organic molecule, methylchloride, on a Si(100)2 × 1 surface. In strong contrast to the behavior of molecular oxygen or nitrogen which were found to react with the silicon substrate, there was no significant interaction between methylchloride and silicon, rather, the formation of alkali-chlorine bonds was observed. Core level and valence band spectroscopies using synchrotron radiation were used to study these systems. Sodium was found to exhibit the strongest interaction with mehtylchloride which was dissociated, while the effects produced by K and Cs were weaker.

  19. Development of a high-resolution soft x-ray (30--1500 eV) beamline at the Advanced Light Source and its use for the study of angle-resolved photoemission extended fine structure

    SciTech Connect

    Huff, W R.A.

    1996-02-01

    ALS Bending magnet beamline 9.3.2 is for high resolution spectroscopy, with circularly polarized light. Fixed included-angle SGM uses three gratings for 30--1500 eV photons; circular polarization is produced by an aperture for selecting the beam above or below the horizontal plane. Photocurrent from upper and lower jaws of entrance slit sets a piezoelectric drive feedback loop on the vertically deflecting mirror for stable beam. End station has a movable platform. With photomeission data from Stanford, structure of c(2{times}2)P/Fe(100) was determined using angle-resolved photoemission extended fine structure (ARPEFS). Multiple-scattering spherical-wave (MSSW) calculations indicate that P atoms adsorb in fourfold hollow sites 1.02A above the first Fe layer. Self-consistent-field X{alpha} scattered wave calculation confirm that the Fe{sub 1}-Fe{sub 2} space is contracted for S/Fe but not for P/Fe; comparison is made to atomic N and O on Fe(100). Final-state effects on ARPEFS curves used literature data from the S 1s and 2p core levels of c(2{times}2)S/Ni(001); a generalized Ramsauer-Townsend splitting is present in the 1s but not 2p data. An approximate method for analyzing ARPEFS data from a non-s initial state using only the higher-{ell} partial wave was tested successfully. ARPEFS data from clean surfaces were collected normal to Ni(111) (3p core levels) and 5{degree} off-normal from Cu(111)(3s, 3p). Fourier transforms (FT) resemble adsorbate systems, showing backscattering signals from atoms up to 4 layers below emitters. 3p FTs show scattering from 6 nearest neighbors in the same crystal layer as the emitters. MSSW calulation indicate that Cu 3p photoemission is mostly d-wave. FTs also indicate double-scattering and single-scattering from laterally distant atoms; calculations indicate that the signal is dominated by photoemission from the first 2 crystal layers.

  20. Chiral asymmetry in the angle-resolved O and C 1s-1 core photoemissions of the R enantiomer of glycidol

    NASA Astrophysics Data System (ADS)

    Powis, Ivan; Harding, Chris J.; Barth, Silko; Joshi, Sanjeev; Ulrich, Volker; Hergenhahn, Uwe

    2008-11-01

    We present measurements of a photoelectron circular dichroism in photoionization from O and C 1s core levels, of the R enantiomer of glycidol (C3H6O2) in the gas phase. This dichroism emerges from a forward-backward asymmetry in the angular distribution of electrons created on ionization with circularly polarized synchrotron radiation and is already fully present in the pure electric dipole approximation. Asymmetry factors obtained for the core levels in this study range up to a few percent, but it is likely that these values are limited by a failure to resolve photoemission from individual atomic sites. Theoretical modeling is provided to examine possible differences between these alternative atomic photoemission sites, and between different conformational structures of glycidol. The calculated chiral angular distribution parameters that support the circular dichroism display a much enhanced sensitivity to the molecular conformation compared to the conventional photoionization cross section and the β parameter. Likely conformer structures can be suggested after comparison with the experiment.

  1. Mott behavior of ultrathin epitaxial LaNiO3 films and interfaces via hard x-ray and standing-wave excited photoemission

    NASA Astrophysics Data System (ADS)

    Gray, Alexander; Kaiser, Alexander; Son, Junwoo; Janotti, Anderson; Yang, See-Hun; Bostwick, Aaron; Ueda, Shigenori; Kobayashi, Keisuke; van de Walle, Chris; Stemmer, Susanne; Fadley, Charles

    2012-02-01

    In this study we apply several emerging x-ray photoemission techniques to study Mott behavior of ultrathin LaNiO3 films and interfaces in a depth-resolved manner. In order to understand the effects of thickness and strain on the electronic structure, we apply hard x-ray photoemission (HAXPES) at 6 keV to epitaxial LaNiO3 films of varying thickness under compressive and tensile strain. Mott metal-to-insulator transition is observed for the thinnest films. Furthermore, standing-wave-excited photoemission is used to study the electronic structure of ultrathin LaNiO3 in a SrTiO3/LaNiO3 superlattice. Standing-wave measurements of core-level and valence band spectra are used to derive layer-resolved densities of states, revealing a suppression of electronic states near the Fermi level in the multilayer as compared to bulk LaNiO3. Further analysis shows that the suppression of these states is not homogeneously distributed over the LaNiO3 layers but is more pronounced near the interfaces.

  2. First-principle calculation of core level binding energies of Li{sub x}PO{sub y}N{sub z} solid electrolyte

    SciTech Connect

    Guille, Émilie; Vallverdu, Germain Baraille, Isabelle

    2014-12-28

    We present first-principle calculations of core-level binding energies for the study of insulating, bulk phase, compounds, based on the Slater-Janak transition state model. Those calculations were performed in order to find a reliable model of the amorphous Li{sub x}PO{sub y}N{sub z} solid electrolyte which is able to reproduce its electronic properties gathered from X-ray photoemission spectroscopy (XPS) experiments. As a starting point, Li{sub 2}PO{sub 2}N models were investigated. These models, proposed by Du et al. on the basis of thermodynamics and vibrational properties, were the first structural models of Li{sub x}PO{sub y}N{sub z}. Thanks to chemical and structural modifications applied to Li{sub 2}PO{sub 2}N structures, which allow to demonstrate the relevance of our computational approach, we raise an issue concerning the possibility of encountering a non-bridging kind of nitrogen atoms (=N{sup −}) in Li{sub x}PO{sub y}N{sub z} compounds.

  3. Physics of the Be(0001) surface core-level spectrum

    SciTech Connect

    Feibelman, P.J.; Stumpf, R. )

    1994-12-15

    First-principles calculations for slabs as many as 13 layers thick show that the three surface core-level features observed on Be(0001) correspond to core-electron ionizations in its three outermost atomic layers. The calculations also imply that the experimental peak identified with core ionization in the bulk is a composite; theoretical core-ionization potentials for the fourth and deeper layers differ by as much as 90 meV. The sign and surprisingly large magnitudes of the Be(0001) surface core-level shifts (SCLS's) are attributed to unusually large surface-state contributions to the three outer layers' local densities of states. Both initial- and final-state effects are substantial in the SCLS's, and their contributions are additive.

  4. Atom-to-atom interactions for atomic layer deposition of trimethylaluminum on Ga-rich GaAs(001)-4 × 6 and As-rich GaAs(001)-2 × 4 surfaces: a synchrotron radiation photoemission study

    PubMed Central

    2013-01-01

    High-resolution synchrotron radiation photoemission was employed to study the effects of atomic-layer-deposited trimethylaluminum (TMA) and water on Ga-rich GaAs(001)-4 × 6 and As-rich GaAs(001)-2 × 4 surfaces. No high charge states were found in either As 3d or Ga 3d core-level spectra before and after the deposition of the precursors. TMA adsorption does not disrupt the GaAs surface structure. For the (4 × 6) surface, the TMA precursor existed in both chemisorbed and physisorbed forms. In the former, TMA has lost a methyl group and is bonded to the As of the As-Ga dimer. Upon water purge, the dimethylaluminum-As group was etched off, allowing the now exposed Ga to bond with oxygen. Water also changed the physisorbed TMA into the As-O-Al(CH3)2 configuration. This configuration was also found in 1 cycle of TMA and water exposure of the (2 × 4) surface, but with a greater strength, accounting for the high interface defect density in the mid-gap region. PMID:23587341

  5. Adsorption of dopamine on rutile TiO2 (110): a photoemission and near-edge X-ray absorption fine structure study.

    PubMed

    Jackman, Mark J; Syres, Karen L; Cant, David J H; Hardman, Samantha J O; Thomas, Andrew G

    2014-07-29

    Synchrotron radiation photoelectron spectroscopy and near-edge X-ray absorption fine structure (NEXAFS) techniques have been used to study the adsorption of dopamine on a rutile TiO2 (110) single crystal. Photoemission results suggest that dopamine bonds through the oxygen molecules in a bidentate fashion. From the data, it is ambiguous whether the oxygens bond to the same 5-fold coordinated surface titanium atom or bridges across two, although based on the bonding of pyrocatechol on rutile TiO2 (110), it is likely that the dopamine bridges two titanium atoms. Using the searchlight effect, the carbon K-edge near-edge X-ray absorption fine structure NEXAFS spectra recorded for dopamine on rutile TiO2 (110) show the phenyl ring to be oriented at 78° ± 5° from the surface and twisted 11 ± 10° relative to the (001) direction.

  6. Adsorption of dopamine on rutile TiO2 (110): a photoemission and near-edge X-ray absorption fine structure study.

    PubMed

    Jackman, Mark J; Syres, Karen L; Cant, David J H; Hardman, Samantha J O; Thomas, Andrew G

    2014-07-29

    Synchrotron radiation photoelectron spectroscopy and near-edge X-ray absorption fine structure (NEXAFS) techniques have been used to study the adsorption of dopamine on a rutile TiO2 (110) single crystal. Photoemission results suggest that dopamine bonds through the oxygen molecules in a bidentate fashion. From the data, it is ambiguous whether the oxygens bond to the same 5-fold coordinated surface titanium atom or bridges across two, although based on the bonding of pyrocatechol on rutile TiO2 (110), it is likely that the dopamine bridges two titanium atoms. Using the searchlight effect, the carbon K-edge near-edge X-ray absorption fine structure NEXAFS spectra recorded for dopamine on rutile TiO2 (110) show the phenyl ring to be oriented at 78° ± 5° from the surface and twisted 11 ± 10° relative to the (001) direction. PMID:25003716

  7. Image potential states in monolayer, bilayer, and trilayer epitaxial graphene studied with time- and angle-resolved two-photon photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Takahashi, Kazutoshi; Imamura, Masaki; Yamamoto, Isamu; Azuma, Junpei; Kamada, Masao

    2014-04-01

    Image potential states (IPSs) on monolayer, bilayer, and trilayer graphene epitaxially grown on SiC(0001) have been studied by time- and angle-resolved two-photon photoemission (2PPE) spectroscopy. The free-electron-like dispersions of even and odd symmetry IPSs with a quantum number of n = 1+, 1-, 2, 3 were observed. All observed IPSs showed the dispersions with effective masses of m*=1.0±0.1me. The 2PPE intensity of the lowest IPS (n = 1+) was attenuated with an increasing number of graphene layers. The time-resolved 2PPE measurements revealed that these IPSs have significantly shorter lifetimes, suggesting a coupling of IPSs with electronic states in the buffer layer and the SiC substrate.

  8. Fermi Surface Evolution and Luttinger Theorem in NaxCoO2: A Systematic Photoemission Study

    SciTech Connect

    Yang, H. B.; Pan, Z. H.; Sekharan, A. K. P.; Sato, T.; Souma, S.; Takahashi, T.; Jin, Rongying; Sales, Brian C; Mandrus, David; Fedorov, A. V.; Wang, Z.; Ding, H.

    2005-01-01

    We report a systematic angle-resolved photoemission study on Na{sub x}CoO{sub 2} for a wide range of Na concentrations (0.3 {le} x {le} 0.72). In all the metallic samples at different x, we observed (i) only a single holelike Fermi surface centered around {Gamma} and (ii) its area changes with x according to the Luttinger theorem. We also observed a surface state that exhibits a larger Fermi surface area. The e{prime}{sub g} band and the associated small Fermi surface pockets near the K points predicted by band calculations are found to sink below the Fermi energy in a manner almost independent of the doping and temperature.

  9. X-ray photoemission study of the Te-precursor surfaces and the initial stages of growth of ZnTe on GaAs (100)

    NASA Astrophysics Data System (ADS)

    Tatarenko, S.; Saminadayar, K.; Cibert, J.

    1987-11-01

    The initial stages of epitaxial growth of ZnTe on GaAs (100) have been studied by x-ray photoemission spectroscopy. The two surface structures (6×1 and (3)1/2×3 ) resulting from the adsorption of Te on GaAs (100) were used as precursor for ZnTe growth. Each of these structures is characterized by two different adsorbed Te states. For the 6×1 structure, the two states are assigned to As-Te-As and tentatively to Te-Te-Te bonds; and for the (3)1/2×3 structure, the assigned bonds are As-Te-As and GaGa Te-As. Growth of ZnTe (100) does not induce any change in the bonds associated with the 6×1 structure but modifies that associated with the (3)1/2×3 surface.

  10. Anomalous temperature dependence in valence band spectra: A resonant photoemission study of layered perovskite Sr{sub 2}CoO{sub 4}

    SciTech Connect

    Pandey, Pankaj K.; Choudhary, R. J. Phase, D. M.

    2014-05-05

    Valence band spectra (VBS) and its modification across Curie temperature (T{sub C}) of Sr{sub 2}CoO{sub 4} thin film are studied using resonant photoemission spectroscopy. It is found that VBS mainly consists of hybridized states of Co-3d t{sub 2g}e{sub g} and O-2p; however, Co-3d e{sub g} states show its prominence only in the ferromagnetic temperature regime. Below T{sub C}, spectral weight transfer takes place anomalously from high binding energy (B.E.) region to low B.E. region, signifying the enhanced intermediate or low spin state Co{sup 4+} ions. It is suggested that spin-lattice coupling and many-body effects in Sr{sub 2}CoO{sub 4} derived from the strong electron correlations lead to such temperature dependence of VBS.

  11. in situ studied correlated oxide LaNiO3 ultra thin film by angle resolved photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Yoo, H. K.; Chang, Y. J.; Kim, K. S.; Moreschini, L.; Jeong, D. W.; Kim, Y. S.; Bostwick, A.; Rotenberg, E.; Noh, T. W.

    2012-02-01

    Recently, RNiO3 (R: rare earth) attracted increasing attention due to the possible realization of the electronic band structure similar to the high-temperature superconductor cuprates. Among them, LaNiO3 based heterostructures have shown various fascinating physical properties such as dimensionality controlled electronic phase transitions. Theoretical works on confined LaNiO3 through heterostructuring predicted cuprate-like band structure and magnetic properties. Here, we reports in-situ angle resolved photoemission spectroscopy results on the LaNiO3 films grown by pulsed laser deposition method. We carefully controlled the thickness of LaNiO3 films from one to 30 unit cells and measured the thickness dependent band dispersions. First, we will discuss the strong electronic correlation effect in bulk-like band structure of thick LaNiO3 films comparing to the previously reported LDA+DMFT calculation. Moreover, we will discuss the thickness dependent band structure. As decreasing the film thickness, we observed the charge redistribution of two Ni eg orbitals at the Fermi surface. The origins of thickness dependent electronic structure will be discussed.

  12. Conduction-band electronic states of YbInCu{sub 4} studied by photoemission and soft x-ray absorption spectroscopies

    SciTech Connect

    Utsumi, Yuki; Kurihara, Hidenao; Maso, Hiroyuki; Tobimatsu, Komei; Sato, Hitoshi; Shimada, Kenya; Namatame, Hirofumi; Hiraoka, Koichi; Kojima, Kenichi; Ohkochi, Takuo; Fujimori, Shin-ichi; Takeda, Yukiharu; Saitoh, Yuji; Mimura, Kojiro; Ueda, Shigenori; Yamashita, Yoshiyuki; Yoshikawa, Hideki; Kobayashi, Keisuke; Oguchi, Tamio; Taniguchi, Masaki

    2011-09-15

    We have studied conduction-band (CB) electronic states of a typical valence-transition compound YbInCu{sub 4} by means of temperature-dependent hard x-ray photoemission spectroscopy (HX-PES) of the Cu 2p{sub 3/2} and In 3d{sub 5/2} core states taken at h{nu}=5.95 keV, soft x-ray absorption spectroscopy (XAS) of the Cu 2p{sub 3/2} core absorption region around h{nu}{approx}935 eV, and soft x-ray photoemission spectroscopy (SX-PES) of the valence band at the Cu 2p{sub 3/2} absorption edge of h{nu}=933.0 eV. With decreasing temperature below the valence transition at T{sub V}=42 K, we have found that (1) the Cu 2p{sub 3/2} and In 3d{sub 5/2} peaks in the HX-PES spectra exhibit the energy shift toward the lower binding-energy side by {approx}40 and {approx}30 meV, respectively, (2) an energy position of the Cu 2p{sub 3/2} main absorption peak in the XAS spectrum is shifted toward higher photon-energy side by {approx}100 meV, with an appearance of a shoulder structure below the Cu 2p{sub 3/2} main absorption peak, and (3) an intensity of the Cu L{sub 3}VV Auger spectrum is abruptly enhanced. These experimental results suggest that the Fermi level of the CB-derived density of states is shifted toward the lower binding-energy side. We have described the valence transition in YbInCu{sub 4} in terms of the charge transfer from the CB to Yb 4f states.

  13. In-Situ observation of wet oxidation kinetics on Si (100) via ambient pressure x-ray photoemission spectroscopy

    SciTech Connect

    Hussain, Zahid; Rossi, Massimiliano; Mun, Bongjin S.; Enta, Yoshiharu; Fadley, Charles S.; Lee, Ki-Suk; Kim, Sang-Koog; Shin, Hyun-Joon; Hussain, Zahid; Ross, Jr., Philip N.

    2007-08-24

    The initial stages of wet thermal oxidation of Si(100)-(2x1) have been investigated by in-situ ambient pressure x-ray photoemission spectroscopy (APXPS), including chemical-state resolution via Si 2p core-level spectra. Real-time growth rates of silicon dioxide have been monitored at 100 mTorr of water vapor. This pressure is considerably higher than in any prior study using XPS. Substrate temperatures have been varied between 250 and 500 C. Above a temperature of {approx} 400 C, two distinct regimes, a rapid and a quasi-saturated one, are identified and growth rates show a strong temperature dependence which cannot be explained by the conventional Deal-Grove model.

  14. Identification and thermal stability of the native oxides on InGaAs using synchrotron radiation based photoemission

    NASA Astrophysics Data System (ADS)

    Brennan, B.; Hughes, G.

    2010-09-01

    A high resolution synchrotron radiation core level photoemission study of the native oxides on In0.53Ga0.47As was carried out in order to determine the various oxidation states present on the surface. The thermal stability of the oxidation states was also investigated by annealing the samples in vacuum at temperatures ranging from 150 to 450 °C. As well as the widely reported oxidation states, various arsenic, gallium, and indium oxides, along with mixed phase gallium arsenic and indium gallium oxides are identified. Elemental binary oxides have been identified as residing at the oxide substrate interface and could play an important role in understanding the growth of metal oxide dielectric layers on the InGaAs surface, due to their apparent chemical stability.

  15. Vacuum space charge effects in sub-picosecond soft X-ray photoemission on a molecular adsorbate layer.

    PubMed

    Dell'Angela, M; Anniyev, T; Beye, M; Coffee, R; Föhlisch, A; Gladh, J; Kaya, S; Katayama, T; Krupin, O; Nilsson, A; Nordlund, D; Schlotter, W F; Sellberg, J A; Sorgenfrei, F; Turner, J J; Öström, H; Ogasawara, H; Wolf, M; Wurth, W

    2015-03-01

    Vacuum space charge induced kinetic energy shifts of O 1s and Ru 3d core levels in femtosecond soft X-ray photoemission spectra (PES) have been studied at a free electron laser (FEL) for an oxygen layer on Ru(0001). We fully reproduced the measurements by simulating the in-vacuum expansion of the photoelectrons and demonstrate the space charge contribution of the high-order harmonics in the FEL beam. Employing the same analysis for 400 nm pump-X-ray probe PES, we can disentangle the delay dependent Ru 3d energy shifts into effects induced by space charge and by lattice heating from the femtosecond pump pulse.

  16. Vacuum space charge effects in sub-picosecond soft X-ray photoemission on a molecular adsorbate layer.

    PubMed

    Dell'Angela, M; Anniyev, T; Beye, M; Coffee, R; Föhlisch, A; Gladh, J; Kaya, S; Katayama, T; Krupin, O; Nilsson, A; Nordlund, D; Schlotter, W F; Sellberg, J A; Sorgenfrei, F; Turner, J J; Öström, H; Ogasawara, H; Wolf, M; Wurth, W

    2015-03-01

    Vacuum space charge induced kinetic energy shifts of O 1s and Ru 3d core levels in femtosecond soft X-ray photoemission spectra (PES) have been studied at a free electron laser (FEL) for an oxygen layer on Ru(0001). We fully reproduced the measurements by simulating the in-vacuum expansion of the photoelectrons and demonstrate the space charge contribution of the high-order harmonics in the FEL beam. Employing the same analysis for 400 nm pump-X-ray probe PES, we can disentangle the delay dependent Ru 3d energy shifts into effects induced by space charge and by lattice heating from the femtosecond pump pulse. PMID:26798795

  17. Plasmon Enhanced Photoemission

    SciTech Connect

    Polyakov, Aleksandr

    2012-05-08

    Next generation ultrabright light sources will operate at megahertz repetition rates with temporal resolution in the attosecond regime. For an X-Ray Free Electron Laser (FEL) to operate at such repetition rate requires a high quantum efficiency (QE) cathode to produce electron bunches of 300 pC per 1.5 μJ incident laser pulse. Semiconductor photocathodes have sufficient QE in the ultraviolet (UV) and the visible spectrum, however, they produce picosecond electron pulses due to the electron-phonon scattering. On the other hand, metals have two orders of magnitude less QE, but can produce femtosecond pulses, that are required to form the optimum electron distribution for high efficiency FEL operation. In this work, a novel metallic photocathode design is presented, where a set of nano-cavities is introduced on the metal surface to increase its QE to meet the FEL requirements, while maintaining the fast time response. Photoemission can be broken up into three steps: (1) photon absorption, (2) electron transport to the surface, and (3) crossing the metal-vacuum barrier. The first two steps can be improved by making the metal completely absorbing and by localizing the fields closer to the metal surface, thereby reducing the electron travel distance. Both of these effects can be achieved by coupling the incident light to an electron density wave on the metal surface, represented by a quasi-particle, the Surface Plasmon Polariton (SPP). The photoemission then becomes a process where the photon energy is transferred to an SPP and then to an electron. The dispersion relation for the SPP defines the region of energies where such process can occur. For example, for gold, the maximum SPP energy is 2.4 eV, however, the work function is 5.6 eV, therefore, only a fourth order photoemission process is possible. In such process, four photons excite four plasmons that together excite only one electron. The yield of such non-linear process depends strongly on the light intensity. In

  18. Study of photoemission and work function of large surface areas, phase 3, phase 4. [wavelength dependences of photoelectric space probe materials

    NASA Technical Reports Server (NTRS)

    1973-01-01

    The photoemission of materials which might be used in probe measurements of the exo-atmospheric electric field is considered by evaluating the wavelength dependence of their photoelectric yield for eleven elements over the range 800 to 3200 A. Yield data for zinc, copper beryllium, platinum, cadmium, graphite, carbon, gold, silver, tantalum, and tungsten show that copper-beryllium is a preferred material. Silver has one of the highest photoemissions when exposed to solar radiation.

  19. A medium-energy photoemission and ab-initio investigation of cubic yttria-stabilised zirconia

    SciTech Connect

    Cousland, G. P.; Cui, X. Y.; Smith, A. E.; Stampfl, C. M.; Wong, L.; Tayebjee, M.; Yu, D.; Triani, G.; Evans, P. J.; Ruppender, H.-J.; Jang, L.-Y.; Stampfl, A. P. J.

    2014-04-14

    Experimental and theoretical investigations into the electronic properties and structure of cubic yttria-stabilized zirconia are presented. Medium-energy x-ray photoemission spectroscopy measurements have been carried out for material with a concentration of 8-9 mol. % yttria. Resonant photoemission spectra are obtained for a range of photon energies that traverse the L2 absorption edge for both zirconium and yttrium. Through correlation with results from density-functional theory (DFT) calculations, based on structural models proposed in the literature, we assign photoemission peaks appearing in the spectra to core lines and Auger transitions. An analysis of the core level features enables the identification of shifts in the core level energies due to different local chemical environments of the constituent atoms. In general, each core line feature can be decomposed into three contributions, with associated energy shifts. Their identification with results of DFT calculations carried out for proposed atomic structures, lends support to these structural models. The experimental results indicate a multi-atom resonant photoemission effect between nearest-neighbour oxygen and yttrium atoms. Near-edge x-ray absorption fine structure spectra for zirconium and yttrium are also presented, which correlate well with calculated Zr- and Y-4d electron partial density-of-states and with Auger electron peak area versus photon energy curve.

  20. Angle-dependent study of a direct optical transition in the sp bands of Ag(111) by one- and two-photon photoemission

    NASA Astrophysics Data System (ADS)

    Winkelmann, Aimo; Sametoglu, Vahit; Zhao, Jin; Kubo, Atsushi; Petek, Hrvoje

    2007-11-01

    We have measured angle-dependent photoemission spectra for one-photon and two-photon excitation from Ag(111). The observed dispersion of the sp -band transition of Ag(111) can be reproduced using a nearly-free-electron model for the initial and final states involved. The observed dispersion agrees with the known band structure. We illustrate how the strong refraction of low-energy electrons becomes a limiting factor to obtain quantitative band-structure information. Conversely, low-energy electrons of a well-defined direct optical interband transition can provide a sensitive probe of the inner potential. We observe asymmetric two-photon photoelectron intensity distributions with respect to detection along the surface normal. These intensity distributions can be well described by a phenomenological model which employs the Fresnel equations to calculate the electric field components of the incident radiation inside the sample. Very good agreement is found using tabulated optical constants and a momentum matrix element, which is oriented along the surface normal. In contrast, the observed intensity distribution for one-photon photoemission from Ag(111) does not fit the simple Fresnel model. We interpret this as the influence of surface photoemission. By comparison to Cu(001), we show that the expected intensity distributions of the Fresnel model for one-photon photoemission and two-photon photoemission are valid for an orientation of the momentum matrix element along the surface normal if the influence of additional effects like surface photoemission can be neglected.

  1. Ultrafast surface dynamics probed with time resolved photoemission

    NASA Astrophysics Data System (ADS)

    Dell'Angela, M.; Hieke, F.; Sorgenfrei, F.; Gerken, N.; Beye, M.; Gerasimova, N.; Redlin, H.; Wurth, W.

    2016-01-01

    Time resolved core level photoemission (trXPS) allows real-time atom-specific investigation of ultrafast surface dynamics. Core levels contain information on the chemical state and the structure of the surface as well as the local charge distribution around specific atoms. Monitoring their evolution after optically exciting the surface, can give valuable information on the electronic (few picosecond time scale) and lattice dynamics (several picosecond timescale). We have performed a trXPS experiment at the free-electron laser FLASH at DESY in Hamburg on a clean Ir(111) surface measuring the temporal evolution of the 4f core levels of Ir(111) after optically exciting the sample. The spectral changes due to X-ray and optical laser induced space charge effects which occur in trXPS experiments with high fluence pump and probe pulses have been fully characterized and controlled during the measurements. At early time scales after the optical excitation we observe time-dependent energy shifts and intensity changes which can be partially attributed to the formation of sidebands. Furthermore, we can clearly identify contributions which result from a change in the surface electron density which then relaxes on a time scale on the order of 2 ps.

  2. First-principles interpretation of core-level spectroscopy of photoelectrochemical materials and processes

    NASA Astrophysics Data System (ADS)

    Pemmaraju, Sri Chaitanya Das; Prendergast, David

    2014-03-01

    We present two case studies of first-principles theoretical methods applied in conjunction with experimental core-level spectroscopy measurements to investigate the electronic structure and dynamical processes in molecular and interfacial systems relevant to photoelectrochemical (PEC) technologies. In the first, we study the core-level and valence spectroscopies of two zinc(II)-porphyrin based Donor-pi-Acceptor (D-p-A) dyes using the occupancy-constrained excited electron and core-hole (XCH) approach and time-dependent density functional theory (TDDFT) simulations. In the second, we use constrained DFT and TDDFT to interpret measured transient core-level shifts in time-resolved femtosecond x-ray photoelectron spectroscopy, investigating the dynamics of the electron injection process from a N3 dye molecule chemisorbed onto a ZnO substrate. These studies illustrate the utility of first-principles methods in guiding the design of better PEC materials. This work was performed at the Molecular Foundry, LBNL, supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.

  3. Electron-ion-ion triple-coincidence spectroscopic study of site-specific fragmentation caused by Si:2p core-level photoionization of F{sub 3}SiCH{sub 2}CH{sub 2}Si(CH{sub 3}){sub 3} vapor

    SciTech Connect

    Nagaoka, S.; Hino, M.; Takemoto, M.; Pruemper, G.; Fukuzawa, H.; Liu, X.-J.; Lischke, T.; Ueda, K.; Tamenori, Y.; Harries, J.; Suzuki, I. H.; Takahashi, O.; Okada, K.; Tabayashi, K.

    2007-02-15

    Site-specific fragmentation caused by Si:2p core-level photoionization of F{sub 3}SiCH{sub 2}CH{sub 2}Si(CH{sub 3}){sub 3} vapor was studied by means of high-resolution energy-selected-electron photoion-photoion triple-coincidence spectroscopy. The ab initio molecular orbital method was used for the theoretical description. F{sub 3}SiCH{sub 2}CH{sub 2}{sup +}-Si(CH{sub 3}){sub 3}{sup +} ion pairs were produced by the 2p photoionization of the Si atoms bonded to the three methyl groups, and SiF{sup +}-containing ion pairs were produced by the 2p photoionization of the Si atoms bonded to the three F atoms.

  4. Angle-resolved electron-energy-loss study of core-level electron excitation in molecules: Determination of the generalized oscillator strength for the carbon 1 s (2. sigma. sub g r arrow 2. pi. sub u ) excitation in CO sub 2

    SciTech Connect

    Boechat Roberty, H.M.; Bielschowsky, C.E.; de Souza, G.G.B. )

    1991-08-01

    As part of a systematic, quantitative study of the angle dependence of core-level-electron excitation by electron impact, we have determined the generalized oscillator strength (GOS) for the carbon 1{ital s}(2{sigma}{sub {ital g}}{r arrow}2{pi}{sub {ital u}}) transition in CO{sub 2}. The experimental results were obtained at an impact energy of 1290 eV, in the angular range of 2{degree}--14{degree}, with an energy resolution of 0.9 eV. Theoretical values for the GOS were also obtained, using {ital ab} {ital initio} Hartree-Fock molecular wave functions and allowing for the relaxation of all the molecular orbitals in the determination of the excited-state wave function.

  5. Valence band study of Sm0.1Ca0.9 - xSrxMnO3 using high resolution photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Dalai, Manas Kumar; Sekhar, Biju Raja; Biswas, Deepnarayan; Thakur, Sangeeta; Maiti, Kalobaran; Chiang, Tai-Chang; Martin, Christine

    2014-03-01

    We have studied the valence band electronic structure of Sm0.1Ca0.9- xSrxMnO3 (x = 0, 0.1, 0.3 and 0.6) at various temperatures using high resolution photoemission spectroscopy (HRPES). The data were taken using a Scienta R4000 energy analyser and the resolution was set at 5 meV. The doping dependent studies of Sm0.1Ca0.9-x SrxMnO3 at 50 K, 100 K and 295 K are quite interesting. The density of eg states near the Fermi level decreases with Sr substitution at the Ca site at 50 K. Also the similar trend has been observed at 100 K. At 295 K the changes in the eg states is quite different than the earlier temperatures where the intensity remains the same for x = 0, 0.1 and 0.3 and then decreases for x = 0.6. These changes in the density of states near the Fermi level will be explained by taking into account the structural, electrical and magnetic properties associated with this system. Permanent affiliation of Manas Kumar Dalai ; CSIR-National Physical Laboratory, New Delhi-110012, India. MKD acknowledges the Indo-US Science and Technology Forum (IUSSTF) for the fellowship.

  6. HREELS and photoemission study of GaSb( 1 0 0 )-(1×3) surfaces prepared by optimal atomic hydrogen cleaning

    NASA Astrophysics Data System (ADS)

    Veal, T. D.; Lowe, M. J.; McConville, C. F.

    2002-03-01

    High-resolution electron-energy-loss spectroscopy (HREELS) and synchrotron-radiation photoemission spectroscopy (SRPES) have been used to study the Sb-stabilised GaSb(1 0 0)-(1×3) surface prepared by a two-stage low-temperature atomic hydrogen cleaning (AHC) procedure. The use of a maximum annealing temperature of 300 °C avoids the degradation of surface stoichiometry associated with higher annealing temperatures. After AHC at a sample temperature of 100 °C, SRPES results show that all Sb oxides have been removed and only a small amount of Ga oxide remains. Further AHC treatment at 300 °C results in a clean surface with a sharp (1×3) low energy electron diffraction pattern. SRPES results indicate that the surface stoichiometry is identical to that previously found for GaSb(1 0 0)-(1×3) prepared by in situ molecular beam epitaxy. Electron energy-dependent HREEL spectra exhibit a coupled plasmon-phonon mode which has been used to study the electronic structure of the near-surface region. Semi-classical dielectric theory simulations of the HREEL spectra of the clean GaSb(1 0 0)-(1×3) surface indicate no detectable electronic damage or dopant passivation results from the AHC treatment. Valence band SRPES indicates that the surface Fermi level is close to the valence band maximum, suggesting the presence of an inversion layer at the surface.

  7. Electronic structure of Ce2RhIn8: A two-dimensional heavy-fermion system studied by angle-resolved photoemission spectroscopy

    DOE PAGES

    Jiang, Rui; Mou, Daixing; Liu, Chang; Zhao, Xin; Yao, Yongxin; Ryu, Hyejin; Petrovic, C.; Ho, Kai -Ming; Kaminski, Adam

    2015-04-01

    We use angle-resolved photoemission spectroscopy (ARPES) to study the 2D heavy fermion superconductor, Ce₂RhIn₈. The Fermi surface is rather complicated and consists of several hole and electron pockets with one of the sheets displaying strong nesting properties with a q-vector of (0.32, 0.32) π/a. We do not observe kz dispersion of the Fermi sheets, which is consistent with the expected 2D character of the electronic structure. Comparison of the ARPES data to band structure calculations suggests that a localized picture of the f-electrons works best. While there is some agreement in the overall band dispersion and location of the Fermimore » sheets, the model does not reproduce all observed bands and is not completely accurate for those it does. As a result, our data paves the way for improving the band structure calculations and the general understanding of the transport and thermodynamical properties of this material.« less

  8. Coupling parameters of many-body interactions for the Al(100) surface state: A high-resolution angle-resolved photoemission spectroscopy study

    NASA Astrophysics Data System (ADS)

    Jiang, J.; Shimada, K.; Hayashi, H.; Iwasawa, H.; Aiura, Y.; Namatame, H.; Taniguchi, M.

    2011-10-01

    We examined the dimensionless coupling parameters of many-body interactions for a free-electron-like surface-derived state in Al(100) by means of high-resolution angle-resolved photoemission spectroscopy. A kink structure was found to exist in the energy-band dispersion near the Fermi level (EF), which was attributed to the electron-phonon interaction. At 50 K, the coupling parameters of the electron-phonon and electron-electron interactions were estimated as λep=0.67±0.05 and λee˜0.003, respectively, indicating that the effective mass enhancement was mainly derived from the electron-phonon interaction. The temperature dependence of the kink structure, as measured by λep(T), was consistent with a theoretical calculation based on the Eliashberg function. A quasiparticle peak with a width of 15-20 meV was found near EF, which was explained well by the simulated spectral function incorporating the self-energy evaluated in this study. We found that the electrons at the surface were strongly scattered by the defects at the surface and that the linewidth was significantly broadened (Γ0=0.238±0.006 eV).

  9. Observation of core-level binding energy shifts between (100) surface and bulk atoms of epitaxial CuInSe{sub 2}

    SciTech Connect

    Nelson, A.J.; Berry, G.; Rockett, A.

    1997-04-01

    Core-level and valence band photoemission from semiconductors has been shown to exhibit binding energy differences between surface atoms and bulk atoms, thus allowing one to unambiguously distinguish between the two atomic positions. Quite clearly, surface atoms experience a potential different from the bulk due to the lower coordination number - a characteristic feature of any surface is the incomplete atomic coordination. Theoretical accounts of this phenomena are well documented in the literature for III-V and II-VI semiconductors. However, surface state energies corresponding to the equilibrium geometry of (100) and (111) surfaces of Cu-based ternary chalcopyrite semiconductors have not been calculated or experimental determined. These compounds are generating great interest for optoelectronic and photovoltaic applications, and are an isoelectronic analog of the II-VI binary compound semiconductors. Surface core-level binding energy shifts depend on the surface cohesive energies, and surface cohesive energies are related to surface structure. For ternary compound semiconductor surfaces, such as CuInSe{sub 2}, one has the possibility of variations in surface stoichiometry. Applying standard thermodynamical calculations which consider the number of individual surface atoms and their respective chemical potentials should allow one to qualitatively determine the magnitude of surface core-level shifts and, consequently, surface state energies.

  10. Doping Dependence of the $(\\pi,\\pi)$ Shadow Band in La-Based Cuprates Studied by Angle-Resolved Photoemission Spectroscopy

    SciTech Connect

    Shen, Z. X.

    2011-08-15

    The ({pi},{pi}) shadow band (SB) in La-based cuprate family (La214) was studied by angle-resolved photoemission spectroscopy (ARPES) over a wide doping range from x = 0.01 to x = 0.25. Unlike the well-studied case of the Bi-based cuprate family, an overall strong, monotonic doping dependence of the SB intensity at the Fermi level (E{sub F}) was observed. In contrast to a previous report for the presence of the SB only close to x = 1/8, we found it exists in a wide doping range, associated with a doping-independent ({pi},{pi}) wave vector but strongly doping-dependent intensity: It is the strongest at x {approx} 0.03 and systematically diminishes as the doping increases until it becomes negligible in the overdoped regime. This SB with the observed doping dependence of intensity can in principle be caused by the antiferromagnetic fluctuations or a particular form of low-temperature orthorhombic lattice distortion known to persist up to x {approx} 0.21 in the system, with both being weakened with increasing doping. However, a detailed binding energy dependent analysis of the SB at x = 0.07 does not appear to support the former interpretation, leaving the latter as a more plausible candidate, despite a challenge in quantitatively linking the doping dependences of the SB intensity and the magnitude of the lattice distortion. Our finding highlights the necessity of a careful and global consideration of the inherent structural complications for correctly understanding the cuprate Fermiology and its microscopic implication.

  11. Plasmon-exciton coupling at Ag nanocluster decorated TiO2(110) surface studied by time-resolved two-photon photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Tan, Shijing; Argondizzo, Adam; Petek, Hrvoje

    We study the spectroscopy and electron dynamics at Ag nanocluster decorated TiO2(110) surface upon photoexcitation of plasmonic modes by two-photon photoemission spectroscopy (2PP). Depositing Ag onto a reduced rutile TiO2(110) surface at room temperature forms pancake-like Ag particles with an average diameter of 4 nm and height of 1.5 nm. Measurements of the 2PP yield from Ag/TiO2 surface with tunable femtosecond laser excitation show enhancement at plasmonic resonances. Exciting with s-polarization (S -->) the plasmonic resonance enhancement has a single peak at 3.1 eV, whereas with p-polarization (P -->) there is an additional more intense resonance at 3.8 eV. We attribute the 3.1 and 3.8 eV peaks to the in-plane and the surface-normal plasmon modes respectively. Crystal azimuth orientation dependent excitation with (S -->) shows an anisotropy in the 2PP spectra for the 3.1 eV in-plane plasmon mode when the laser electric field is aligned in the [001] vs. [ 1 1 0 ] directions. The existence of two plasmon modes and the in-plane plasmon anisotropy imply that the plasmon modes are perturbed by coherent coupling with excitons in the rutile TiO2 substrate. We speculate that plasmon-exciton resonant energy transfer could play an important role in the plasmonically enhanced photocatalysis at the Ag/TiO2 surface.

  12. Momentum resolution in inverse photoemission

    SciTech Connect

    Zumbülte, A.; Schmidt, A. B.; Donath, M.

    2015-01-15

    We present a method to determine the electron beam divergence, and thus the momentum resolution, of an inverse-photoemission setup directly from a series of spectra measured on Cu(111). Simulating these spectra with different beam divergences shows a distinct influence of the divergence on the appearance of the Shockley surface state. Upon crossing the Fermi level, its rise in intensity can be directly linked with the beam divergence. A comparison of measurement and simulation enables us to quantify the momentum resolution independent of surface quality, energy resolution, and experimental geometry. With spin resolution, a single spectrum taken around the Fermi momentum of a spin-split surface state, e.g., on Au(111), is sufficient to derive the momentum resolution of an inverse-photoemission setup.

  13. Momentum resolution in inverse photoemission.

    PubMed

    Zumbülte, A; Schmidt, A B; Donath, M

    2015-01-01

    We present a method to determine the electron beam divergence, and thus the momentum resolution, of an inverse-photoemission setup directly from a series of spectra measured on Cu(111). Simulating these spectra with different beam divergences shows a distinct influence of the divergence on the appearance of the Shockley surface state. Upon crossing the Fermi level, its rise in intensity can be directly linked with the beam divergence. A comparison of measurement and simulation enables us to quantify the momentum resolution independent of surface quality, energy resolution, and experimental geometry. With spin resolution, a single spectrum taken around the Fermi momentum of a spin-split surface state, e.g., on Au(111), is sufficient to derive the momentum resolution of an inverse-photoemission setup.

  14. Photoemission Spectroscopy of Delta- Plutonium: Experimental Review

    NASA Astrophysics Data System (ADS)

    Tobin, J. G.

    2002-03-01

    The electronic structure of Plutonium, particularly delta- Plutonium, remains ill defined and without direct experimental verification. Recently, we have embarked upon a program of study of alpha- and delta- Plutonium, using synchrotron radiation from the Advanced Light Source in Berkeley, CA, USA [1]. This work is set within the context of Plutonium Aging [2] and the complexities of Plutonium Science [3]. The resonant photoemission of delta-plutonium is in partial agreement with an atomic, localized model of resonant photoemission, which would be consistent with a correlated electronic structure. The results of our synchrotron- based studies will be compared with those of recent laboratory- based works [4,5,6]. The talk will conclude with a brief discussion of our plans for the future, such as the performance of spin-resolving and dichroic photoemission measurements of Plutonium [7] and the development of single crystal ultrathin films of Plutonium. This work was performed under the auspices of the U.S. Department of Energy by the University of California, Lawrence Livermore National Laboratory under Contract No. W-7405-Eng-48. 1. J. Terry, R.K. Schulze, J.D. Farr, T. Zocco, K. Heinzelman, E. Rotenberg, D.K. Shuh, G. van der Laan, D.A. Arena, and J.G. Tobin, “5f Resonant Photoemission from Plutonium”, UCRL-JC-140782, Surf. Sci. Lett., accepted October 2001. 2. B.D. Wirth, A.J. Schwartz, M.J. Fluss, M.J. Caturla, M.A. Wall, and W.G. Wolfer, MRS Bulletin 26, 679 (2001). 3. S.S. Hecker, MRS Bulletin 26, 667 (2001). 4. T. Gouder, L. Havela, F. Wastin, and J. Rebizant, Europhys. Lett. 55, 705 (2001); MRS Bulletin 26, 684 (2001); Phys. Rev. Lett. 84, 3378 (2000). 5. A.J. Arko, J.J. Joyce, L. Morales, J. Wills, J. Lashley, F. Wastin, and J. Rebizant, Phys. Rev. B 62, 1773 (2000). 6. L.E. Cox, O. Eriksson, and B.R. Cooper, Phys. Rev. B 46, 13571 (1992). 7. J. Tobin, D.A. Arena, B. Chung, P. Roussel, J. Terry, R.K. Schulze, J.D. Farr, T. Zocco, K. Heinzelman, E

  15. Chemical potential shift and gap-state formation in SrTiO{sub 3−δ} revealed by photoemission spectroscopy

    SciTech Connect

    Pal, Prabir Kumar, Pramod; Aswin, V.; Dogra, Anjana; Joshi, Amish G.

    2014-08-07

    In this study, we report on investigations of the electronic structure of SrTiO{sub 3} annealed at temperature ranging between 550 and 840 °C in an ultrahigh vacuum. Annealing induced oxygen vacancies (O{sub vac}) impart considerable changes in the electronic structure of SrTiO{sub 3}. Using core-level photoemission spectroscopy, we have studied the chemical potential shift (Δμ) as a function of annealing temperature. The result shows that the chemical potential monotonously increases with electron doping in SrTiO{sub 3−δ}. The monotonous increase of the chemical potential rules out the existence of electronic phase separation in the sample. Using valence band photoemission, we have demonstrated the formation of a low density of states at the near Fermi level electronic spectrum of SrTiO{sub 3−δ}. The gap-states were observed by spectral weight transfer over a large energy scale of the stoichiometric band gap of SrTiO{sub 3} system leading finally to an insulator-metal transition. We have interpreted our results from the point of structural distortions induced by oxygen vacancies.

  16. Photoemission Electron Microscopy of a Plasmonic Silver Nanoparticle Trimer

    SciTech Connect

    Peppernick, Samuel J.; Joly, Alan G.; Beck, Kenneth M.; Hess, Wayne P.; Wang, Jinyong; Wang, Yi-Chung; Wei, Wei

    2013-07-01

    We present a combined experimental and theoretical study to investigate the spatial distribution of photoelectrons emitted from core-shell silver (Ag) nanoparticles. We use two-photon photoemission microscopy (2P-PEEM) to spatially resolve electron emission from a trimeric core-shell aggregate of triangular symmetry. Finite difference time domain (FDTD) simulations are performed to model the intensity distributions of the electromagnetic near-fields resulting from femtosecond (fs) laser excitation of localized surface plasmon oscillations in the triangular core-shell structure. We demonstrate that the predicted FDTD near-field intensity distribution reproduces the 2P-PEEM photoemission pattern.

  17. Photocathode device that replenishes photoemissive coating

    DOEpatents

    Moody, Nathan A.; Lizon, David C.

    2016-06-14

    A photocathode device may replenish its photoemissive coating to replace coating material that desorbs/evaporates during photoemission. A linear actuator system may regulate the release of a replenishment material vapor, such as an alkali metal, from a chamber inside the photocathode device to a porous cathode substrate. The replenishment material deposits on the inner surface of a porous membrane and effuses through the membrane to the outer surface, where it replenishes the photoemissive coating. The rate of replenishment of the photoemissive coating may be adjusted using the linear actuator system to regulate performance of the photocathode device during photoemission. Alternatively, the linear actuator system may adjust a plasma discharge gap between a cartridge containing replenishment material and a metal grid. A potential is applied between the cartridge and the grid, resulting in ejection of metal ions from the cartridge that similarly replenish the photoemissive coating.

  18. O 1s core-level shifts at the anatase TiO2(101)/N3 photovoltaic interface: Signature of H-bonded supramolecular assembly

    NASA Astrophysics Data System (ADS)

    Patrick, Christopher E.; Giustino, Feliciano

    2011-08-01

    We here report an atomic-scale first-principles investigation of the O 1s core-level shifts at the interface between TiO2 and the dye N3 found in dye-sensitized solar cells. We first perform extensive validation of our computational setup in the case of small molecules containing carboxylic acid groups in the gas phase. Then we calculate the O 1s core-level shifts for a variety of atomistic models of the TiO2/N3 interface. We investigate in detail the effects of water contamination, dye packing density, exchange and correlation functionals, and hydrogen-bonding interactions on the calculated core-level spectra. The quantitative comparison between our calculated core-level shifts and measured photoemission spectra [Johansson , J. Phys. Chem. BJPCBFK1520-610610.1021/jp0525282 109, 22256 (2005)] leads us to propose a new atomic-scale model of the TiO2/N3 interface, where the dyes are arranged in supramolecular H-bonded assemblies. Our interface models describe dry TiO2/N3 films as in [Johansson , J. Phys. Chem. BJPCBFK1520-610610.1021/jp0525282 109, 22256 (2005)], and are of direct relevance to solid-state dye-sensitized solar cells. Our present work suggests that the adsorption energetics is not a reliable indicator of the quality of an interface model, and highlights the importance of combining experimental and computational spectroscopy for determining the atomic-scale structure of nanostructured solar cell interfaces.

  19. The reaction of lithium with dimethyl carbonate and diethyl carbonate in ultrahigh vacuum studied by X-ray photoemission spectroscopy

    SciTech Connect

    Zhuang, G.; Chen, Y.; Ross, P.N. Jr.

    1999-02-16

    The reaction of dimethyl carbonate (DMC) and diethyl carbonate (DEC) with clean metallic lithium in ultrahigh vacuum was studied by the use of X-ray photoelectron spectroscopy with the temperature-programmed reaction methodology. Both molecules are of interest as solvents in ambient-temperature lithium batteries. The solvent molecules were condensed onto the surface of an evaporated lithium film at 120 K, and spectra were collected as the sample was warmed in ca. 25 to 30-K increments. The reaction of either DMC or DEC with lithium was initiated at 180 K, a temperature much lower than their bulk melting temperatures, producing lithium methyl carbonate, methyllithium and lithium ethyl carbonate, and ethyllithium, respectively. At temperatures greater than 270--300 K, the lithium alkyl carbonates start to decompose with Li{sub 2}O, elemental carbon, and alkyllithium as products on the surface. Both DMC and DEC are more reactive toward metallic Li than another carbonate solvent, propylene carbonate, which the authors have studied by the same methodology. Because methyl and ethyllithium are highly soluble in the parent solvent, electrodeposited Li is predicted to have poor stability in an electrolyte composed of either DMC or DEC.

  20. Surface and subsurface properties of a BaLi 4 gettering alloy studied using X-ray photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Magnano, E.; Vandré, S.; Kovac, J.; Narducci, E.; Caloi, R.; Manini, P.; Sancrotti, M.

    1998-05-01

    A barium-lithium alloy in a 1:4 atomic ratio is analysed using XPS and Ar +-ion depth profiling. The effects induced by RT gas exposure (air, N 2 and O 2) and vacuum annealing at low temperature (100°C) are studied in detail. A strong reactivity of the alloy surface is found, even at RT. Dosing BaLi 4 with N 2 does not lead to an appreciable change in the nitrogen surface concentration. However, its concentration increases after repeated Ar + sputtering, demonstrating the existence of a chemical reaction with the bulk alloy. This is shown to be in good agreement with N 2 sorption tests carried out at RT on BaLi 4 powder.

  1. Exploring electronic structure of one-atom thick polycrystalline graphene films: A nano angle resolved photoemission study

    PubMed Central

    Avila, José; Razado, Ivy; Lorcy, Stéphane; Fleurier, Romain; Pichonat, Emmanuelle; Vignaud, Dominique; Wallart, Xavier; Asensio, María C.

    2013-01-01

    The ability to produce large, continuous and defect free films of graphene is presently a major challenge for multiple applications. Even though the scalability of graphene films is closely associated to a manifest polycrystalline character, only a few numbers of experiments have explored so far the electronic structure down to single graphene grains. Here we report a high resolution angle and lateral resolved photoelectron spectroscopy (nano-ARPES) study of one-atom thick graphene films on thin copper foils synthesized by chemical vapor deposition. Our results show the robustness of the Dirac relativistic-like electronic spectrum as a function of the size, shape and orientation of the single-crystal pristine grains in the graphene films investigated. Moreover, by mapping grain by grain the electronic dynamics of this unique Dirac system, we show that the single-grain gap-size is 80% smaller than the multi-grain gap recently reported by classical ARPES. PMID:23942471

  2. Core-level shifts in fcc random alloys: A first-principles approach

    NASA Astrophysics Data System (ADS)

    Olovsson, W.; Göransson, C.; Pourovskii, L. V.; Johansson, B.; Abrikosov, I. A.

    2005-08-01

    First-principles theoretical calculations of the core-level binding-energy shift (CLS) for eight binary face-centered-cubic (fcc) disordered alloys, CuPd, AgPd, CuNi, NiPd, CuAu, PdAu, CuPt, and NiPt, are carried out within density-functional theory (DFT) using the coherent potential approximation. The shifts of the Cu and Ni 2p3/2 , Ag and Pd 3d5/2 , and Pt and Au 4f7/2 core levels are calculated according to the complete screening picture, which includes both initial-state (core-electron energy eigenvalue) and final-state (core-hole screening) effects in the same scheme. The results are compared with available experimental data, and the agreement is shown to be good. The CLSs are analyzed in terms of initial- and final-state effects. We also compare the complete screening picture with the CLS obtained by the transition-state method, and find very good agreement between these two alternative approaches for the calculations within the DFT. In addition the sensitivity of the CLS to relativistic and magnetic effects is studied.

  3. Core-Level Crossing and the High-Pressure Equation of State of Heavy Elements

    NASA Astrophysics Data System (ADS)

    Wills, John

    2015-06-01

    The structural properties of the 5d transition metal osmium have recently been probed at static pressures up to ~ 770 GPa. In this study, anomalies in the hcp c/a ratio were found at pressures of in the vicinity of 150 GPa and 440 GPa. The anomaly at 150 GPa approximately coincides in pressure with an electron topological transition (ETT) observed in Density Functional Theory (DFT) band structure. However, no ETT is observed at higher pressures. Instead, we find that the anomaly in the c / a ratio of osmium is correlated with the crossing of the 5p3 / 2 and 4f7 / 2 ``core'' levels, which at this pressure are found to have bandwidths ~ .2-.3 Ry, in our DFT calculations. In this talk, I discuss the calculated structural properties and calculated equation of state of osmium and other heavy 5d elements at pressures less than 1 TPa and the effect of core-level crossing on the equation of state and structural properties of these elements.

  4. Wigner photoemission time delay from endohedral anions

    NASA Astrophysics Data System (ADS)

    Kumar, Ashish; Varma, Hari R.; Deshmukh, Pranawa C.; Manson, Steven T.; Dolmatov, Valeriy K.; Kheifets, Anatoli

    2016-10-01

    Characteristic features of Wigner photoemission time delay from endohedral anions A@C60q along with their dependence on the anion charge q are unraveled. Specifically, significant enhancement of the time delay in the innermost dipole photoionization channels near threshold is found, owing to the presence of the Coulomb confined resonances (CRs). Moreover, it is shown that interchannel coupling of the inner-shell Coulomb CRs with outer-shell photoionization channels results in resonantly enhanced time delay in the release of the outer-shell photoelectron well above, several hundreds eV, the outer-shell thresholds. It is also demonstrated that, and explained why, photoionization cross sections of the innermost subshells as well as outer subshells (near the inner-subshell threshold) depends only very weakly on the anion charge q , but the dependence of the corresponding time delays on q can be significant. Furthermore, Coulomb CRs are found to emerge in the innermost quadrupole photoionization channels as well, thereby causing considerable time delay in the quadrupole photoemission. These findings are illustrated in calculations of the photoionization of inner and outer subshells of the endohedral anions Ne@C60-1 and Ne@C60-5 that were chosen as case studies.

  5. Momentum dependence of 4f hybridization in heavy-fermion compounds: Angle-resolved photoemission study of YbIr2Si2 and YbRh2Si2

    SciTech Connect

    Danzenbacher, S.; Kucherenko, Y.; Vyalikh, D.V.; Holder, M.; Laubschat, C.; Yaresko, A.N.; Krellner, C.; Hossain, Z.; Geibel, C.; Zhou, X.J.; Yang, W.L.; Mannella, N.; Hussain, Z.; Shen, Z.X.; Shi, M.; Patthey, L.; Molodtsov, S.L.

    2010-04-15

    Heavy-fermion compounds YbIr2Si2 and YbRh2Si2 were studied by means of angle-resolved photoemission (PE). The splittings and dispersions of the 4f13 bulk and surface PE signals in the region of the expected energy crossings of the 4f final states and the valence bands in the Brillouin zone are observed. The experimental results are explained in terms of a simplified periodic Anderson model by a momentum dependence of the electron hopping matrix element between the 4f and valence-band states.

  6. 3s- and 3p-core level excitations in 3d-transition metal oxides from electron-energy-loss spectroscopy

    NASA Astrophysics Data System (ADS)

    Steiner, P.; Zimmermann, R.; Reinert, F.; Engel, Th.; Hüfner, S.

    1995-03-01

    3s- and 3p-core level excitations for a large number of 3d-transition metal oxides, with a formal 3d occupation from 3d0 to 3d10, have been measured by electron energy loss spectroscopy in reflection geometry (REELS) with primary energies 200 eV≤ E 0≤1600 eV. Their intensities decrease systematically with the formal 3d-count, classifying them as transitions to empty 3d-states. The structure of the 3s excitations is analysed in detail and is compared to the 3s-XPS photoemission spectra of the samples. This 3s-REELS structure and its change with the 3d occupation can be explained by the assumption that the excitation arises mainly from a 3s23dn→3s13dn+1 quadrupole transition.

  7. Relativistic calculations of angle-dependent photoemission time delay

    NASA Astrophysics Data System (ADS)

    Kheifets, Anatoli; Mandal, Ankur; Deshmukh, Pranawa C.; Dolmatov, Valeriy K.; Keating, David A.; Manson, Steven T.

    2016-07-01

    Angular dependence of photoemission time delay for the valence n p3 /2 and n p1 /2 subshells of Ar, Kr, and Xe is studied in the dipole relativistic random phase approximation. Strong angular anisotropy of the time delay is reproduced near respective Cooper minima while the spin-orbit splitting affects the time delay near threshold.

  8. Core-level spectroscopy investigation of the Mo{sub 0.75}Re{sub 0.25}(100) surface

    SciTech Connect

    Lyman, P.F.; Zehner, D.M.

    1993-10-01

    Preferential surface segregation in the Mo{sub 0.75}(100) surface region was investigated using high-resolution core-level spectroscopy with synchrotron radiation. The magnitude and direction of the surface core-level shifts observed in this study can be qualitatively understood by comparison to W and Mo core-level shifts. Measured core-level intensities are found to be consistent with the segregation of Mo to the surface of the alloy, with an enrichment of Re in the second layer (as found in previous investigations). It is inferred that both Tc and Os will segregate to the Mo{sub 0.75}Re{sub 0.25}(100) surface.

  9. Angle Resolved Photoemission Spectroscopy Studies of the Mott Insulator to Superconductor Evolution in Ca2-xNaxCuO2Cl2

    SciTech Connect

    Shen, Kyle Michael

    2005-09-02

    It is widely believed that many of the exotic physical properties of the high-T{sub c} cuprate superconductors arise from the proximity of these materials to the strongly correlated, antiferromagnetic Mott insulating state. Therefore, one of the fundamental questions in the field of high-temperature superconductivity is to understand the insulator-to-superconductor transition and precisely how the electronic structure of Mott insulator evolves as the first holes are doped into the system. This dissertation presents high-resolution, doping dependent angle-resolved photoemission (ARPES) studies of the cuprate superconductor Ca{sub 2-x}Na{sub x}CuO{sub 2}Cl{sub 2}, spanning from the undoped parent Mott insulator to a high-temperature superconductor with a T{sub c} of 22 K. A phenomenological model is proposed to explain how the spectral lineshape, the quasiparticle band dispersion, and the chemical potential all progress with doping in a logical and self-consistent framework. This model is based on Franck-Condon broadening observed in polaronic systems where strong electron-boson interactions cause the quasiparticle residue, Z, to be vanishingly small. Comparisons of the low-lying states to different electronic states in the valence band strongly suggest that the coupling of the photohole to the lattice (i.e. lattice polaron formation) is the dominant broadening mechanism for the lower Hubbard band states. Combining this polaronic framework with high-resolution ARPES measurements finally provides a resolution to the long-standing controversy over the behavior of the chemical potential in the high-T{sub c} cuprates. This scenario arises from replacing the conventional Fermi liquid quasiparticle interpretation of the features in the Mott insulator by a Franck-Condon model, allowing the reassignment of the position of the quasiparticle pole. As a function of hole doping, the chemical potential shifts smoothly into the valence band while spectral weight is transferred

  10. Electric field and temperature dependence of dielectric permittivity in strontium titanate investigated by a photoemission study on Pt/SrTiO{sub 3}:Nb junctions

    SciTech Connect

    Hirose, Sakyo; Okushi, Hideyo; Yoshikawa, Hideki; Adachi, Yutaka; Ohsawa, Takeo; Haneda, Hajime; Ueda, Shigenori; Ando, Akira; Ohashi, Naoki

    2015-05-11

    Schottky junctions made from platinum and niobium-doped strontium titanate (SrTiO{sub 3}:Nb) were investigated by hard X-ray photoemission (HXPES) and through a band bending behavior simulation using a phenomenological model, which assumes a decrease in dielectric constant due to an electric field. Thus, we confirmed that the observed HXPES spectra at relatively high temperatures, e.g., >250 K, were well simulated using this phenomenological model. In contrast, it was inferred that the model was not appropriate for junction behavior at lower temperatures, e.g., <150 K. Therefore, a reconstruction of the phenomenological model is necessary to adequately explain the dielectric properties of SrTiO{sub 3}.

  11. FeMn/Fe/Co/Cu(1,1,10) films studied using the magneto-optic Kerr effect and photoemission electron microscopy

    SciTech Connect

    Meng, Y.; Li, J.; Tan, A.; Park, J.; Jin, E.; Son, H.; Doran, A.; Scholl, A.; Arenholz, E.; Zhao, H. W.; Hwang, Chanyong; Qiu, Z. Q.

    2011-07-31

    FeMn/Fe/Co/Cu(1,1,10) films were grown epitaxially and investigated using the magneto-optic Kerr effect and photoemission electron microscopy. We found that FeMn/Fe/Co/Cu(1,1,10) exhibits the same properties as FeMn/Co/Cu(1,1,10) for the ferromagnetic phase of the face centered cubic (fcc) Fe film but a different property for the non-ferromagnetic phase of the fcc Fe film. This result indicates that the characteristic property reported in the literature for FeMn/Co/Cu(001) comes from the FeMn spin structure and is independent of the ferromagnetic layer.

  12. Core-level excitation and fragmentation of chlorine dioxide

    NASA Astrophysics Data System (ADS)

    Flesch, R.; Plenge, J.; Rühl, E.

    2006-03-01

    Inner-shell excitation and fragmentation of chlorine dioxide (OClO) in the Cl 2p- and O 1s-excitation regime is reported. The electronic structure of the element-selectively excited radical is studied by X-ray absorption and total cation yields. A comparison of both approaches allows us to estimate the absolute photoionization cross-section and the ionization yield near the Cl 2p- and O 1s-absorption edges. The latter quantity is characteristically enhanced in core-ionization continua. We observe below both core-absorption edges intense core-to-valence-transitions. These are assigned in comparison with related work on core-excited sulfur dioxide. These results give clear evidence that the highest molecular orbital of OClO is half-filled. High-resolution spectra recorded in the Cl 2p-regime show evidence for Rydberg transitions. The extrapolation of the term values of the low-lying Rydberg states allows us to derive the Cl 2p-ionization energy of OClO. Fragmentation of core-excited OClO is reported. Photoelectron-photoion-coincidence (PEPICO) spectra are recorded, indicating that singly and doubly charged fragments are formed. Fission of the doubly and multiply charged OClO leads to singly charged fragments. These are measured by photoion-photoion-coincidence (PIPICO) spectra, where characteristic changes in intensity of the fission channels in the Cl 2p- and O 1s-continuum are observed.

  13. Laser-assisted photoemission from surfaces

    SciTech Connect

    Saathoff, G.; Miaja-Avila, L.; Murnane, M. M.; Kapteyn, H. C.; Aeschlimann, M.

    2008-02-15

    We investigate the laser-assisted photoelectric effect from a solid surface. By illuminating a Pt(111) sample simultaneously with ultrashort 1.6 and 42 eV pulses, we observe sidebands in the extreme ultraviolet photoemission spectrum, and accurately extract their amplitudes over a wide range of laser intensities. Our results agree with a simple model, in which soft x-ray photoemission is accompanied by the interaction of the photoemitted electron with the laser field. This strong effect can definitively be distinguished from other laser surface interaction phenomena, such as hot electron excitation, above-threshold photoemission, and space-charge acceleration. Thus, laser-assisted photoemission from surfaces promises to extend pulse duration measurements to higher photon energies, as well as opening up measurements of femtosecond-to-attosecond electron dynamics in solid and surface-adsorbate systems.

  14. Coherent and incoherent processes in resonant photoemission

    SciTech Connect

    Magnuson, M.; Karis, O.; Weinelt, M.

    1997-04-01

    In this contribution the authors present the distinction between coherent and incoherent processes in resonant photoemission. As a first step they determine whether an autoionization process is photoemission-like or Auger-like. The discussion is based on measurements for a weakly bonded adsorption system, Ar/Pt(111). This type of system is well adapted to investigate these effects since it yields distinctly shifted spectral features depending on the nature of the process. After this, the question of resonance photoemission in metallic systems is addressed. This is done in connection with measurements at the 2p edges for Ni metal. Ni has been one of the prototype systems for resonant photoemission. The resonances have been discussed in connection with the strong correlation and d-band localization effects in this system. Based on the results some general comments about the appearance of resonant effects in metallic systems are made.

  15. Ultrafast angle-resolved photoemission spectroscopy of quantum materials

    NASA Astrophysics Data System (ADS)

    Smallwood, Christopher L.; Kaindl, Robert A.; Lanzara, Alessandra

    2016-07-01

    Techniques in time- and angle-resolved photoemission spectroscopy have facilitated a number of recent advances in the study of quantum materials. We review developments in this field related to the study of incoherent nonequilibrium electron dynamics, the analysis of interactions between electrons and collective excitations, the exploration of dressed-state physics, and the illumination of unoccupied band structure. Future prospects are also discussed.

  16. Photoemission of Alq{sub 3} and C{sub 60} films on Al and LiF/Al substrates

    SciTech Connect

    Joensson, S.K.M.; Salaneck, W.R.; Fahlman, M.

    2005-07-01

    Photoemission studies of thin films of Alq{sub 3} and C{sub 60} deposited on Al and LiF/Al substrates have been performed in order to deduce the interactions of the organic films with the substrates. For all cases there is evidence of strong interaction resulting in the formation of interfacial dipoles. Attempts to explain the origin of these interfacial dipoles and the type of interface formed in each case have been done through analysis of the valence electronic structure and core levels of the materials. The origin of the interfacial dipoles is mainly covalent interaction when the organic films are deposited on Al substrates, and charge transfer between the organic molecules and the metal through the LiF sandwich layer when the organic films are deposited on LiF/Al substrates. For thick-enough LiF films, however, there is no interaction between the organic films and the substrates. In no case does the LiF dissociate, unlike what is found for the reverse order of deposition. Two charge-transfer-induced gap states are found for (sub)monolayer films of Alq{sub 3} deposited on LiF/Al. We propose that the formation of two gap states corresponds to negatively charged fac-Alq{sub 3}.

  17. Nonlinear Photoemission Electron Micrographs of Plasmonic Nanoholes in Gold Thin Films

    SciTech Connect

    Gong, Yu; Joly, Alan G.; El-Khoury, Patrick Z.; Hess, Wayne P.

    2014-11-06

    Nonlinear photoemission electron microscopy of isolated nanoholes in gold thin films map propagating surface plasmon polaritons (SPPs) launched from the lithographically patterned plasmonic structures. A damped sinusoidal elongated ring-like photoemission beat pattern is observed from the nanoholes, following low angle of incidence irradiation of these structures with sub-15 fs 780 nm laser pulses. A notable agreement between finite difference time domain simulations and experiment corroborates our assignment of the observed photoemission patterns to SPPs launched from isolated nanoholes and probed through nonlinear photoemission. We also demonstrate how the efficiency of coupling light waves into isolated plasmonic holes can be tuned by varying hole diameter. In this regard, a simple intuitive geometrical model, which accounts for the observed and simulated diameter dependent plasmonic response, is proposed. Overall, this study paves the way for designing nanohole assemblies where optical coupling and subsequent plasmon propagation can be rationally controlled through 2D SPP interferometry

  18. Calculations of Photoemission from Rutile

    NASA Astrophysics Data System (ADS)

    Hjalmarson, Harold; Schultz, Peter; Moore, Chris

    2015-03-01

    Photoemission is a well-known mechanism for release of electrons from a surface during electrical breakdown of a gas such as air. During air breakdown, UV photons, which are emitted from the highly excited gas molecules, are absorbed in the surfaces such as the cathode and the anode. These absorbed photons create energetic electrons, and a small portion of these electrons reach the surface. Those that overcome the potential energy barrier at the surface tend to be emitted. In this talk, the Boltzmann equation that describes these phenomena is formulated. A Monte Carlo probabilistic method is used to obtain the rate of electron emission as a function of photon energy. The role of bandstructure effects will be discussed. This bandstructure information is obtained by using a density-functional theory (DFT) method. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

  19. PLS photoemission electron microscopy beamline

    NASA Astrophysics Data System (ADS)

    Kang, Tai-Hee; Kim, Ki-jeong; Hwang, C. C.; Rah, S.; Park, C. Y.; Kim, Bongsoo

    2001-07-01

    The performance of a recently commissioned beamline at the Pohang Light Source (PLS) is described. The beamline, which is located at 4B1 at PLS, is a Varied Line Spacing (VLS) Plane Grating Monochromator (PGM) beamline. VLS PGM has become very popular because of the simple scanning mechanism and the fixed exit slit. The beamline which takes 3 mrad horizontal beam fan from bending magnet, covers the energy range 200-1000 eV for Photoemission Electron Microscopy (PEEM), X-ray Photoelectron Spectroscopy (XPS) and Magnetic Circular Dichroism (MCD) experiments. Simplicity of the optics and high flux with medium resolution were the design goals for these applications. The beamline consists of a horizontal focusing mirror, a vertical focusing mirror, VLS plane grating and exit slit. The source of PLS could be used as a virtual entrance slit because of its small size and stability. The flux and the resolution of the beamline at the experimental station have been measured using an ion chamber and a calibrated photodiode. Test images of PEEM from a standard sample were taken to illustrate the further performance of the beamline and PEEM station.

  20. Site-specific intermolecular valence-band dispersion in α-phase crystalline films of cobalt phthalocyanine studied by angle-resolved photoemission spectroscopy

    SciTech Connect

    Yamane, Hiroyuki; Kosugi, Nobuhiro

    2014-12-14

    The valence band structure of α-phase crystalline films of cobalt phthalocyanine (CoPc) grown on Au(111) is investigated by using angle-resolved photoemission spectroscopy (ARPES) with synchrotron radiation. The photo-induced change in the ARPES peaks is noticed in shape and energy of the highest occupied molecular orbital (HOMO, C 2p) and HOMO-1 (Co 3d) of CoPc, and is misleading the interpretation of the electronic properties of CoPc films. From the damage-free normal-emission ARPES measurement, the clear valence-band dispersion has been first observed, showing that orbital-specific behaviors are attributable to the interplay of the intermolecular π-π and π-d interactions. The HOMO band dispersion of 0.1 eV gives the lower limit of the hole mobility for α-CoPc of 28.9 cm{sup 2} V{sup −1} s{sup −1} at 15 K. The non-dispersive character of the split HOMO-1 bands indicates that the localization of the spin state is a possible origin of the antiferromagnetism.

  1. Epitaxial growth of CeO{sub 2}(111) film on Ru(0001): Scanning tunneling microscopy (STM) and x-ray photoemission spectroscopy (XPS) study

    SciTech Connect

    Hasegawa, Tomo; Shahed, Syed Mohammad Fakruddin; Sainoo, Yasuyuki; Beniya, Atsushi; Isomura, Noritake; Watanabe, Yoshihide; Komeda, Tadahiro

    2014-01-28

    We formed an epitaxial film of CeO{sub 2}(111) by sublimating Ce atoms on Ru(0001) surface kept at elevated temperature in an oxygen ambient. X-ray photoemission spectroscopy measurement revealed a decrease of Ce{sup 4+}/Ce{sup 3+} ratio in a small temperature window of the growth temperature between 1070 and 1096 K, which corresponds to the reduction of the CeO{sub 2}(111). Scanning tunneling microscope image showed that a film with a wide terrace and a sharp step edge was obtained when the film was grown at the temperatures close to the reduction temperature, and the terrace width observed on the sample grown at 1060 K was more than twice of that grown at 1040 K. On the surface grown above the reduction temperature, the surface with a wide terrace and a sharp step was confirmed, but small dots were also seen in the terrace part, which are considerably Ce atoms adsorbed at the oxygen vacancies on the reduced surface. This experiment demonstrated that it is required to use the substrate temperature close to the reduction temperature to obtain CeO{sub 2}(111) with wide terrace width and sharp step edges.

  2. Epitaxial growth of CeO2(111) film on Ru(0001): Scanning tunneling microscopy (STM) and x-ray photoemission spectroscopy (XPS) study

    NASA Astrophysics Data System (ADS)

    Hasegawa, Tomo; Shahed, Syed Mohammad Fakruddin; Sainoo, Yasuyuki; Beniya, Atsushi; Isomura, Noritake; Watanabe, Yoshihide; Komeda, Tadahiro

    2014-01-01

    We formed an epitaxial film of CeO2(111) by sublimating Ce atoms on Ru(0001) surface kept at elevated temperature in an oxygen ambient. X-ray photoemission spectroscopy measurement revealed a decrease of Ce4+/Ce3+ ratio in a small temperature window of the growth temperature between 1070 and 1096 K, which corresponds to the reduction of the CeO2(111). Scanning tunneling microscope image showed that a film with a wide terrace and a sharp step edge was obtained when the film was grown at the temperatures close to the reduction temperature, and the terrace width observed on the sample grown at 1060 K was more than twice of that grown at 1040 K. On the surface grown above the reduction temperature, the surface with a wide terrace and a sharp step was confirmed, but small dots were also seen in the terrace part, which are considerably Ce atoms adsorbed at the oxygen vacancies on the reduced surface. This experiment demonstrated that it is required to use the substrate temperature close to the reduction temperature to obtain CeO2(111) with wide terrace width and sharp step edges.

  3. A review of electron-phonon coupling seen in the high-Tc superconductors by angle-resolved photoemission studies (ARPES)

    NASA Astrophysics Data System (ADS)

    Cuk, T.; Lu, D. H.; Zhou, X. J.; Shen, Z.-X.; Devereaux, T. P.; Nagaosa, N.

    2005-01-01

    This issue of pss (b) - basic solid state physics contains a collection of Review Articles on the rather controversially discussed topic of Electron-Phonon Interaction in High-Temperature Superconductors, guest-edited by Miodrag Kuli, Johann Wolfgang Goethe-Universität Frankfurt/Main, Germany, with a Preface written by V. L. Ginzburg and E. G. Maksimov [1].The cover picture, taken from the review [2] by T. Cuk et al., shows plots of the electron-phonon coupling vertex, g2(k, k), where k, k are the initial and final electron momentum for electrons scattered by the bond-buckling phonon B1g (the out-of-phase vibration of the in-plane oxygen) in a tight-binding model of the copper-oxygen plane. The momentum dependence of this vertex, along with the d-wave superconducting gap and the van Hove singularity at the anti-node, accounts for the momentum dependence of the collective mode coupling seen in angle-resolved photoemission data on Bi2212.The present issue also sees the start of our rapid research letters, the fastest peer-reviewed publication medium in solid state physics. For more information see www.pss-rapid.com and the Editorial by the Editor-in-Chief Martin Stutzmann on page 7 [3].

  4. Interface properties of magnetic tunnel junction La0.7Sr0.3MnO3/SrTiO3 superlattices studied by standing-wave excited photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Gray, A. X.; Papp, C.; Balke, B.; Yang, S.-H.; Huijben, M.; Rotenberg, E.; Bostwick, A.; Ueda, S.; Yamashita, Y.; Kobayashi, K.; Gullikson, E. M.; Kortright, J. B.; de Groot, F. M. F.; Rijnders, G.; Blank, D. H. A.; Ramesh, R.; Fadley, C. S.

    2010-11-01

    The chemical and electronic-structure profiles of magnetic tunnel junction (MTJ) La0.7Sr0.3MnO3/SrTiO3 (LSMO/STO) superlattices have been quantitatively determined via soft and hard x-ray standing-wave excited photoemission, x-ray absorption and x-ray reflectivity, in conjunction with x-ray optical and core-hole multiplet theoretical modeling. Epitaxial superlattice samples consisting of 48 and 120 bilayers of LSMO and STO, each nominally four unit cells thick, and still exhibiting LSMO ferromagnetism, were studied. By varying the incidence angle around the superlattice Bragg condition, the standing wave was moved vertically through the interfaces. By comparing experiment to x-ray optical calculations, the detailed chemical profile of the superlattice and its interfaces was quantitatively derived with angstrom precision. The multilayers were found to have a small ˜6% change in periodicity from top to bottom. Interface compositional mixing or roughness over ˜6Å was also found, as well as a significant change in the soft x-ray optical coefficients of LSMO near the interface. The soft x-ray photoemission data exhibit a shift in the position of the Mn3p peak near the interface, which is not observed for Mn3s . Combined with core-hole multiplet theory incorporating Jahn-Teller distortion, these results indicate a change in the Mn bonding state near the LSMO/STO interface. Our results thus further clarify the reduced (MTJ) performance of LSMO/STO compared to ideal theoretical expectations.

  5. The effect of core level crossing on the high-pressure equation of state of osmium

    NASA Astrophysics Data System (ADS)

    Wills, John

    2015-03-01

    The equation of state of the 5d transition metal osmium has been studied with a combination of experiment and theory at pressures up to 500 GPa. The experimental results show a c/a ratio increasing by approximately 1 percent over this pressure range and displaying anomalies at pressures near 180 GPa and near 400 GPa. We have use all-electron fully relativistic density functional theory (DFT) calculations to study the cold equation of state and structural parameters of osmium at pressures up to 500 GPa, using one LDA and two GGA functionals. The increase in the c/a ratio agrees well with experiment, and we find anomalies, although less extreme, near the experimentally observed pressures. We find that the high pressure anomaly coincides with the crossing and hybridization of the 4f(7/2) and 5p(3/2) semi-core levels. In this talk we discuss the theoretical results and methodology and the possible implication for the equations of state of the 5d transition and actinide metals.

  6. Femtomagnetism in graphene induced by core level excitation of organic adsorbates

    PubMed Central

    Ravikumar, Abhilash; Baby, Anu; Lin, He; Brivio, Gian Paolo; Fratesi, Guido

    2016-01-01

    We predict the induction or suppression of magnetism in the valence shell of physisorbed and chemisorbed organic molecules on graphene occurring on the femtosecond time scale as a result of core level excitations. For physisorbed molecules, where the interaction with graphene is dominated by van der Waals forces and the system is non-magnetic in the ground state, numerical simulations based on density functional theory show that the valence electrons relax towards a spin polarized configuration upon excitation of a core-level electron. The magnetism depends on efficient electron transfer from graphene on the femtosecond time scale. On the other hand, when graphene is covalently functionalized, the system is magnetic in the ground state showing two spin dependent mid gap states localized around the adsorption site. At variance with the physisorbed case upon core-level excitation, the LUMO of the molecule and the mid gap states of graphene hybridize and the relaxed valence shell is not magnetic anymore. PMID:27089847

  7. High resolution core level spectroscopy of hydrogen-terminated (1 0 0) diamond

    NASA Astrophysics Data System (ADS)

    Schenk, A. K.; Rietwyk, K. J.; Tadich, A.; Stacey, A.; Ley, L.; Pakes, C. I.

    2016-08-01

    Synchrotron-based photoelectron spectroscopy experiments are presented that address a long standing inconsistency in the treatment of the C1s core level of hydrogen terminated (1 0 0) diamond. Through a comparison of surface and bulk sensitive measurements we show that there is a surface related core level component to lower binding energy of the bulk diamond component; this component has a chemical shift of -0.16+/- 0.05 eV which has been attributed to carbon atoms which are part of the hydrogen termination. Additionally, our results indicate that the asymmetry of the hydrogen terminated (1 0 0) diamond C1s core level is an intrinsic aspect of the bulk diamond peak which we have attributed to sub-surface carbon layers.

  8. Pressure-induced crossing of the core levels in 5 d metals

    NASA Astrophysics Data System (ADS)

    Tal, Alexey A.; Katsnelson, Mikhail I.; Ekholm, Marcus; Jönsson, H. Johan M.; Dubrovinsky, Leonid; Dubrovinskaia, Natalia; Abrikosov, Igor A.

    2016-05-01

    A pressure-induced interaction between core electrons, the core-level crossing (CLC) transition, has been observed in hcp Os at P ≈400 GPa [L. Dubrovinsky et al., Nature (London) 525, 226 (2015)], 10.1038/nature14681. By carrying out a systematic theoretical study for all metals of the 5 d series (Hf, Ta, W, Re, Os, Ir, Pt, Au) we have found that the CLC transition is a general effect for this series of metals. While in Pt it occurs at ≈1500 GPa , at a pressure substantially higher than in Os, in Ir it occurs already at 80 GPa. Moreover, we predict that in Re the CLC transition may take place already at ambient pressure. We explain the effect of the CLC and analyze the shift of the transition pressure across the series within the Thomas-Fermi model. In particular, we show that the effect has many common features with the atomic collapse in rare-earth elements.

  9. Atomic signatures of local environment from core-level spectroscopy in β -Ga2O3

    NASA Astrophysics Data System (ADS)

    Cocchi, Caterina; Zschiesche, Hannes; Nabok, Dmitrii; Mogilatenko, Anna; Albrecht, Martin; Galazka, Zbigniew; Kirmse, Holm; Draxl, Claudia; Koch, Christoph T.

    2016-08-01

    We present a joint theoretical and experimental study on core-level excitations from the oxygen K edge of β -Ga2O3 . A detailed analysis of the electronic structure reveals the importance of O-Ga hybridization effects in the conduction region. The spectrum from O 1 s core electrons is dominated by excitonic effects, which overall redshift the absorption onset by 0.5 eV, and significantly redistribute the intensity to lower energies. Analysis of the spectra obtained within many-body perturbation theory reveals atomic fingerprints of the inequivalent O atoms. From the comparison of energy-loss near-edge fine-structure (ELNES) spectra computed with respect to different crystal planes, with measurements recorded under the corresponding diffraction conditions, we show how the spectral contributions of specific O atoms can be enhanced while quenching others. These results suggest ELNES, combined with ab initio many-body theory, as a very powerful technique to characterize complex systems, with sensitivity to individual atomic species and to their local environment.

  10. Photoemission Experiments for Charge Characteristics of Individual Dust Grains

    NASA Technical Reports Server (NTRS)

    Abbas, M. M.; Craven, P. D.; Spann, J. F.; West, E.; Pratico, J.; Tankosic, D.; Venturini, C. C.; Six, N. Frank (Technical Monitor)

    2001-01-01

    Photoemission experiments with UV radiation have been performed to investigate the microphysics and charge characteristics of individual isolated dust grains of various compositions and sizes by using the electrodynamic balance facility at NASA Marshall Space Flight Center. Dust particles of 2-10 gm diameter are levitated in a vacuum chamber at pressures approximately 10(exp-5) torr and exposed to a collimated beam of UV radiation in the 120-200 nm spectral range from a deuterium lamp source with a MgF2 window. A monochromator is used to select the UV wavelength with a spectral resolution of 8 nm. The electrodynamic facility permits measurements of the charge and diameters of particles of known composition, and monitoring of photoemission rates with the incident UV radiation. Experiments have been conducted on test particles of silica and polystyrene to determine the photoelectric yields and surface equilibrium potentials when exposed to UV radiation. A brief description of an experimental procedure for photoemission studies is given and some preliminary laboratory measurements of the photoelectric yields of individual dust particles are presented.

  11. Bulk sensitive hard x-ray photoemission electron microscopy

    SciTech Connect

    Patt, M. Wiemann, C.; Weber, N.; Escher, M.; Merkel, M.; Gloskovskii, A.; Drube, W.; Schneider, C. M.

    2014-11-15

    Hard x-ray photoelectron spectroscopy (HAXPES) has now matured into a well-established technique as a bulk sensitive probe of the electronic structure due to the larger escape depth of the highly energetic electrons. In order to enable HAXPES studies with high lateral resolution, we have set up a dedicated energy-filtered hard x-ray photoemission electron microscope (HAXPEEM) working with electron kinetic energies up to 10 keV. It is based on the NanoESCA design and also preserves the performance of the instrument in the low and medium energy range. In this way, spectromicroscopy can be performed from threshold to hard x-ray photoemission. The high potential of the HAXPEEM approach for the investigation of buried layers and structures has been shown already on a layered and structured SrTiO{sub 3} sample. Here, we present results of experiments with test structures to elaborate the imaging and spectroscopic performance of the instrument and show the capabilities of the method to image bulk properties. Additionally, we introduce a method to determine the effective attenuation length of photoelectrons in a direct photoemission experiment.

  12. Surface effects on core-level binding energies and valence in thulium chalcogenides

    NASA Astrophysics Data System (ADS)

    Kaindl, G.; Laubschat, C.; Reihl, B.; Pollak, R. A.; Mårtensson, N.; Holtzberg, F.; Eastman, D. E.

    1982-08-01

    Vacuum-cleaved (100) surfaces of mixed-valent TmSe, divalent TmTe, and trivalent TmS were studied by high-resolution, angle-integrated photoelectron spectroscopy with the use of synchrotron radiation in the energy range 30<=hν<=110 eV. In the topmost surface layers of TmSe and TmTe the 4f levels are found to be shifted to higher binding energies by 0.32+/-0.04 and 0.41+/-0.05 eV, respectively. In both TmSe and TmS the topmost surface layers are divalent. In the case of TmSe a separation of the Tm2+ 4f12 spectral feature into surface and bulk contributions allows a determination of the bulk mean valence v¯=2.55+/-0.05. While a shift of the Se 3d levels to lower binding energy is observed for Se atoms in the topmost surface layer of TmSe, no such shift can be resolved for the Te 4d levels of TmTe. The surface-derived divalent spectral features can be quenched completely in all three cases by exposure of the surfaces to submonolayer amounts of oxygen, resulting in the formation of trivalent surface oxides. Values for the electron mean free path l are derived from the observed surface- and bulk-spectral intensities, with l decreasing with decreasing electron kinetic energy down to ≅45 eV. Smaller singularity indices α of the Doniach-Sunjić line shapes as well as smaller extrinsic losses are observed for photoemission from the divalent surface layers as compared to the bulk.

  13. Theory of hot electron photoemission from graphene

    NASA Astrophysics Data System (ADS)

    Ang, Lay Kee; Liang, Shijun

    Motivated by the development of Schottky-type photodetectors, some theories have been proposed to describe how the hot carriers generated by the incident photon are transported over the Schottky barrier through the internal photoelectric effect. One of them is Fowler's law proposed as early as 1931, which studied the temperature dependence of photoelectric curves of clean metals. This law is very successful in accounting for mechanism of detecting photons of energy lower than the band gap of semiconductor based on conventional metal/semiconductor Schottky diode. With the goal of achieving better performance, graphene/silicon contact-based- graphene/WSe2 heterostructure-based photodetectors have been fabricated to demonstrate superior photodetection efficiency. However, the theory of how hot electrons is photo-excited from graphene into semiconductor remains unknown. In the current work, we first examine the photoemission process from suspended graphene and it is found that traditional Einstein photoelectric effect may break down for suspended graphene due to the unique linear band structure. Furthermore, we find that the same conclusion applies for 3D graphene analog (e.g. 3D topological Dirac semi-metal). These findings are very useful to further improve the performance of graphene-based photodetector, hot-carrier solar cell and other kinds of sensor.

  14. Modeling Shallow Core-Level Transitions in the Reflectance Spectra of Gallium-Containing Semiconductors

    NASA Astrophysics Data System (ADS)

    Stoute, Nicholas; Aspnes, David

    2012-02-01

    The electronic structure of covalent materials is typically approached by band theory. However, shallow core level transitions may be better modeled by an atomic-scale approach. We investigate shallow d-core level reflectance spectra in terms of a local atomic-multiplet theory, a novel application of a theory typically used for higher-energy transitions on more ionic type material systems. We examine specifically structure in reflectance spectra of GaP, GaAs, GaSb, GaSe, and GaAs1-xPx due to transitions that originate from Ga3d core levels and occur in the 20 to 25 eV range. We model these spectra as a Ga^+3 closed-shell ion whose transitions are influenced by perturbations on 3d hole-4p electron final states. These are specifically spin-orbit effects on the hole and electron, and a crystal-field effect on the hole, attributed to surrounding bond charges and positive ligand anions. Empirical radial-strength parameters were obtained by least-squares fitting. General trends with respect to anion electronegativity are consistent with expectations. In addition to the spin-orbit interaction, crystal-field effects play a significant role in breaking the degeneracy of the d levels, and consequently are necessary to understand shallow 3d core level spectra.

  15. Understanding electronegative effects in core-level electron spectroscopies; application to the high temperature superconductors

    NASA Astrophysics Data System (ADS)

    Ramaker, David E.

    1989-12-01

    The nature of the core level reflected in x ray photoelectron spectroscopy, Auger electron spectrosocopy, and x ray absorption near edge structure is considered. An understanding of the effects of anion and cation electronegativity on spectra for the transition metal halides is obtained. This knowledge is applied to understand similar spectra for the high temperature superconductors.

  16. A New Spin on Photoemission Spectroscopy

    SciTech Connect

    Jozwiak, Chris

    2008-12-01

    The electronic spin degree of freedom is of general fundamental importance to all matter. Understanding its complex roles and behavior in the solid state, particularly in highly correlated and magnetic materials, has grown increasingly desirable as technology demands advanced devices and materials based on ever stricter comprehension and control of the electron spin. However, direct and efficient spin dependent probes of electronic structure are currently lacking. Angle Resolved Photoemission Spectroscopy (ARPES) has become one of the most successful experimental tools for elucidating solid state electronic structures, bolstered by-continual breakthroughs in efficient instrumentation. In contrast, spin-resolved photoemission spectroscopy has lagged behind due to a lack of similar instrumental advances. The power of photoemission spectroscopy and the pertinence of electronic spin in the current research climate combine to make breakthroughs in Spin and Angle Resolved Photoemission Spectroscopy (SARPES) a high priority . This thesis details the development of a unique instrument for efficient SARPES and represents a radical departure from conventional methods. A custom designed spin polarimeter based on low energy exchange scattering is developed, with projected efficiency gains of two orders of magnitude over current state-of-the-art polarimeters. For energy analysis, the popular hemispherical analyzer is eschewed for a custom Time-of-Flight (TOF) analyzer offering an additional order of magnitude gain in efficiency. The combined instrument signifies the breakthrough needed to perform the high resolution SARPES experiments necessary for untangling the complex spin-dependent electronic structures central to today's condensed matter physics.

  17. Comparative angle-resolved photoemission spectroscopy study of CaRuO3 and SrRuO3 thin films: Pronounced spectral weight transfer and possible precursor of lower Hubbard band

    NASA Astrophysics Data System (ADS)

    Yang, H. F.; Fan, C. C.; Liu, Z. T.; Yao, Q.; Li, M. Y.; Liu, J. S.; Jiang, M. H.; Shen, D. W.

    2016-09-01

    In the prototypical 4 d system (Sr ,Ca ) RuO3 , the degree and origin of electron correlations, and how they correlate with physical properties, still remain elusive, though extensive studies have been performed. In this work we present a comparative electronic structure study of high-quality epitaxial CaRuO3 and SrRuO3 thin films, by means of reactive molecular beam epitaxy and in situ angle-resolved photoemission spectroscopy. We found that while SrRuO3 possesses sharp features signaling the Fermi liquid state, the isostructural CaRuO3 exhibits broad features and its spectral weight is markedly transferred from the Fermi level to -1.2 eV forming a "hump" structure which resembles the Mott-Hubbard system (Sr ,Ca ) VO3 . We suggest that this hump is the precursor of the lower Hubbard band, and the U /W (U and W represent the on-site Coulomb interactions and bandwidth, respectively) of our CaRuO3 thin film is much larger than that of SrRuO3. In addition, we discuss the origin of electron correlations as well as the ferromagnetism in SrRuO3 which is absent in CaRuO3. Our findings put constraints on future studies, and also show that perovskite ruthenates are indeed an experimentally tunable system for the study of electron correlations.

  18. An x-ray photoemission electron microscopy study of the formation of Ti-Al phases in 4 mol% TiCl3 catalyzed NaAlH4 during high energy ball milling.

    PubMed

    Dobbins, Tabbetha; Abrecht, Mike; Uprety, Youaraj; Moore, Kristan

    2009-05-20

    This study reports reaction pathways to form TiAlx metallic complexes during the high energy ball milling of 4 mol% TiCl3 with NaAlH4 powders determined using local structure analysis of Tix+ and Alx+ species. Using x-ray photoemission electron microscopy (XPEEM) and x-ray diffraction (XRD), the oxidation state of Alx+ and Tix+ and the crystalline compounds existing in equilibrium with NaAlH4 were tracked for samples milled for times of 0 (i.e. mixing), 5, and 25 min. XPEEM analysis of the Al K edge after 5 min of milling reveals that Al remains in the 3+ oxidation state (i.e. in NaAlH4) around Ti0-rich regions of the sample. After 25 min of high energy milling, Ti0 has reacted with Al3+ (in nearby NaAlH4) to form TiAlx complexes. This study reports the pathway for TiAlx complex formation during milling of 4 mol% TiCl3catalyzed NaAlH4 to be as follows: (1) Ti3+ reduces to Ti0 (with Al3+ near Ti0 regions) and (2) Ti0 reacts with Al3+ in NaAlH4 to form TiAlx complexes.

  19. An x-ray photoemission electron microscopy study of the formation of Ti-Al phases in 4 mol% TiCl3 catalyzed NaAlH4 during high energy ball milling

    NASA Astrophysics Data System (ADS)

    Dobbins, Tabbetha; Abrecht, Mike; Uprety, Youaraj; Moore, Kristan

    2009-05-01

    This study reports reaction pathways to form TiAlx metallic complexes during the high energy ball milling of 4 mol% TiCl3 with NaAlH4 powders determined using local structure analysis of Tix+ and Alx+ species. Using x-ray photoemission electron microscopy (XPEEM) and x-ray diffraction (XRD), the oxidation state of Alx+ and Tix+ and the crystalline compounds existing in equilibrium with NaAlH4 were tracked for samples milled for times of 0 (i.e. mixing), 5, and 25 min. XPEEM analysis of the Al K edge after 5 min of milling reveals that Al remains in the 3+ oxidation state (i.e. in NaAlH4) around Ti0-rich regions of the sample. After 25 min of high energy milling, Ti0 has reacted with Al3+ (in nearby NaAlH4) to form TiAlx complexes. This study reports the pathway for TiAlx complex formation during milling of 4 mol% TiCl3 catalyzed NaAlH4 to be as follows: (1) Ti3+ reduces to Ti0 (with Al3+ near Ti0 regions) and (2) Ti0 reacts with Al3+ in NaAlH4 to form TiAlx complexes.

  20. Tetrapeptide unfolding dynamics followed by core-level spectroscopy: a first-principles approach.

    PubMed

    Taioli, Simone; Simonucci, Stefano; A Beccara, Silvio; Garavelli, Marco

    2015-05-01

    In this work we demonstrate that core level analysis is a powerful tool for disentangling the dynamics of a model polypeptide undergoing conformational changes in solution and disulphide bond formation. In particular, we present computer simulations within both initial and final state approximations of 1s sulphur core level shifts (S1s CLS) of the CYFC (cysteine-phenylalanine-tyrosine-cysteine) tetrapeptide for different folding configurations. Using increasing levels of accuracy, from Hartree-Fock and density functional theory to configuration interaction via a multiscale algorithm capable of reducing drastically the computational cost of electronic structure calculations, we find that distinct peptide arrangements present S1s CLS sizeably different (in excess of 0.5 eV) with respect to the reference disulfide bridge state. This approach, leading to experimentally detectable signals, may represent an alternative to other established spectroscopic techniques.

  1. Time dependence of FEL-induced surface photovoltage on semiconductor interfaces measured with synchroton radiation photoemission spectroscopy

    SciTech Connect

    Marsi, M.; Delboulbe, A.; Garzella, D.

    1995-12-31

    During the last year, the first surface science experiments simultaneously using a Free Electron Laser (FEL) and Synchrotron Radiation (SR) have been performed on SuperACO at LURE (Orsay, France). These {open_quotes}two color{close_quotes} experiments studied the surface photovoltage (SPV) induced on semiconductor surfaces and interfaces by the SuperACO FEL, a storage ring FEL delivering 350 nm photons which am naturally synchronized with the SR; the SPV was measured by synchrotron radiation core-level photoemission spectroscopy on the high-resolution SU3 undulator beamline. We will describe the experimental setup, which allowed us to convey the FEL light onto the samples sitting in the SU3 experimental station by means of a series of mirrors, and show the results we obtained for prototypical systems such as Ag/GaAs(110) and Si(111) 2 x 1. The dependence of the SPV was studied in function of various parameters, changing sample doping and photon flux; but our efforts were mainly devoted to studying its dependence on the time delay between the FEL pump and the SR probe. On SuperACO, such delay can be varied between 1 and 120 ns, the limits being given by the time duration of a SR pulse and by the interval between two consecutive positron bunches, respectively. The results show a clear temporal dependence of the amount of SPV on cleaved Si surfaces, where as the Ag/GaAs(110) does not show any difference on the ns time scale. We will discuss these results in terms of the role of surface recombination in the dynamics of the photoinduced electron-hole pairs. These studies follow the evolution of the density of electrostatic charge at surfaces and interfaces on a nanosecond time scale, and might pave the way for a new series of experiments: for example, one might explore what are the physical mechanisms limiting the time response of Schottky diodes.

  2. orbital selective correlation reduce in collapse tetragonal phase of CaFe2(As0.935P0.065)2 and electronic structure reconstruction studied by angel resolved photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Zeng, Lingkun

    We performed an angle-resolved photoemission spectroscopy (ARPES) study of the CaFe2(As0.935P0.065)2 in the collapse tetragonal(CT) phase and uncollapse tetragonal(UCT) phase. We find in the CT phase the electronic correlation dramatically reduces respective to UCT phase. Meanwhile, the reduction of correlation in CT phase show an orbital selective effect: correlation in dxy reduces the most, and then dxz/yz, while the one in dz2-r2 almost keeps the same. In CT phase, almost all bands sink downwards to higher binding energy, leading to the hole like bands around Brillouin zone(BZ) center sink below EF compared with UCT phase. However, the electron pocket around Brillouin Zone(BZ) corner(M) in UCT phase, forms a hole pocket around BZ center(Z point) in CT phase. Moreover, the dxy exhibits larger movement down to higher binding energy, resulting in farther away from dyz/xz and closer to dxy.We propose the electron filling ,namely high spin state in UCT phase to low spin state in CT phase(due to competing between crystal structure field and Hund's coupling), other than the Fermi surface nesting might be responsible for the absent of magnetic ordering.

  3. Photoemission study of LaAl O3 /SrTi O3 and LaAl O3 /Nb :SrTi O3 : Insulator-insulator versus insulator-semiconductor interfaces

    NASA Astrophysics Data System (ADS)

    Susaki, Tomofumi; Ueda, Shigenori; Matsuzaki, Kosuke; Kobayashi, Toshihiro; Toda, Yoshitake; Hosono, Hideo

    2016-08-01

    By hard x-ray photoemission spectroscopy we have studied the electronic states of LaAl O3 /SrTi O3 (100) and LaAlO3/Nb : SrTiO3(100) heterostructures, where the polar LaAl O3 layer is grown on the insulating and conducting substrates, respectively. The analysis of the valence band has shown that the electron affinity is as small as +0.4 eV in both the LaAl O3 /SrTi O3 and LaAl O3 /Nb :SrTi O3 heterostructures. The interface is "staggered type" (type II) in both of the heterostructures with the valence band maximum of LaAl O3 above the valence band maximum of SrTi O3 . The valence band offset of 0.42 eV in the LaAl O3 /SrTi O3 heterostructure has increased to 0.61 eV in the LaAl O3 /Nb :SrTi O3 as the LaAl O3 component shifts towards the lower binding energy side. The electronic states of LaAl O3 and SrTi O3 have been merged with each other in the lower energy part of the valence band of the LaAl O3 /Nb :SrTi O3 heterostructures.

  4. Electronic structure of Li{sub 1+x}[Mn{sub 0.5}Ni{sub 0.5}]{sub 1−x}O{sub 2} studied by photoemission and x-ray absorption spectroscopy

    SciTech Connect

    Yokoyama, Y.; Ootsuki, D.; Sugimoto, T.; Wadati, H.; Okabayashi, J.; Yang, Xu; Du, Fei; Chen, Gang; Mizokawa, T.

    2015-07-20

    We have studied the electronic structure of Li{sub 1+x}[Mn{sub 0.5}Ni{sub 0.5}]{sub 1−x}O{sub 2} (x = 0.00 and 0.05), one of the promising cathode materials for Li ion battery, by means of x-ray photoemission and absorption spectroscopy. The results show that the valences of Mn and Ni are basically 4+ and 2+, respectively. However, the Mn{sup 3+} component in the x = 0.00 sample gradually increases with the bulk sensitivity of the experiment, indicating that the Jahn-Teller active Mn{sup 3+} ions are introduced in the bulk due to the site exchange between Li and Ni. The Mn{sup 3+} component gets negligibly small in the x = 0.05 sample, which indicates that the excess Li suppresses the site exchange and removes the Jahn-Teller active Mn{sup 3+}.

  5. Surface and bulk 4f-photoemission spectra of CeIn{sub 3} and CeSn{sub 3}

    SciTech Connect

    Kim, H.; Tjernberg, O.; Chiaia, G.; Kumigashira, H.; Takahashi, T.; Duo, L.; Sakai, O.; Kasaya, M.; Lindau, I.

    1997-07-01

    Resonant photoemission spectroscopy was performed on CeIn{sub 3} and CeSn{sub 3} at the 4d-4f and 3d-4f core thresholds. Using the different surface sensitivity between the two photon energies, surface and bulk 4f-photoemission spectra were derived for both compounds. With the noncrossing approximation of the Anderson impurity model, the 4d-4f resonant spectra together with the surface and bulk spectra were self-consistently analyzed to obtain the microscopic parameters such as the 4f-electron energy and the hybridization strength with conduction electrons. The result shows a substantial difference in these parameters between the surface and the bulk, indicating that it is important to take into account the surface effect in analyzing photoemission spectra of Ce compounds. It is also found that the 4f surface core-level shift is different between CeIn{sub 3} and CeSn{sub 3}. {copyright} {ital 1997} {ital The American Physical Society}

  6. Layer-resolved photoemission tomography: The p -sexiphenyl bilayer upon Cs doping

    NASA Astrophysics Data System (ADS)

    Reinisch, E. M.; Puschnig, P.; Ules, T.; Ramsey, M. G.; Koller, G.

    2016-04-01

    The buried interface between a molecular thin film and the metal substrate is generally not accessible to the photoemission experiment. With the example of a sexiphenyl (6 P ) bilayer on Cu we show that photoemission tomography can be used to study the electronic level alignment and geometric structure, where it was possible to assign the observed orbital emissions to the individual layers. We further study the Cs doping of this bilayer. Initial Cs exposure leads to a doping of only the first interface layer, leaving the second layer unaffected except for a large energy shift. This result shows that it is in principle possible to chemically modify just the interface, which is important to issues like tuning of the energy level alignment and charge transfer to the interface layer. Upon saturating the film with Cs, photoemission tomography shows a complete doping (6 p4 - ) of the bilayer, with the molecular geometry changing such that the spectra become dominated by σ -orbital emissions.

  7. Simple theoretical analysis of the Einstein’s photoemission from quantum confined superlattices

    NASA Astrophysics Data System (ADS)

    Pahari, S.; Bhattacharya, S.; Roy, S.; Saha, A.; De, D.; Ghatak, K. P.

    2009-11-01

    In this paper, we study the Einstein's photoemission from III-V, II-VI, IV-VI and HgTe/CdTe quantum well superlattices (QWSLs) with graded interfaces and quantum well effective mass superlattices in the presence of a quantizing magnetic field on the basis of newly formulated dispersion relations in the respective cases. Besides, the same has been studied from the afore-mentioned quantum dot superlattices and it appears that the photoemission oscillates with increasing carrier degeneracy and quantizing magnetic field in different manners. In addition, the photoemission oscillates with film thickness and increasing photon energy in quantum steps together with the fact that the solution of the Boltzmann transport equation will introduce new physical ideas and new experimental findings under different external conditions. The influence of band structure is apparent from all the figures and we have suggested three applications of the analyses of this paper in the fields of superlattices and microstructures.

  8. Core-level binding-energy shifts for the metallic elements

    NASA Astrophysics Data System (ADS)

    Johansson, Börje; Mårtensson, Nils

    1980-05-01

    A general treatment of core-level binding-energy shifts in metals relative to the free atom is introduced and applied to all elemental metals in the Periodic Table. The crucial ingredients of the theoretical description are (a) the assumption of a fully screened final state in the metallic case and (b) the (Z+1) approximation for the screening valence charge distribution around the core-ionized site. This core-ionized site is, furthermore, treated as an impurity in an otherwise perfect metal. The combination of the complete screening picture and the (Z+1) approximation makes it possible to introduce a Born-Haber cycle which connects the initial state with the final state of the core-ionization process. From this cycle it becomes evident that the main contributions to the core-level shift are the cohesive energy difference between the (Z+1) and Z metal and an appropriate ionization energy of the (Z+1) atom (usually the first ionization potential). The appearance of the ionization potential in the shift originates from the assumption of a charge-neutral final state, while the contribution from the cohesive energies essentially describes the change of bonding properties between the initial and final state of the site. The calculated shifts show very good agreement with available experimental values (at present, for 19 elements). For the other elements we have made an effort to combine experimental ionization potentials with theoretical calculations in order to obtain accurate estimates of some of the atomic-core-level binding energies. Such energies together with measured metallic binding energies give "pseudoexperimental" shifts for many elements. Our calculated core-level shifts agree exceedingly well also with these data. For some of the transition elements the core-level shift shows a deviating behavior in comparison with that of neighboring elements. This is shown to be due to a difference in the atomic ground-state configuration, such as, for example, d5s in

  9. Raising Photoemission Efficiency with Surface Acoustic Waves

    SciTech Connect

    A. Afanasev, F. Hassani, C.E. Korman, V.G. Dudnikov, R.P. Johnson, M. Poelker, K.E.L. Surles-Law

    2012-07-01

    We are developing a novel technique that may help increase the efficiency and reduce costs of photoelectron sources used at electron accelerators. The technique is based on the use of Surface Acoustic Waves (SAW) in piezoelectric materials, such as GaAs, that are commonly used as photocathodes. Piezoelectric fields produced by the traveling SAW spatially separate electrons and holes, reducing their probability of recombination, thereby enhancing the photoemission quantum efficiency of the photocathode. Additional advantages could be increased polarization provided by the enhanced mobility of charge carriers that can be controlled by the SAW and the ionization of optically-generated excitons resulting in the creation of additional electron-hole pairs. It is expected that these novel features will reduce the cost of accelerator operation. A theoretical model for photoemission in the presence of SAW has been developed, and experimental tests of the technique are underway.

  10. X-ray photoemission and energy dispersive spectroscopy of hydroxyapatite-coated titanium

    SciTech Connect

    Drummond, J.L.; Steinberg, A.D.; Krauss, A.R.

    1997-07-01

    The purpose of this study was to determine the chemical composition changes of hydroxyapatite (HA) coated titanium using surface analysis (X-ray photoemission) and bulk analysis (energy dispersive spectroscopy). The specimens examined were controls and specimens aged 30 min and 3 h at room temperature in distilled water and 0.2M sodium phosphate buffer (pH 7.2). Each X-ray photoemission cycle consisted of three scans followed by argon sputtering for 10 min for usually 20 cycles, corresponding to a sampling depth of {approximately}1,500 {angstrom}. The energy dispersive spectroscopy analysis was on a 110 by 90 {micro}m area for 500 s. The X-ray photoemission results indicated the oxidation effect of water on the titanium (as TiO{sub 2}) and the effect of the buffer to increase the surface concentration of phosphorus. No differences in the chemical composition were observed by energy dispersive spectroscopy analysis.

  11. X-ray photoemission spectroscopy of nonmetallic materials: Electronic structures of boron and BxOy

    NASA Astrophysics Data System (ADS)

    Ong, C. W.; Huang, H.; Zheng, B.; Kwok, R. W. M.; Hui, Y. Y.; Lau, W. M.

    2004-04-01

    Although an increasing volume of x-ray photoemission spectroscopic (XPS) data has been accumulated on boron and boron-rich compounds because of their unusual properties, including a unique three-center, two-electron bonding configuration, their common nonmetallic nature has been overlooked. Typically, the measured energy-state data are not clarified by surface Fermi level positions of these nonmetallic samples, which compromises the scientific contents of the data. In the present study, we revisited the XPS studies of sputter-cleaned β-rhombohedral boron (βr-B), the oxidized surface of βr-B, B6O pellet, and polished B2O3, to illustrate the impact and resolution of this scientific issue. These samples were chosen because βr-B is the most thermodynamically stable polytype of pure boron, B2O3 is its fully oxidized form, and B6O is the best known superhard family member of boron-rich compounds. From our XPS measurements, including those from a sputter-cleaned gold as a metal reference, we deduced that our βr-B had a surface Fermi level located at 0.7±0.1 eV from its valence-band maximum (VBM) (referred as EFL) and a binding energy for its B 1s core level at 187.2 eV from VBM (Eb,VBM). The latter attribute, unlike typical XPS binding energy data that are referenced to a sample-dependent Fermi level (Eb,FL), is immune from any uncertainties and variations arising from sample doping and surface charging. For bulk B2O3, we found an Eb,VBM for its B 1s core level at 190.5 eV and an Eb,FL at 193.6 eV. For our βr-B subjected to a surface oxidation treatment, an overlayer structure of ˜1.2 nm B2O3/˜2 nm B2O/B was found. By comparing the data from this sample and those from βr-B and bulk B2O3, we infer that the oxide overlayer carried some negative fixed charge and this induced on the semiconducting βr-B sample an upward surface band bending of ˜0.6 eV. As for our B6O sample, we found an EFL of ˜1.7 eV and two different chemical states having Eb,VBM of 185.4 and

  12. Einstein's Photoemission from Quantum Confined Superlattices.

    PubMed

    Debbarma, S; Ghatak, K P

    2016-01-01

    This paper is dedicated to the 83th Birthday of Late Professor B. R. Nag, D.Sc., formerly Head of the Departments of Radio Physics and Electronics and Electronic Science of the University of Calcutta, a firm believer of the concept of theoretical minimum of Landau and an internationally well known semiconductor physicist, to whom the second author remains ever grateful as a student and research worker from 1974-2004. In this paper, an attempt is made to study, the Einstein's photoemission (EP) from III-V, II-VI, IV-VI, HgTe/CdTe and strained layer quantum well heavily doped superlattices (QWHDSLs) with graded interfaces in the presence of quantizing magnetic field on the basis of newly formulated electron dispersion relations within the frame work of k · p formalism. The EP from III-V, II-VI, IV-VI, HgTe/CdTe and strained layer quantum wells of heavily doped effective mass superlattices respectively has been presented under magnetic quantization. Besides the said emissions, from the quantum dots of the aforementioned heavily doped SLs have further investigated for the purpose of comparison and complete investigation in the context of EP from quantum confined superlattices. Using appropriate SLs, it appears that the EP increases with increasing surface electron concentration and decreasing film thickness in spiky manners, which are the characteristic features of such quantized hetero structures. Under magnetic quantization, the EP oscillates with inverse quantizing magnetic field due to Shuvnikov-de Haas effect. The EP increases with increasing photo energy in a step-like manner and the numerical values of EP with all the physical variables are totally band structure dependent for all the cases. The most striking features are that the presence of poles in the dispersion relation of the materials in the absence of band tails create the complex energy spectra in the corresponding HD constituent materials of such quantum confined superlattices and effective electron

  13. Strongly correlated valence electrons and core-level chemical bonding of Lithium at terapascal pressures

    NASA Astrophysics Data System (ADS)

    Hu, Anguang; Zhang, Fan

    2015-03-01

    As the simplest pure metal, lithium exhibits some novel properties on electrical conductivity and crystal structures under high pressure. All-electron density functional theory simulations, recently developed by using the linear combination of localized Slater atomic orbitals, revealed that the bandwidth of its valence bands remains almost unchanged within about 3.5 eV even up to a terapascal pressure range. This indicates that the development from delocalized to strongly correlated electronic systems takes place under compression, resulting in metal-semiconductor and superconductivity transitions together with a sequence of new high-pressure crystal phases, discovered experimentally. In contrast to the valence bands, the core-level bands become broadening up to about 10 eV at terapascal pressures. It means the transformation from chemical non-bonding to bonding for core electrons. Thus, dense lithium under compression can be characterized as core-level chemical bonding and a completely new class of strongly correlated materials with narrow bands filled in s-electron shells only.

  14. Core level excitations—A fingerprint of structural and electronic properties of epitaxial silicene

    SciTech Connect

    Friedlein, R. Fleurence, A.; Aoyagi, K.; Yamada-Takamura, Y.; Jong, M. P. de; Van Bui, H.; Wiggers, F. B.; Yoshimoto, S.; Koitaya, T.; Shimizu, S.; Noritake, H.; Mukai, K.; Yoshinobu, J.

    2014-05-14

    From the analysis of high-resolution Si 2p photoelectron and near-edge x-ray absorption fine structure (NEXAFS) spectra, we show that core level excitations of epitaxial silicene on ZrB{sub 2}(0001) thin films are characteristically different from those of sp{sup 3}-hybridized silicon. In particular, it is revealed that the lower Si 2p binding energies and the low onset in the NEXAFS spectra as well as the occurrence of satellite features in the core level spectra are attributed to the screening by low-energy valence electrons and interband transitions between π bands, respectively. The analysis of observed Si 2p intensities related to chemically distinct Si atoms indicates the presence of at least one previously unidentified component. The presence of this component suggests that the observation of stress-related stripe domains in scanning tunnelling microscopy images is intrinsically linked to the relaxation of Si atoms away from energetically unfavourable positions.

  15. Study of hard disk and slider surfaces using X-ray photoemission electron microscopy and near-edge X-ray absorption fine structure spectroscopy

    SciTech Connect

    Anders, S.; Stammler, T.; Bhatia, C.S.; Fong, W.; Chen, C.Y.; Bogy, D.B.

    1998-04-01

    X-ray Photo Emission Electron Microscopy (X-PEEM) and Near Edge X-ray Absorption Fine Structure (NEXAFS) spectroscopy were applied to study the properties of amorphous hard carbon overcoats on disks and sliders, and the properties of the lubricant. The modification of lubricants after performing thermal desorption studies was measured by NEXAFS, and the results are compared to the thermal desorption data. The study of lubricant degradation in wear tracks is described. Sliders were investigated before and after wear test, and the modification of the slider coating as well as the transfer of lubricant to the slider was studied. The studies show that the lubricant is altered chemically during the wear. Fluorine is removed and carboxyl groups are formed.

  16. Monochromatic electron photoemission from diamondoid monolayers

    SciTech Connect

    Yang, Wanli; Yang, Wanli L.; Fabbri, J.D.; Willey, T.M.; Lee, J.R.I.; Dahl, J.E.; Carlson, R.M.K.; Schreiner, P.R.; Fokin, A.A.; Tkachenko, B.A.; Fokina, N.A.; Meevasana, W.; Mannella, N.; Tanaka, K.; Zhou, X.J.; van Buuren, T.; Kelly, M.A.; Hussain, Z.; Melosh, N.A.; Shen, Z.-X.

    2007-02-27

    We found monochromatic electron photoemission from large-area self-assembled monolayers of a functionalized diamondoid, [121]tetramantane-6-thiol. Photoelectron spectra of the diamondoid monolayers exhibited a peak at the low-kinetic energy threshold; up to 68percent of all emitted electrons were emitted within this single energy peak. The intensity of the emission peak is indicative of diamondoids being negative electron affinity materials. With an energy distribution width of less than 0.5 electron volts, this source of monochromatic electrons may find application in technologies such as electron microscopy, electron beam lithography, and field-emission flatpanel displays.

  17. Direct comparative study on the energy level alignments in unoccupied/occupied states of organic semiconductor/electrode interface by constructing in-situ photoemission spectroscopy and Ar gas cluster ion beam sputtering integrated analysis system

    SciTech Connect

    Yun, Dong-Jin Chung, JaeGwan; Kim, Yongsu; Park, Sung-Hoon; Kim, Seong-Heon; Heo, Sung

    2014-10-21

    Through the installation of electron gun and photon detector, an in-situ photoemission and damage-free sputtering integrated analysis system is completely constructed. Therefore, this system enables to accurately characterize the energy level alignments including unoccupied/occupied molecular orbital (LUMO/HOMO) levels at interface region of organic semiconductor/electrode according to depth position. Based on Ultraviolet Photoemission Spectroscopy (UPS), Inverse Photoemission Spectroscopy (IPES), and reflective electron energy loss spectroscopy, the occupied/unoccupied state of in-situ deposited Tris[4-(carbazol-9-yl)phenyl]amine (TCTA) organic semiconductors on Au (E{sub LUMO}: 2.51 eV and E{sub HOMO}: 1.35 eV) and Ti (E{sub LUMO}: 2.19 eV and E{sub HOMO}: 1.69 eV) electrodes are investigated, and the variation of energy level alignments according to work function of electrode (Au: 4.81 eV and Ti: 4.19 eV) is clearly verified. Subsequently, under the same analysis condition, the unoccupied/occupied states at bulk region of TCTA/Au structures are characterized using different Ar gas cluster ion beam (Ar GCIB) and Ar ion sputtering processes, respectively. While the Ar ion sputtering process critically distorts both occupied and unoccupied states in UPS/IPES spectra, the Ar GCIB sputtering process does not give rise to damage on them. Therefore, we clearly confirm that the in-situ photoemission spectroscopy in combination with Ar GCIB sputtering allows of investigating accurate energy level alignments at bulk/interface region as well as surface region of organic semiconductor/electrode structure.

  18. Physics of the Be(10{bar 1} 0) Surface Core Level Spectrum

    SciTech Connect

    Lizzit, S.; Pohl, K. |; Baraldi, A.; Comelli, G.; Fritzsche, V.; Plummer, E.W. |; Stumpf, R.; Hofmann, P. ||

    1998-10-01

    Photoelectron diffraction has been utilized to confirm the theoretical prediction that the surface core level shifts observed for Be(10{bar 1}0) have been improperly assigned. The original assignment based upon the relative intensity of the shifted components was intuitively obvious: the peak with the largest shift of {minus}0.7 eV with respect to the bulk was associated with the surface plane, the next peak shifted by {minus}0.5 eV stems from the second layer, and the third peak at {minus}0.22 eV from the third and fourth layers. First-principles theory and our experimental data show that the largest shift is associated with the second plane, not the first plane. {copyright} {ital 1998} {ital The American Physical Society }

  19. Exciton and core-level electron confinement effects in transparent ZnO thin films

    PubMed Central

    Mosquera, Adolfo A.; Horwat, David; Rashkovskiy, Alexandr; Kovalev, Anatoly; Miska, Patrice; Wainstein, Dmitry; Albella, Jose M.; Endrino, Jose L.

    2013-01-01

    The excitonic light emission of ZnO films have been investigated by means of photoluminescence measurements in ultraviolet-visible region. Exciton confinement effects have been observed in thin ZnO coatings with thickness below 20 nm. This is enhanced by a rise of the intensity and a blue shift of the photoluminescence peak after extraction of the adsorbed species upon annealing in air. It is found experimentally that the free exciton energy (determined by the photoluminescence peak) is inversely proportional to the square of the thickness while core-level binding energy is inversely proportional to the thickness. These findings correlate very well with the theory of kinetic and potential confinements.

  20. Exploring the core level shift origin of sulfur and thiolates on Pd(111) surfaces.

    PubMed

    Salvarezza, Roberto Carlos; Carro, Pilar

    2015-10-01

    Thiol molecules on planar metal surfaces are widely used for building sensing and electronic devices and also as capping agents to protect and to control the size and shape of nanoparticles. In the case of Pd the thiol molecules exhibit a complex behavior because C-S bond scission is possible, resulting in a significant amount of co-adsorbed S. Therefore identification of these species on Pd is a key point for many applications, a task that is usually achieved by XPS. Here we show, from DFT calculations, that the core level shift (CLS) of the S 2p binding energy (BE) of thiol and sulfur on different thiol-Pd(111) surface models strongly depends on the adsorbed or subsurface state of sulfur atoms. Our results reflect the complexity of S 2p BE behavior and contribute to understanding and reanalyzing the experimental data of thiolated Pd surfaces.

  1. PHOTOEMISSION AS A PROBE OF THE COLLECTIVE EXCITATIONS IN CONDENSED MATTER SYSTEMS.

    SciTech Connect

    JOHNSON, P.D.; VALLA, T.

    2006-08-01

    New developments in instrumentation have recently allowed photoemission measurements to be performed with very high energy and momentum resolution.[1] This has allowed detailed studies of the self-energy corrections to the lifetime and mass renormalization of excitations in the vicinity of the Fermi level. These developments come at an opportune time. Indeed the discovery of high temperature superconductivity in the cuprates and related systems is presenting a range of challenges for condensed matter physics.[2] Does the mechanism of high T{sub c} superconductivity represent new physics? Do we need to go beyond Landau's concept of the Fermi liquid?[3] What, if any, is the evidence for the presence or absence of quasiparticles in the excitation spectra of these complex oxides? The energy resolution of the new instruments is comparable to or better than the energy or temperature scale of superconductivity and the energy of many collective excitations. As such, photoemission has again become recognized as an important probe of condensed matter. Studies of the high T{sub c} superconductors and related materials are aided by the observation that they are two dimensional. To understand this, we note that the photoemission process results in both an excited photoelectron and a photohole in the final state. Thus the experimentally measured photoemission peak is broadened to a width reflecting contributions from both the finite lifetime of the photohole and the momentum broadening of the outgoing photoelectron.

  2. A photoemission study of the effectiveness of nickel, manganese, and cobalt based corrosion barriers for silicon photo-anodes during water oxidation

    NASA Astrophysics Data System (ADS)

    O'Connor, Robert; Bogan, Justin; McCoy, Anthony; Byrne, Conor; Hughes, Greg

    2016-05-01

    Silicon is an attractive material for solar water splitting applications due to its abundance and its capacity to absorb a large fraction of incident solar radiation. However, it has not received as much attention as other materials due to its tendency to oxidize very quickly in aqueous environments, particularly when it is employed as the anode where it drives the oxygen evolution reaction. In recent years, several works have appeared in the literature examining the suitability of thin transition metal oxide films grown on top of the silicon to act as a corrosion barrier. The film should be transparent to solar radiation, allow hole transport from the silicon surface to the electrolyte, and stop the diffusion of oxygen from the electrolyte back to the silicon. In this work, we compare Mn-oxide, Co-oxide, and Ni-oxide thin films grown using physical vapor deposition in order to evaluate which material offers the best combination of photocurrent and corrosion protection. In addition to the electrochemical data, we also present a detailed before-and-after study of the surface chemistry of the films using x-ray photoelectron spectroscopy. This approach allows for a comprehensive analysis of the mechanisms by which the corrosion barriers protect the underlying silicon, and how they degrade during the water oxidation reaction.

  3. Chemical bonding and charge redistribution - Valence band and core level correlations for the Ni/Si, Pd/Si, and Pt/Si systems

    NASA Technical Reports Server (NTRS)

    Grunthaner, P. J.; Grunthaner, F. J.; Madhukar, A.

    1982-01-01

    Via a systematic study of the correlation between the core and valence level X-ray photoemission spectra, the nature of the chemical bonding and charge redistribution for bulk transition metal silicides has been examined. Particular emphasis is placed on Pt2Si and PtSi. It is observed that the strength of the metal (d)-silicon (p) interaction increases in the order Ni2Si, Pd2Si, Pt2Si. It is also observed that both the metal and silicon core lines shift to higher binding energy as the silicides are formed. The notion of charge redistribution for metallic bonds is invoked to explain these data.

  4. Molecular photoemission studies using synchrotron radiation

    SciTech Connect

    Truesdale, C.M.

    1983-04-01

    The angular distributions of photoelectrons and Auger electrons were measured by electron spectroscopy using synchrotron radiation. The experimental results are compared with theoretical calculations to interpret the electronic behavior of photoionization for molecular systems.

  5. Photoemission study of Li@C60

    NASA Astrophysics Data System (ADS)

    Yagi, Hajime; Ogasawara, Naoko; Zenki, Masashi; Miyazaki, Takafumi; Hino, Shojun

    2016-05-01

    Ultraviolet and X-ray photoelectron spectra (UPS and XPS) of thin films prepared by either depositing or applying [Li@C60]+(PF6)- on the substrates are presented. The UPS and XPS of [Li@C60]+(PF6)- applied films suggest that PF6- anions come out from the surface by annealing at 250 °C. The UPS and XPS of the deposited thin films indicate that the film does not contain PF6- anion but is composed of only Li@C60. Changing the sublimation temperature reveals that encapsulated Li cations begin to escape from the C60 cage when heated above 550 °C.

  6. Attosecond interferometry on surfaces: Laser-assisted photoemission from Ag(111) and Au(111) by an XUV pulse train

    NASA Astrophysics Data System (ADS)

    Ambrosio, Marcelo J.; Thumm, Uwe

    2016-05-01

    Motivated by recent RABBITT experiments, we numerically investigated electron emission from metal surfaces by a pulse train of phase coherent attosecond XUV pulses into the assisting electric field of a time-delayed IR laser pulse. From the delay-dependent oscillations of the first-sideband-electron yields in our simulated spectra we deduced the atomic phases of the pulse train's higher harmonic components. These calculations allow us to extract physical properties of solid surfaces, as we numerically demonstrate for the Ag(111) and Au(111) surfaces targeted in, including photoemission from conduction-band and core-level electrons. Supported by the NSF and the Division of Chemical Sciences, Office of the Basic Energy Sciences, Office of Energy Research, US DoE.

  7. An imaging photoemission polarimeter for soft X-rays

    NASA Technical Reports Server (NTRS)

    Kaaret, Philip; Novick, Robert; Heckler, A.; Shaw, P.; Fraser, G. W.

    1990-01-01

    Results of investigations are reviewed to assess the polarization dependence of photoemission in the optical, UV, and soft X-ray bands, as well as present a design for an imaging photoelectric polarimeter. Data regarding the effect of the dependence in the soft X-ray band are emphasized including the quantity of photons produced by each X-ray. The phase shift encountered in some experiments indicates that a third axis is present; the importance of the phase shift in understanding the vectoral photoeffect is emphasized. Measurements of the pulse height show that this measure is proportional to the number of electrons photoemitted by the incident X-ray. The development of X-ray polarimeters can be significantly improved as a result of the study of polarization sensitivity in the photoelectric effect. The design of a photoelectric polarimeter is presented, and the potential uses for the instrument include measuring the polarization of supernova remnants, AGN, and black hole candidates.

  8. Compact extreme ultraviolet source for laboratory-based photoemission spectromicroscopy

    NASA Astrophysics Data System (ADS)

    Schmitz, Christoph; Wilson, Daniel; Rudolf, Denis; Wiemann, Carsten; Plucinski, Lukasz; Riess, Sally; Schuck, Martin; Hardtdegen, Hilde; Schneider, Claus M.; Tautz, F. Stefan; Juschkin, Larissa

    2016-06-01

    We report on the combination of a state-of-the-art energy-filtering photoemission electron microscope with an intense yet compact laboratory-based gas discharge extreme ultraviolet (EUV) light source. Using a photon energy of 71.7 eV from oxygen plasma (O5+ spectral line), we demonstrate element-selective photoelectron imaging in real space and band structure mapping in reciprocal space. Additionally, the high surface sensitivity of the EUV light was used to study the surface oxidation on islands of the phase-change material Ge1Sb2Te4 . The EUV light source allows the extension of spectromicroscopy, previously only feasible at synchrotron beamlines, to laboratory-based work.

  9. Calculation of 3s photoemission spectra of vanadium on graphite

    SciTech Connect

    Krueger, P.; Taguchi, M.; Parlebas, J.C.; Kotani, A.

    1997-06-01

    A few years ago, a satellite structure in the vanadium 3s x-ray photoemission spectroscopy (XPS) spectrum of V clusters upon graphite was observed and attributed to the presence of magnetic moments on the V surface. Here, we present calculations of these spectra using a cluster model that takes into account intra-atomic d-d and d{endash}core electron correlation and hybridization between V d and graphite {pi} states. When the V-graphite distance is increased from 1.5 to 2.0 {Angstrom} the system undergoes a low-to-high spin transition, which is clearly evidenced in the evolution of the XPS line shape. Although direct comparison with experiment is difficult, our study suggests that the observed satellite is due to core hole screening rather than a magnetic moment on the V atom. {copyright} {ital 1997} {ital The American Physical Society}

  10. High- Tc superconductivity: new issues from photoemission data

    NASA Astrophysics Data System (ADS)

    Margaritondo, G.; Grioni, M.; Vobornik, I.; Pavuna, D.

    2001-11-01

    Recent high-resolution photoemission results on high- Tc superconductors and other low-dimensional systems solve some critical issues but also open new fundamental questions. A recent breakthrough enabled us to clarify the interplay of conflicting periodicities in photoemission data, thus legitimizing the photoemission analysis of crystals with super-periodicities. On the other hand, results on the role of doping and of intentional disorder in Bi 2Sr 2CaCu 2O 8+ x single crystals raise questions about the origin of the pseudogap.

  11. The electronic and chemical structure of the a-B3CO0.5:Hy-to-metal interface from photoemission spectroscopy: implications for Schottky barrier heights.

    PubMed

    Driver, M Sky; Paquette, Michelle M; Karki, S; Nordell, B J; Caruso, A N

    2012-11-01

    The electronic and chemical structure of the metal-to-semiconductor interface was studied by photoemission spectroscopy for evaporated Cr, Ti, Al and Cu overlayers on sputter-cleaned as-deposited and thermally treated thin films of amorphous hydrogenated boron carbide (a-B(x)C:H(y)) grown by plasma-enhanced chemical vapor deposition. The films were found to contain ~10% oxygen in the bulk and to have approximate bulk stoichiometries of a-B(3)CO(0.5):H(y). Measured work functions of 4.7/4.5 eV and valence band maxima to Fermi level energy gaps of 0.80/0.66 eV for the films (as-deposited/thermally treated) led to predicted Schottky barrier heights of 1.0/0.7 eV for Cr, 1.2/0.9 eV for Ti, 1.2/0.9 eV for Al, and 0.9/0.6 eV for Cu. The Cr interface was found to contain a thick partial metal oxide layer, dominated by the wide-bandgap semiconductor Cr(2)O(3), expected to lead to an increased Schottky barrier at the junction and the formation of a space-charge region in the a-B(3)CO(0.5):H (y) layer. Analysis of the Ti interface revealed a thick layer of metal oxide, comprising metallic TiO and Ti (2)O (3), expected to decrease the barrier height. A thinner, insulating Al(2)O(3) layer was observed at the Al-to-a-B(3)CO(0.5):H(y) interface, expected to lead to tunnel junction behavior. Finally, no metal oxides or other new chemical species were evident at the Cu-to-a-B(3)CO(0.5):H(y) interface in either the core level or valence band photoemission spectra, wherein characteristic metallic Cu features were observed at very thin overlayer coverages. These results highlight the importance of thin-film bulk oxygen content on the metal-to-semiconductor junction character as well as the use of Cu as a potential Ohmic contact material for amorphous hydrogenated boron carbide semiconductor devices such as high-efficiency direct-conversion solid-state neutron detectors.

  12. Core level photoelectron spectroscopy on the lanthanide-induced hydrolysis of DNA

    NASA Astrophysics Data System (ADS)

    Shigekawa, Hidemi; Ikawa, Hiroyuki; Yoshizaki, Ryozo; Iijima, Yoshitoki; Sumaoka, Jun; Komiyama, Makoto

    1996-03-01

    The electronic structures of the complexes of diphenyl phosphate (DPP), a model compound of DNA, with lanthanide ions have been investigated to shed light on the mechanism of the cerium (IV)-induced nonenzymatic hydrolysis of DNA. Binding energies of the P 2p core level of DPP were 134.2 eV for the complexes with La(III), Eu(III), and Lu(III), and was 134.4 eV for the Ce(IV) complex, when the metal/DPP molar ratio was 1:1. When the molar ratio was increased, only Ce(IV), the most active metal ion for DNA hydrolysis, showed a chemical shift of ˜0.5 eV toward the higher binding energy region. The chemical shift of ˜0.5 eV toward the higher binding energy region. The chemical shift was due to the systematic increase in the intensity of the higher binding energy component. The observed change in the electronic structure of the DPP-Ce(IV) complex may be related to the superb ability of Ce(IV) for the hydrolysis of DNA.

  13. Adsorption and dissociation of acidic trace gases on ice surfaces - caught in the act with core level spectroscopy

    NASA Astrophysics Data System (ADS)

    Waldner, Astrid; Orlando, Fabrizio; Ammann, Markus; Kleibert, Armin; Huthwelker, Thomas; Peter, Thomas; Bartels-Rausch, Thorsten

    2015-04-01

    Chemistry and physical processes in Earth's ice and snow cover can change the composition of the atmosphere and the contaminant content of the cryosphere. They have thus direct impacts on geochemical cycles and the climate system. Our ability to predict the fate of chemicals in snow or air masses in exchange with the cryosphere on a regional scale or to model those in snow chemistry models is currently hampered by our limited understanding of the underlying mechanisms on a molecular level. So far, direct experimental observations under environmentally relevant conditions of the ice surface and of the adsorption of trace gases to it are very limited. The unique approach of this study is to combine two surface sensitive spectroscopic methods to directly probe the hydrogen-bonding network at the ice surface ( ~1 nm depth) and the concentration, depth profile (~1 to 10 nm), and dissociation degree of the dopant. We present first core-electron photoemission (XPS) and partial electron yield X-ray absorption (NEXAFS) measurements of formic acid adsorbed to ice at 240 K. The analysis of oxygen NEXAFS spectra reveals information on changes in the hydrogen-bonding network of the ice surface upon adsorption of formic acid. Depth profiles based on XPS measurements indicate that the adsorbed acid stays at the ice surface. Furthermore we obtained a preliminary estimation of the degree of formic acid dissociation at the ice surface. Results are compared to earlier core-electron studies of several trace gases adsorbed to ice at 240 K and compared to results from more traditional method to and snow to reveal fundamental aspects of the ice surface and how it interacts with dopants. Even with the focus on adsorption of acidic trace gases to ice, results of this study will thus be of high relevance also for other chemical processes in ice and snow. This is of interest not only in environmental science but also in material science, cryobiology, and astrophysics.

  14. O- and H-induced surface core level shifts on Ru(0001): prevalence of the additivity rule

    NASA Astrophysics Data System (ADS)

    Lizzit, S.; Zhang, Y.; Kostov, K. L.; Petaccia, L.; Baraldi, A.; Menzel, D.; Reuter, K.

    2009-04-01

    In previous work on adsorbate-induced surface core level shifts (SCLSs), the effects caused by O atom adsorption on Rh(111) and Ru(0001) were found to be additive: the measured shifts for first-layer Ru atoms depended linearly on the number of directly coordinated O atoms. Density-functional theory calculations quantitatively reproduced this effect, allowed separation of initial- and final-state contributions, and provided an explanation in terms of a roughly constant charge transfer per O atom. We have now conducted similar measurements and calculations for three well-defined adsorbate and coadsorbate layers containing O and H atoms: (1 × 1)-H, (2 × 2)-(O+H) and (2 × 2)-(O+3H) on Ru(0001). As H is stabilized in fcc sites in the prior two structures and in hcp sites in the latter, this enables us to not only study coverage and coadsorption effects on the adsorbate-induced SCLSs, but also the sensitivity to similar adsorption sites. Remarkably good agreement is obtained between experiment and calculations for the energies and geometries of the layers, as well as for all aspects of the SCLS values. The additivity of the next-neighbor adsorbate-induced SCLSs is found to prevail even for the coadsorbate structures. While this confirms the suggested use of SCLSs as fingerprints of the adsorbate configuration, their sensitivity is further demonstrated by the slightly different shifts unambiguously determined for H adsorption in either fcc or hcp hollow sites.

  15. Observation by resonant angle-resolved photoemission of a critical thickness for 2-dimensional electron gas formation in SrTiO{sub 3} embedded in GdTiO{sub 3}

    SciTech Connect

    Nemšák, S.; Conti, G.; Palsson, G. K.; Conlon, C.; Fadley, C. S.; Cho, S.; Rault, J. E.; Avila, J.; Asensio, M.-C.; Jackson, C. A.; Moetakef, P.; Janotti, A.; Bjaalie, L.; Himmetoglu, B.; Van de Walle, C. G.; Stemmer, S.; Balents, L.; Schneider, C. M.

    2015-12-07

    For certain conditions of layer thickness, the interface between GdTiO{sub 3} (GTO) and SrTiO{sub 3} (STO) in multilayer samples has been found to form a two-dimensional electron gas (2DEG) with very interesting properties including high mobilities and ferromagnetism. We have here studied two trilayer samples of the form [2 nm GTO/1.0 or 1.5 unit cells STO/10 nm GTO] as grown on (001) (LaAlO{sub 3}){sub 0.3}(Sr{sub 2}AlTaO{sub 6}){sub 0.7}, with the STO layer thicknesses being at what has been suggested is the critical thickness for 2DEG formation. We have studied these with Ti-resonant angle-resolved and angle-integrated photoemission and find that the spectral feature in the spectra associated with the 2DEG is present in the 1.5 unit cell sample, but not in the 1.0 unit cell sample. We also observe through core-level spectra additional states in Ti and Sr, with the strength of a low-binding-energy state for Sr being associated with the appearance of the 2DEG, and we suggest it to have an origin in final-state core-hole screening.

  16. Photoemission from Shockley surface state on Ag(111)

    NASA Astrophysics Data System (ADS)

    Karkare, Siddharth; Wan, Weishi; Feng, Jun; Padmore, Howard

    We present measurements of quantum yield and transverse momentum distributions of electrons emitted from the Shockley surface state on Ag(111) surface using near threshold photons. Our measurements shed light on the validity of the conservation of transverse momentum during photoemission when the kinetic energy of electrons is less than 0.1 eV. We also develop a one-step photoemission model that quantitatively explains photoemission from single crystal metal surfaces. This model accurately calculates the dependence of the electron yield on the angle of incidence and the polarization of incident light (vectorial photoelectric effect). We show excellent agreement between the measured and calculated photoemission properties of the Ag(111) surface. Our measurements show that Ag(111) surface can act as an excellent electron source for several applications like Free Electron Lasers and Ultra-fast Electron Diffraction.

  17. Accurate determination of the valence band edge in hard x-ray photoemission spectra using GW theory

    NASA Astrophysics Data System (ADS)

    Lischner, Johannes; Nemšák, Slavomír; Conti, Giuseppina; Gloskovskii, Andrei; Pálsson, Gunnar Karl; Schneider, Claus M.; Drube, Wolfgang; Louie, Steven G.; Fadley, Charles

    2016-04-01

    We introduce a new method for determining accurate values of the valence-band maximum in x-ray photoemission spectra. Specifically, we align the sharpest peak in the valence-band region of the experimental spectrum with the corresponding feature of a theoretical valence-band density of states curve from ab initio GW theory calculations. This method is particularly useful for soft and hard x-ray photoemission studies of materials with a mixture of valence-band characters, where strong matrix element effects can render standard methods for extracting the valence-band maximum unreliable. We apply our method to hydrogen-terminated boron-doped diamond, which is a promising substrate material for novel solar cell devices. By carrying out photoemission experiments with variable light polarizations, we verify the accuracy of our analysis and the general validity of the method.

  18. Internal Photoemission Spectroscopy of 2-D Materials

    NASA Astrophysics Data System (ADS)

    Nguyen, Nhan; Li, Mingda; Vishwanath, Suresh; Yan, Rusen; Xiao, Shudong; Xing, Huili; Cheng, Guangjun; Hight Walker, Angela; Zhang, Qin

    Recent research has shown the great benefits of using 2-D materials in the tunnel field-effect transistor (TFET), which is considered a promising candidate for the beyond-CMOS technology. The on-state current of TFET can be enhanced by engineering the band alignment of different 2D-2D or 2D-3D heterostructures. Here we present the internal photoemission spectroscopy (IPE) approach to determine the band alignments of various 2-D materials, in particular SnSe2 and WSe2, which have been proposed for new TFET designs. The metal-oxide-2-D semiconductor test structures are fabricated and characterized by IPE, where the band offsets from the 2-D semiconductor to the oxide conduction band minimum are determined by the threshold of the cube root of IPE yields as a function of photon energy. In particular, we find that SnSe2 has a larger electron affinity than most semiconductors and can be combined with other semiconductors to form near broken-gap heterojunctions with low barrier heights which can produce a higher on-state current. The details of data analysis of IPE and the results from Raman spectroscopy and spectroscopic ellipsometry measurements will also be presented and discussed.

  19. Universal versus Material-Dependent Two-Gap Behaviors in the High-Tc Cuprates: Angle-Resolved Photoemission Study of La_2-xSr_xCuO_4

    SciTech Connect

    Yoshida, T.

    2010-06-04

    We have investigated the doping and temperature dependences of the pseudogap/superconducting gap in the single-layer cuprate La{sub 2-x}Sr{sub x}CuO{sub 4} by angle-resolved photoemission spectroscopy. The results clearly exhibit two distinct energy and temperature scales, namely, the gap around ({pi}, 0) of magnitude {Delta}{asterisk} and the gap around the node characterized by the d-wave order parameter {delta}{sub 0}, like the double-layer cuprate Bi2212. In comparison with Bi2212 having higher T{sub c}'s, {delta}{sub 0} is smaller, while {delta}{asterisk} and T{ampersand} are similar. This result suggests that {delta}{asterisk} and T{asterisk} are approximately material-independent properties of a single Cu0{sub 2} plane, in contrast the material-dependent {delta}{sub 0}, representing the pairing strength.

  20. Metal-insulator transition and tunable Dirac-cone surface state in the topological insulator TlBi1 -xSbxTe2 studied by angle-resolved photoemission

    NASA Astrophysics Data System (ADS)

    Trang, Chi Xuan; Wang, Zhiwei; Yamada, Keiko; Souma, Seigo; Sato, Takafumi; Takahashi, Takashi; Segawa, Kouji; Ando, Yoichi

    2016-04-01

    We report a systematic angle-resolved photoemission spectroscopy on topological insulator (TI) TlBi1 -xSbxTe2 which is bulk insulating at 0.5 ≲x ≲0.9 and undergoes a metal-insulator-metal transition with the Sb content x . We found that this transition is characterized by a systematic hole doping with increasing x , which results in the Fermi-level crossings of the bulk conduction and valence bands at x ˜0 and x ˜1 , respectively. The Dirac point of the topological surface state is gradually isolated from the valence-band edge, accompanied by a sign reversal of Dirac carriers. We also found that the Dirac velocity is the largest among known solid-solution TI systems. The TlBi1 -xSbxTe2 system thus provides an excellent platform for Dirac-cone engineering and device applications of TIs.

  1. Communication: Induced photoemission from nonadiabatic dynamics assisted by dynamical Stark effect.

    PubMed

    Arasaki, Yasuki; Scheit, Simona; Takatsuka, Kazuo

    2013-04-28

    Through nonadiabatic interaction due to electron transfer as that in alkali halides, vibrational dynamics on the ionic potential energy surface (large dipole moment) is coupled to that on the covalent surface (small dipole moment). Thus, population transfer between the states should cause long-range electron jump between two remote sites, which thereby leads to a sudden change of the large molecular dipole moment. Therefore, by making repeated use of the dynamical Stark effect, one may expect emission of photons from it. We show with coupled quantum wavepacket dynamics calculation that such photoemission can indeed occur and can be controlled by an external field. The present photoemission can offer an alternative scheme to study femtosecond and subfemtosecond vibrational and electronic dynamics and may serve as a unique optical source. PMID:23635103

  2. Spin polarization and magnetic dichroism in photoemission from core and valence states in localized magnetic systems. IV. Core-hole polarization in resonant photoemission

    NASA Astrophysics Data System (ADS)

    van der Laan, Gerrit; Thole, B. T.

    1995-12-01

    A simple theory is presented for core-hole polarization probed by resonant photoemission in a two-steps approximation. After excitation from a core level to the valence shell, the core hole decays into two shallower core holes under emission of an electron. The nonspherical core hole and the final state selected cause a specific angle and spin distribution of the emitted electron. The experiment is characterized by the ground-state moments, the polarization of the light, and the spin and angular distribution of the emitted electron. The intensity is a sum over ground-state expectation values of tensor operators times the probability to create a polarized core hole using polarized light, times the probability for decay of such a core hole into the final state. We give general expressions for the angle- and spin-dependent intensities in various regimes of Coulomb and spin-orbit interaction: LS, LSJ, and jjJ coupling. The core-polarization analysis, which generalizes the use of sum rules in x-ray absorption spectroscopy where the integrated peak intensities give ground-state expectation values of the spin and orbital moment operators, makes it possible to measure different linear combinations of these operators. As an application the 2p3/23p3p decay in ferromagnetic nickel is calculated using Hartree-Fock values for the radial matrix elements and phase factors, and compared with experiment, the dichroism is smaller in the 3P final state but stronger in the 1D, 1S peak.

  3. Antenna-coupled Photoemission from Single Quantum Emitters

    NASA Astrophysics Data System (ADS)

    Bharadwaj, Palash

    Optical antennas are analogs of their radiowave and microwave counterparts, and can be defined as devices that serve to efficiently convert free-propagating optical radiation to localized energy, and vice-versa. Colloidal metal nanoparticles with their strong plasmonic optical response offer a convenient realization of optical antennas. Such nanoparticle antennas serve to spatially enhance and localize fields, and modify the excitation rate and the radiative decay rate when placed close to single emitters (molecules, quantum dots, etc.). In addition, they can also cause undesirable losses, leading to an increase in the non-radiative decay rates of these emitters. This interplay of rates can lead to a strong modification of the emission characteristics over the intrinsic behavior. We study photoemission from single emitters coupled to antennas of different geometries made from colloidal metal nanoparticles. We demonstrate enhancements of fluorescence from single quantum emitters by a factor 10 to 100, with the highest enhancements resulting for molecules with very low intrinsic quantum yields. Such enhancements afford an improvement in resolution for fluorescence imaging down to lambda/40. We also investigate changes to fluorescence blinking of a colloidal quantum dots (QD) coupled to an antenna, as a function of antenna-QD distance. We find that power-law blinking is preserved unaltered even as the antenna drastically modifies the excitonic decay rate in the QD, and reduces the blinking probability. This resilience of the power-law to change provides evidence that blinking statistics are not swayed by environment-induced variations in kinetics, and offers clues towards identifying the as-yet unknown mechanism behind universal fluorescence intermittency. Finally, in analogy with traditional electromagnetic antennas, we excite proto-typical optical antennas using electrons (current) instead of photons (fields). We excite localized plasmons using low energy tunneling

  4. X-ray photo-emission and energy dispersive spectroscopy of HA coated titanium

    SciTech Connect

    Drummond, J.L.; Steinberg, A.D.; Krauss, A.R.

    1997-08-01

    The purpose of this study was to determine the chemical composition changes of hydroxyapatite (HA) coated titanium using surface analysis (x-ray photo-emission) and bulk analysis (energy dispersive spectroscopy). The specimens examined were controls, 30 minutes and 3 hours aged specimens in distilled water or 0.2M sodium phosphate buffer (pH 7.2) at room temperature. Each x-ray photo-emission cycle consisted of 3 scans followed by argon sputtering for 10 minutes for a total of usually 20 cycles, corresponding to a sampling depth of {approximately} 1500 {angstrom}. The energy dispersive spectroscopy analysis was on a 110 by 90 {mu}m area for 500 sec. Scanning electron microscopy examination showed crystal formation (3P{sub 2}O{sub 5}*2CAO*?H{sub 2}O by energy dispersive spectroscopy analysis) on the HA coating for the specimens aged in sodium phosphate buffer. The x-ray photo-emission results indicated the oxidation effect of water on the titanium (as TiO{sub 2}) and the effect of the buffer to increase the surface concentration of phosphorous. No differences in the chemical composition were observed by energy dispersive spectroscopy analysis. The crystal growth was only observed for the sodium phosphate buffer specimens and only on the HA surface.

  5. Angle resolved photoemission from organic semiconductors: orbital imaging beyond the molecular orbital interpretation

    NASA Astrophysics Data System (ADS)

    Dauth, M.; Wiessner, M.; Feyer, V.; Schöll, A.; Puschnig, P.; Reinert, F.; Kümmel, S.

    2014-10-01

    Fascinating pictures that can be interpreted as showing molecular orbitals have been obtained with various imaging techniques. Among these, angle resolved photoemission spectroscopy (ARPES) has emerged as a particularly powerful method. Orbital images have been used to underline the physical credibility of the molecular orbital concept. However, from the theory of the photoemission process it is evident that imaging experiments do not show molecular orbitals, but Dyson orbitals. The latter are not eigenstates of a single-particle Hamiltonian and thus do not fit into the usual simple interpretation of electronic structure in terms of molecular orbitals. In a combined theoretical and experimental study we thus check whether a Dyson-orbital and a molecular-orbital based interpretation of ARPES lead to differences that are relevant on the experimentally observable scale. We discuss a scheme that allows for approximately calculating Dyson orbitals with moderate computational effort. Electronic relaxation is taken into account explicitly. The comparison reveals that while molecular orbitals are frequently good approximations to Dyson orbitals, a detailed understanding of photoemission intensities may require one to go beyond the molecular orbital picture. In particular we clearly observe signatures of the Dyson-orbital character for an adsorbed semiconductor molecule in ARPES spectra when these are recorded over a larger momentum range than in earlier experiments.

  6. Theoretical predictions of the impact of nuclear dynamics and environment on core-level spectra of organic molecules

    NASA Astrophysics Data System (ADS)

    Prendergast, David; Schwartz, Craig; Uejio, Janel; Saykally, Richard

    2009-03-01

    Core-level spectroscopy provides an element-specific probe of local electronic structure and bonding, but linking details of atomic structure to measured spectra relies heavily on accurate theoretical interpretation. We present first principles simulations of the x-ray absorption of a range of organic molecules both in isolation and aqueous solvation, highlighting the spectral impact of internal nuclear motion as well as solvent interactions. Our approach uses density functional theory with explicit inclusion of the core-level excited state within a plane-wave supercell framework. Nuclear degrees of freedom are sampled using various molecular dynamics techniques. We indicate specific cases for molecules in their vibrational ground state at experimental conditions, where nuclear quantum effects must be included. Prepared by LBNL under Contract DE-AC02-05CH11231.

  7. Temperature-dependent internal photoemission probe for band parameters

    NASA Astrophysics Data System (ADS)

    Lao, Yan-Feng; Perera, A. G. Unil

    2012-11-01

    The temperature-dependent characteristic of band offsets at the heterojunction interface was studied by an internal photoemission (IPE) method. In contrast to the traditional Fowler method independent of the temperature (T), this method takes into account carrier thermalization and carrier/dopant-induced band-renormalization and band-tailing effects, and thus measures the band-offset parameter at different temperatures. Despite intensive studies in the past few decades, the T dependence of this key band parameter is still not well understood. Re-examining a p-type doped GaAs emitter/undoped AlxGa1-xAs barrier heterojunction system disclosed its previously ignored T dependency in the valence-band offset, with a variation up to ˜-10-4 eV/K in order to accommodate the difference in the T-dependent band gaps between GaAs and AlGaAs. Through determining the Fermi energy level (Ef), IPE is able to distinguish the impurity (IB) and valence bands (VB) of extrinsic semiconductors. One important example is to determine Ef of dilute magnetic semiconductors such as GaMnAs, and to understand whether it is in the IB or VB.

  8. Photoemission from Ag, Cu, and CsI

    SciTech Connect

    Srinivasan-Rao, T.; Fischer, J.; Tsang, T.

    1992-06-01

    Photoemission characteristics of three different cathodes, CsI, Ag film and Cu were investigated. CsI, upon irradiation by 213 nm, 10ps laser pulse yields a quantum efficiency of 4% at O.2[mu]J input energy. The saturation mechanism observed at higher input energies require further investigation. Ag film, upon irradiation by 630 nm, 300 fs laser emit prompt photoelectrons after absorbing 2 photons. There was no evidence of optical damage of the film up to 10[sup 11] W/cm[sup 2]. At low intensities, photoemission from Cu is a simple [nu]-e[sup [minus

  9. Si1-XGex/Si-Heterojunction Internal-Photoemission Detectors

    NASA Technical Reports Server (NTRS)

    Lin, True-Lon; Maserjian, Joseph

    1992-01-01

    Cutoff wavelengths tailored by choice of Ge content. Infrared detectors based on internal photoemission at Si1-xGex/Si heterojunctions exhibited photoresponses at wavelengths from 2 to 12 micrometers in initial tests. Si1-xGex/Si-heterojunction internal-photoemission detectors tailored for use at wavelengths of order of 10 micrometers. Future developments expected to include integration of such devices with silicon readout circuitry to form infrared-imaging arrays. Imaging arrays operating in important wavelength range of 8 to 12 micrometers can be fabricated relatively inexpensively for use in outer-space, military, and industrial applications.

  10. Electronic band structure and photoemission: A review and projection

    SciTech Connect

    Falicov, L.M.

    1987-09-01

    A brief review of electronic-structure calculations in solids, as a means of interpreting photoemission spectra, is presented. The calculations are, in general, of three types: ordinary one-electron-like band structures, which apply to bulk solids and are the basis of all other calculations; surface modified calculations, which take into account, self-consistently if at all possible, the presence of a vacuum-solid interface and of the electronic modifications caused thereby; and many-body calculations, which go beyond average-field approximations and consider dynamic rearrangement effects caused by electron-electron correlations during the photoemission process. 44 refs.

  11. Synchrotron radiation photoemission study of interfacial electronic structure of HfO{sub 2} on In{sub 0.53}Ga{sub 0.47}As(001)-4 × 2 from atomic layer deposition

    SciTech Connect

    Pi, T. W. E-mail: gkwer@verizon.net E-mail: mhong@phys.ntu.edu.tw; Lin, T. D.; Chang, Y. C.; Hong, M. E-mail: gkwer@verizon.net E-mail: mhong@phys.ntu.edu.tw; Lin, H. Y.; Kwo, J. E-mail: gkwer@verizon.net E-mail: mhong@phys.ntu.edu.tw; Wertheim, G. K. E-mail: gkwer@verizon.net E-mail: mhong@phys.ntu.edu.tw

    2014-01-27

    The growth of a passivating layer on a In{sub 0.53}Ga{sub 0.47}As(001)-4 × 2 surface by atomic-layer deposition of tetrakis[ethylmethylamino]Hafnium (TEMAHf)) followed by the water pulse was investigated by synchrotron radiation photoemission. The Hf atoms maintain four-fold coordination, both after the initial TEMAHf deposition and the subsequent water pulse. The Hf atoms initially bond to the As dangling bonds of the surface As atom located on the edges of the raised ridges. One EMA ligand is removed in this process. Subsequent water exposure substitutes OH ligand for one or more remaining EMA ligands. These in turn react with TEMAHf to form Hf-O-Hf bonds allowing the hafnium oxides to grow. The surface In atoms on the terrace of the raised ridges were partially removed, but none bonded of the precursor atoms. Correlations between the interfacial electronic structure and the electric performance are discussed.

  12. Photoemission of Single Dust Grains for Heliospheric Conditions

    NASA Technical Reports Server (NTRS)

    Spann, James F., Jr.; Venturini, Catherine C.; Abbas, Mian M.; Comfort, Richard H.

    2000-01-01

    Initial results of an experiment to measure the photoemission of single dust grains as a function of far ultraviolet wavelengths are presented. Coulombic forces dominate the interaction of the dust grains in the heliosphere. Knowledge of the charge state of dust grains, whether in a dusty plasma (Debye length < intergrain distance) or in the diffuse interplanetary region, is key to understanding their interaction with the solar wind and other solar system constituents. The charge state of heliospheric grains is primarily determined by primary electron and ion collisions, secondary electron emission and photoemission due to ultraviolet sunlight. We have established a unique experimental technique to measure the photoemission of individual micron-sized dust grains in vacuum. This technique resolves difficulties associated with statistical measurements of dust grain ensembles and non-static dust beams. The photoemission yield of Aluminum Oxide 3-micron grains For wavelengths from 120-300 nm with a spectral resolution of 1 nm FWHM is reported. Results are compared to interplanetary conditions.

  13. Exploring the Electronic Structure and Chemical Homogeneity of Individual Bi2Te3 Nanowires by Nano-Angle-Resolved Photoemission Spectroscopy.

    PubMed

    Krieg, Janina; Chen, Chaoyu; Avila, José; Zhang, Zeying; Sigle, Wilfried; Zhang, Hongbin; Trautmann, Christina; Asensio, Maria Carmen; Toimil-Molares, Maria Eugenia

    2016-07-13

    Due to their high surface-to-volume ratio, cylindrical Bi2Te3 nanowires are employed as model systems to investigate the chemistry and the unique conductive surface states of topological insulator nanomaterials. We report on nanoangle-resolved photoemission spectroscopy (nano-ARPES) characterization of individual cylindrical Bi2Te3 nanowires with a diameter of 100 nm. The nanowires are synthesized by electrochemical deposition inside channels of ion-track etched polymer membranes. Core level spectra recorded with submicron resolution indicate a homogeneous chemical composition along individual nanowires, while nano-ARPES intensity maps reveal the valence band structure at the single nanowire level. First-principles electronic structure calculations for chosen crystallographic orientations are in good agreement with those revealed by nano-ARPES. The successful application of nano-ARPES on single one-dimensional nanostructures constitutes a new avenue to achieve a better understanding of the electronic structure of topological insulator nanomaterials.

  14. Electronic Properties of Pseudomorphic Metallic Films: Photoemission and Inverse Photoemission Measurements

    NASA Astrophysics Data System (ADS)

    Mankey, Gary Jay

    Recent developments in experimental physics have made possible the production and characterization of ultrathin metallic films of atomic dimension. The methods used to grow pseudomorphic fcc films of Ni, Co, and Fe on Cu(001) are described. High-quality epitaxial films are produced by vapor deposition in an ultra-high vacuum environment on suitably prepared substrates. The morphology of these films is characterized using a variety of experimental techniques: Auger electron spectroscopy, low-energy electron diffraction, reflection high-energy electron diffraction, and thermal desorption spectroscopy of adsorbed hydrogen. The magnetic properties of the films are measured with a surface magneto-optic Kerr effect magnetometer. The occupied and unoccupied electronic band dispersions and critical point energies are determined with photoemission and inverse photoemission measurements. These measurements are used as eigenvalues for an empirical combined interpolation scheme bandstructure calculation of the energy bands along the fcc(001) surface normal. Results are presented for Cu(001), Ni(001), Co(001), and paramagnetic Fe(001). Changes in the unoccupied electronic states in the ultrathin film limit are determined for Co and Fe films on Cu(111). The Co films exhibit a bulk-like electronic structure similar to hcp Co(0001) down to films one atomic layer thick. The low-spin ferromagnetic phase of fcc Fe is produced on Cu(111) for films below 5 atomic layers thick. Above this thickness, the Fe films revert to a bulk-like bcc(110) phase. The development of the electronic structure is measured for ultrathin Cu films grown on a specially prepared fcc Co(001) substrate. The Cu 3d band is significantly narrowed for films 1 atomic layer thick and bulk-like for films 3 atomic layers thick (one fcc unit cell). The s, p band exhibits quantum-well states due to the discretization of reciprocal space in the direction perpendicular to the film surface. These quantum-well states are

  15. Inner-shell photoemission from atoms and molecules using synchrotron radiation

    SciTech Connect

    Lindle, D.W.

    1983-12-01

    Photoelectron spectroscopy, in conjunction with synchrotron radiation, has been used to study inner-shell photoemission from atoms and molecules. The time structure of the synchrotron radiation permits the measurements of time-of-flight (TOF) spectra of Auger and photoelectrons, thereby increasing the electron collection efficiency. The double-angle TOF method yielded angle-resolved photoelectron intensities, which were used to determine photoionization cross sections and photoelectron angular distributions in several cases. Comparison to theoretical calculations has been made where possible to help explain observed phenomena in terms of the electronic structure and photoionization dynamics of the systems studied. 154 references, 23 figures, 7 tables.

  16. Li induced effects in the core level and π-band electronic structure of graphene grown on C-face SiC

    SciTech Connect

    Johansson, Leif I. Xia, Chao; Virojanadara, Chariya

    2015-11-15

    Studies of the effects induced in the electronic structure after Li deposition, and subsequent heating, on graphene samples prepared on C-face SiC are reported. The as prepared graphene samples are essentially undoped, but after Li deposition, the Dirac point shifts down to 1.2 eV below the Fermi level due to electron doping. The shape of the C 1s level also indicates a doping concentration of around 10{sup 14 }cm{sup −2} after Li deposition, when compared with recent calculated results of core level spectra of graphene. The C 1s, Si 2p, and Li 1s core level results show little intercalation directly after deposition but that most of the Li has intercalated after heating at 280 °C. Heating at higher temperatures leads to desorption of Li from the sample, and at 1030 °C, Li can no longer be detected on the sample. The single π-band observable from multilayer C-face graphene samples in conventional angle resolved photoelectron spectroscopy is reasonably sharp both on the initially prepared sample and after Li deposition. After heating at 280 °C, the π-band appears more diffuse and possibly split. The Dirac point becomes located at 0.4 eV below the Fermi level, which indicates occurrence of a significant reduction in the electron doping concentration. Constant energy photoelectron distribution patterns extracted from the as prepared graphene C-face sample and also after Li deposition and heating at 280 °C look very similar to earlier calculated distribution patterns for monolayer graphene.

  17. Core level photoionization on free sub-10-nm nanoparticles using synchrotron radiation

    SciTech Connect

    Meinen, Jan; Leisner, Thomas; Khasminskaya, Svetlana; Eritt, Markus; Antonsson, Egill; Langer, Burkhard; Ruehl, Eckart

    2010-08-15

    A novel instrument is presented, which permits studies on singly charged free nanoparticles in the diameter range from 1 to 30 nm using synchrotron radiation in the soft x-ray regime. It consists of a high pressure nanoparticle source, a high efficiency nanoparticle beam inlet, and an electron time-of-flight spectrometer suitable for probing surface and bulk properties of free, levitated nanoparticles. We show results from x-ray photoelectron spectroscopy study near the Si L{sub 3,2}-edge on 8.2 nm SiO{sub 2} particles prepared in a nanoparticle beam. The possible use of this apparatus regarding chemical reactions on the surface of nanometer-sized particles is highlighted. This approach has the potential to be exploited for process studies on heterogeneous atmospheric chemistry.

  18. Induced photoemission from driven nonadiabatic dynamics in an avoided crossing system

    SciTech Connect

    Arasaki, Yasuki; Mizuno, Yuta; Takatsuka, Kazuo; Scheit, Simona

    2014-12-21

    When vibrational dynamics on an ionic state (large dipole moment) is coupled to that on a neutral state (small dipole moment) such as at an avoided crossing in the alkali halide system, the population transfer between the states cause oscillation of the molecular dipole, leading to dipole emission. Such dynamics may be driven by an external field. We study how the coupled wavepacket dynamics is affected by the parameters (intensity, frequency) of the driving field with the aim of making use of the photoemission as an alternative detection scheme of femtosecond and subfemtosecond vibrational and electronic dynamics or as a characteristic optical source.

  19. Doppler effect in resonant photoemission from SF6: correlation between Doppler profile and Auger emission anisotropy.

    PubMed

    Kitajima, M; Ueda, K; De Fanis, A; Furuta, T; Shindo, H; Tanaka, H; Okada, K; Feifel, R; Sorensen, S L; Gel'mukhanov, F; Baev, A; Agren, H

    2003-11-21

    Fragmentation of the SF6 molecule upon F 1s excitation has been studied by resonant photoemission. The F atomiclike Auger line exhibits the characteristic Doppler profile that depends on the direction of the photoelectron momentum relative to the polarization vector of the radiation as well as on the photon energy. The measured Doppler profiles are analyzed by the model simulation that takes account of the anisotropy of the Auger emission in the molecular frame. The Auger anisotropy extracted from the data decreases with an increase in the F-SF5 internuclear distance.

  20. Optical communication with two-photon coherent states. III - Quantum measurements realizable with photoemissive detectors

    NASA Technical Reports Server (NTRS)

    Yuen, H. P.; Shapiro, J. H.

    1980-01-01

    Homodyne detection is shown to achieve the same signal-to-noise ratio as the quantum field quadrature measurement, thus providing a receiver which realizes linear modulation TCS performance gain. The full equivalence of homodyne detection and single-quadrature field measurement is established. A heterodyne configuration which uses a TCS image-band oscillator in addition to the usual coherent state local oscillator is studied. Results are obtained by means of a representation theorem which shows that photoemissive detection realizes the photon flux density measurement.

  1. Design of electrostatic microcolumn for nanoscale photoemission source in massively parallel electron-beam lithography

    NASA Astrophysics Data System (ADS)

    Wen, Ye; Du, Zhidong; Pan, Liang

    2015-10-01

    Microcolumns are widely used for parallel electron-beam lithography because of their compactness and the ability to achieve high spatial resolution. A design of an electrostatic microcolumn for our recent nanoscale photoemission sources is presented. We proposed a compact column structure (as short as several microns in length) for the ease of microcolumn fabrication and lithography operation. We numerically studied the influence of several design parameters on the optical performance such as microcolumn diameter, electrode thickness, beam current, working voltages, and working distance. We also examined the effect of fringing field between adjacent microcolumns during parallel lithography operations.

  2. An innovative Yb-based ultrafast deep ultraviolet source for time-resolved photoemission experiments.

    PubMed

    Boschini, F; Hedayat, H; Dallera, C; Farinello, P; Manzoni, C; Magrez, A; Berger, H; Cerullo, G; Carpene, E

    2014-12-01

    Time- and angle-resolved photoemission spectroscopy is a powerful technique to study ultrafast electronic dynamics in solids. Here, an innovative optical setup based on a 100-kHz Yb laser source is presented. Exploiting non-collinear optical parametric amplification and sum-frequency generation, ultrashort pump (hν = 1.82 eV) and ultraviolet probe (hν = 6.05 eV) pulses are generated. Overall temporal and instrumental energy resolutions of, respectively, 85 fs and 50 meV are obtained. Time- and angle-resolved measurements on BiTeI semiconductor are presented to show the capabilities of the setup. PMID:25554305

  3. An innovative Yb-based ultrafast deep ultraviolet source for time-resolved photoemission experiments

    SciTech Connect

    Boschini, F.; Hedayat, H.; Dallera, C.; Cerullo, G.; Farinello, P.; Manzoni, C.; Carpene, E.; Magrez, A.; Berger, H.

    2014-12-15

    Time- and angle-resolved photoemission spectroscopy is a powerful technique to study ultrafast electronic dynamics in solids. Here, an innovative optical setup based on a 100-kHz Yb laser source is presented. Exploiting non-collinear optical parametric amplification and sum-frequency generation, ultrashort pump (hν = 1.82 eV) and ultraviolet probe (hν = 6.05 eV) pulses are generated. Overall temporal and instrumental energy resolutions of, respectively, 85 fs and 50 meV are obtained. Time- and angle-resolved measurements on BiTeI semiconductor are presented to show the capabilities of the setup.

  4. Role of Strong Correlation in the Recent Angle-Resolved Photoemission Spectroscopy Experiments on Cuprate Superconductors

    SciTech Connect

    Yunoki, S.; Dagotto, Elbio R; Sorella, S.

    2005-01-01

    Motivated by recent photoemission experiments on cuprates, the low-lying excitations of a strongly correlated superconducting state are studied numerically. It is observed that along the nodal direction these low-lying one-particle excitations show a linear momentum dependence for a wide range of excitation energies and, thus, they do not present a kinklike structure. The nodal Fermi velocity vF, as well as other observables, are systematically evaluated directly from the calculated dispersions, and they are found to compare well with experiments. It is argued that the parameter dependence of v{sub F} is quantitatively explained by a simple picture of a renormalized Fermi velocity.

  5. Two-photon Photo-emission of Ultrathin Film PTCDA Morphologies on Ag(111)

    SciTech Connect

    Yang, Aram; Yang, Aram; Shipman, Steven T.; Garrett-Roe, Sean; Johns, James; Strader, Matt; Szymanski, Paul; Muller, Eric; Harris, Charles B.

    2007-11-29

    Morphology- and layer-dependent electronic structure and dynamics at the PTCDA/Ag(111) interface have been studied with angle-resolved two-photon photoemission. In Stranski-Krastanov growth modes, the exposed wetting layer inhibited the evolution of the vacuum level and valence band to bulk values. For layer-by-layer growth, we observed the transition of electron structure from monolayer to bulk values within eight monolayers. Effective masses and lifetimes of the conduction band and the n=1 image potential state were measured to be larger for disordered layers. The effective mass was interpreted in the context of charge mobility measurements.

  6. Electron attachment rate constant measurement by photoemission electron attachment ion mobility spectrometry (PE-EA-IMS)

    NASA Astrophysics Data System (ADS)

    Su, Desheng; Niu, Wenqi; Liu, Sheng; Shen, Chengyin; Huang, Chaoqun; Wang, Hongmei; Jiang, Haihe; Chu, Yannan

    2012-12-01

    Photoemission electron attachment ion mobility spectrometry (PE-EA-IMS), with a source of photoelectrons induced by vacuum ultraviolet radiation on a metal surface, has been developed to study electron attachment reaction at atmospheric pressure using nitrogen as the buffer gas. Based on the negative ion mobility spectra, the rate constants for electron attachment to tetrachloromethane and chloroform were measured at ambient temperature as a function of the average electron energy in the range from 0.29 to 0.96 eV. The experimental results are in good agreement with the data reported in the literature.

  7. Interference of fluorescence x-rays and coherent excitation of core levels

    SciTech Connect

    Ma, Y. |; Blume, M.

    1994-08-01

    The question of coherence in inelastic x-ray absorption and fluorescence processes among identical interacting atoms is studied using a simple diatomic model. Conditions for the coherence are discussed in terms of energy scales, such as the core hole life-time, instrument energy resolutions, and the splitting of the electronic levels. As in the classical Young double-slit experiment, the primary requirement is that it be impossible to determine which atom has undergone the excitation-decay process.

  8. Site-specific fragmentation caused by core-level photoionization: Effect of chemisorption

    NASA Astrophysics Data System (ADS)

    Nagaoka, Shin-ichi; Mase, Kazuhiko; Nakamura, Arinobu; Nagao, Masashi; Yoshinobu, Jun; Tanaka, Shin-ichiro

    2002-08-01

    We used the energy-selected-photoelectron photoion coincidence (ESPEPICO) method to study site-specific fragmentation caused by C:1s photoionization of 1,1,1-trifluoro-2-propanol-d1 [CF3)CD(OHCH3, TFIP-d1] on a Si(100) surface. High-resolution electron energy loss spectroscopy showed that TFIP-d1 is dissociatively chemisorbed like (CF3)(CH3))CDO-Si(100, and different chemical shifts at the three carbon sites were observed by photoelectron spectroscopy. The site-specific fragmentation evident in the ESPEPICO spectra of the sub-monolayer at room temperature indicates that the TFIP-d1 there has an O-Si bond oriented in the trans position with respect to the C-CF3 bond. Here we discuss the fragmentation processes in light of the results obtained with the ESPEPICO method and the Auger-electron photoion coincidence method.

  9. Photoemission from Ag, Cu, and CsI

    SciTech Connect

    Srinivasan-Rao, T.; Fischer, J.; Tsang, T.

    1992-06-01

    Photoemission characteristics of three different cathodes, CsI, Ag film and Cu were investigated. CsI, upon irradiation by 213 nm, 10ps laser pulse yields a quantum efficiency of 4% at O.2{mu}J input energy. The saturation mechanism observed at higher input energies require further investigation. Ag film, upon irradiation by 630 nm, 300 fs laser emit prompt photoelectrons after absorbing 2 photons. There was no evidence of optical damage of the film up to 10{sup 11} W/cm{sup 2}. At low intensities, photoemission from Cu is a simple {nu}-e{sup {minus}} interaction, the nonlinearity of the process depending strongly on trace impurities. At higher intensities, there appears to be a change in the emission mechanism.

  10. Generalized Franck-Condon principle for resonant photoemission

    NASA Astrophysics Data System (ADS)

    Sałek, Paweł; Gel'mukhanov, Faris; Ågren, Hans; Björneholm, Olle; Svensson, Svante

    1999-10-01

    A generalized Franck-Condon (GFC) principle for resonant x-ray Raman scattering and for resonant photoemission in particular is derived and numerically investigated. The GFC amplitudes differ from ordinary FC amplitudes by the presence of photon and photoelectron phase factors which describe the coupling-or interference-of the x-ray photons or Auger electrons with the nuclear motion. With the GFC amplitudes, a Kramers-Heisenberg relation is obtained for vibronic transitions that corrects the so-called lifetime-vibrational interference formula. For resonant photoemission in the soft-x-ray region involving typical bound potential surfaces, the generalization gives a contribution to the FC factors that can amount to 20%. For core excitation above the dissociation threshold, the GFC principle relates to Doppler effects on the ejected photoelectron both for the so-called ``molecular'' and ``atomic'' bands. The role of the GFC principle in direct photoionization is briefly discussed.

  11. Experimental setup for high energy photoemission using synchrotron radiation

    SciTech Connect

    Torelli, P.; Sacchi, M.; Cautero, G.; Cautero, M.; Krastanov, B.; Lacovig, P.; Pittana, P.; Sergo, R.; Tommasini, R.; Fondacaro, A.; Offi, F.; Paolicelli, G.; Stefani, G.; Grioni, M.; Verbeni, R.; Monaco, G.; Panaccione, G.

    2005-02-01

    The instrument VOLPE (volume photoemission from solids) is an experimental setup dedicated to high energy photoemission (PE) experiments. The instrument is equipped with an electrostatic hemispherical spectrometer especially designed to analyze high energy electrons (up to 10 keV) with high resolving power. In order to attain an energy resolution of a few tens of millielectron volts, we designed and constructed a dedicated input lens system, high stability power supplies, and a low dark-count detector and readout electronics. The system has been tested and is now operational on the ID16 beamline at European Synchrotron Radiation Facility, where an optical layout has been developed to perform high energy, high resolution PE experiments. First results show an overall energy resolution (electron + photon) of 71{+-}7 meV at 5934 eV. The effective attenuation length of the photoelectrons is estimated to be 5{+-}0.5 nm at a kinetic energy of 5 keV.

  12. Core level regulatory network of osteoblast as molecular mechanism for osteoporosis and treatment

    PubMed Central

    Zhu, Xiaomei; Li, Jun; Liang, Yuhong; Liu, Tao; Zhu, Yanxia; Zhang, Bingbing; Tan, Shuang; Guo, Huajie; Guan, Shuguang; Ao, Ping; Zhou, Guangqian

    2016-01-01

    To develop and evaluate the long-term prophylactic treatment for chronic diseases such as osteoporosis requires a clear view of mechanism at the molecular and systems level. While molecular signaling pathway studies for osteoporosis are extensive, a unifying mechanism is missing. In this work, we provide experimental and systems-biology evidences that a tightly connected top-level regulatory network may exist, which governs the normal and osteoporotic phenotypes of osteoblast. Specifically, we constructed a hub-like interaction network from well-documented cross-talks among estrogens, glucocorticoids, retinoic acids, peroxisome proliferator-activated receptor, vitamin D receptor and calcium-signaling pathways. The network was verified with transmission electron microscopy and gene expression profiling for bone tissues of ovariectomized (OVX) rats before and after strontium gluconate (GluSr) treatment. Based on both the network structure and the experimental data, the dynamical modeling predicts calcium and glucocorticoids signaling pathways as targets for GluSr treatment. Modeling results further reveal that in the context of missing estrogen signaling, the GluSr treated state may be an outcome that is closest to the healthy state. PMID:26783964

  13. Core-level spectra and molecular deformation in adsorption: V-shaped pentacene on Al(001).

    PubMed

    Baby, Anu; Lin, He; Brivio, Gian Paolo; Floreano, Luca; Fratesi, Guido

    2015-01-01

    By first-principle simulations we study the effects of molecular deformation on the electronic and spectroscopic properties as it occurs for pentacene adsorbed on the most stable site of Al(001). The rationale for the particular V-shaped deformed structure is discussed and understood. The molecule-surface bond is made evident by mapping the charge redistribution. Upon X-ray photoelectron spectroscopy (XPS) from the molecule, the bond with the surface is destabilized by the electron density rearrangement to screen the core hole. This destabilization depends on the ionized carbon atom, inducing a narrowing of the XPS spectrum with respect to the molecules adsorbed hypothetically undistorted, in full agreement to experiments. When looking instead at the near-edge X-ray absorption fine structure (NEXAFS) spectra, individual contributions from the non-equivalent C atoms provide evidence of the molecular orbital filling, hybridization, and interchange induced by distortion. The alteration of the C-C bond lengths due to the V-shaped bending decreases by a factor of two the azimuthal dichroism of NEXAFS spectra, i.e., the energy splitting of the sigma resonances measured along the two in-plane molecular axes.

  14. Core-level spectra and molecular deformation in adsorption: V-shaped pentacene on Al(001)

    PubMed Central

    Lin, He; Brivio, Gian Paolo; Floreano, Luca; Fratesi, Guido

    2015-01-01

    Summary By first-principle simulations we study the effects of molecular deformation on the electronic and spectroscopic properties as it occurs for pentacene adsorbed on the most stable site of Al(001). The rationale for the particular V-shaped deformed structure is discussed and understood. The molecule–surface bond is made evident by mapping the charge redistribution. Upon X-ray photoelectron spectroscopy (XPS) from the molecule, the bond with the surface is destabilized by the electron density rearrangement to screen the core hole. This destabilization depends on the ionized carbon atom, inducing a narrowing of the XPS spectrum with respect to the molecules adsorbed hypothetically undistorted, in full agreement to experiments. When looking instead at the near-edge X-ray absorption fine structure (NEXAFS) spectra, individual contributions from the non-equivalent C atoms provide evidence of the molecular orbital filling, hybridization, and interchange induced by distortion. The alteration of the C–C bond lengths due to the V-shaped bending decreases by a factor of two the azimuthal dichroism of NEXAFS spectra, i.e., the energy splitting of the sigma resonances measured along the two in-plane molecular axes. PMID:26734516

  15. Core level regulatory network of osteoblast as molecular mechanism for osteoporosis and treatment.

    PubMed

    Yuan, Ruoshi; Ma, Shengfei; Zhu, Xiaomei; Li, Jun; Liang, Yuhong; Liu, Tao; Zhu, Yanxia; Zhang, Bingbing; Tan, Shuang; Guo, Huajie; Guan, Shuguang; Ao, Ping; Zhou, Guangqian

    2016-01-26

    To develop and evaluate the long-term prophylactic treatment for chronic diseases such as osteoporosis requires a clear view of mechanism at the molecular and systems level. While molecular signaling pathway studies for osteoporosis are extensive, a unifying mechanism is missing. In this work, we provide experimental and systems-biology evidences that a tightly connected top-level regulatory network may exist, which governs the normal and osteoporotic phenotypes of osteoblast. Specifically, we constructed a hub-like interaction network from well-documented cross-talks among estrogens, glucocorticoids, retinoic acids, peroxisome proliferator-activated receptor, vitamin D receptor and calcium-signaling pathways. The network was verified with transmission electron microscopy and gene expression profiling for bone tissues of ovariectomized (OVX) rats before and after strontium gluconate (GluSr) treatment. Based on both the network structure and the experimental data, the dynamical modeling predicts calcium and glucocorticoids signaling pathways as targets for GluSr treatment. Modeling results further reveal that in the context of missing estrogen signaling, the GluSr treated state may be an outcome that is closest to the healthy state. PMID:26783964

  16. The Origin of the Monochromatic Photoemission Peak in Diamondoid Monolayers

    SciTech Connect

    Clay, William A.; Liu, Zhi; Yang, Wanli; Fabbri, Jason D.; Dahl, Jeremy E.; Carlson, Robert M.K.; Sun, Steven; Pianetta, Piero A.; Melosh, Nicholas; Shen, Zhi-Xun; /Stanford U., Geballe Lab. /LBNL, ALS /Chevron Petroleum Tech., Richmond /SLAC, SSRL

    2008-10-31

    Recent photoemission experiments have discovered a highly monochromatized secondary electron peak emitted from diamondoid self-assembled monolayers on metal substrates. New experimental data and simulation results are presented to show that a combination of negative electron affinity and strong electron-phonon scattering is responsible for this behavior. The simulation results are generated using a simple Monte Carlo transport algorithm. The simulated spectra contain the main spectral features of the measured ones.

  17. Tetragonal and collapsed-tetragonal phases of CaFe2As2 : A view from angle-resolved photoemission and dynamical mean-field theory

    NASA Astrophysics Data System (ADS)

    van Roekeghem, Ambroise; Richard, Pierre; Shi, Xun; Wu, Shangfei; Zeng, Lingkun; Saparov, Bayrammurad; Ohtsubo, Yoshiyuki; Qian, Tian; Sefat, Athena S.; Biermann, Silke; Ding, Hong

    2016-06-01

    We present a study of the tetragonal to collapsed-tetragonal transition of CaFe2As2 using angle-resolved photoemission spectroscopy and dynamical mean field theory-based electronic structure calculations. We observe that the collapsed-tetragonal phase exhibits reduced correlations and a higher coherence temperature due to the stronger Fe-As hybridization. Furthermore, a comparison of measured photoemission spectra and theoretical spectral functions shows that momentum-dependent corrections to the density functional band structure are essential for the description of low-energy quasiparticle dispersions. We introduce those using the recently proposed combined "screened exchange + dynamical mean field theory" scheme.

  18. Time- and angle-resolved photoemission spectroscopy of hydrated electrons near a liquid water surface.

    PubMed

    Yamamoto, Yo-ichi; Suzuki, Yoshi-Ichi; Tomasello, Gaia; Horio, Takuya; Karashima, Shutaro; Mitríc, Roland; Suzuki, Toshinori

    2014-05-01

    We present time- and angle-resolved photoemission spectroscopy of trapped electrons near liquid surfaces. Photoemission from the ground state of a hydrated electron at 260 nm is found to be isotropic, while anisotropic photoemission is observed for the excited states of 1,4-diazabicyclo[2,2,2]octane and I- in aqueous solutions. Our results indicate that surface and subsurface species create hydrated electrons in the bulk side. No signature of a surface-bound electron has been observed.

  19. Time- and Angle-Resolved Photoemission Spectroscopy of Hydrated Electrons Near a Liquid Water Surface

    NASA Astrophysics Data System (ADS)

    Yamamoto, Yo-ichi; Suzuki, Yoshi-Ichi; Tomasello, Gaia; Horio, Takuya; Karashima, Shutaro; Mitríc, Roland; Suzuki, Toshinori

    2014-05-01

    We present time- and angle-resolved photoemission spectroscopy of trapped electrons near liquid surfaces. Photoemission from the ground state of a hydrated electron at 260 nm is found to be isotropic, while anisotropic photoemission is observed for the excited states of 1,4-diazabicyclo[2,2,2]octane and I- in aqueous solutions. Our results indicate that surface and subsurface species create hydrated electrons in the bulk side. No signature of a surface-bound electron has been observed.

  20. High resolution photoemission experiments on copper oxide superconductors

    NASA Astrophysics Data System (ADS)

    Rameau, Jonathan David

    The mechanism for achieving high transition temperatures (T c) in copper oxide superconductors and the nature of the mysterious "pseudogap" phase from which this phenomenon arises are two of the most pressing issues in solid state physics. High resolution angle resolved photoemission spectroscopy (ARPES), which can directly probe the momentum and energy dependence of the electronic structure of a crystal, is considered one of the foremost tools for unraveling these mysteries. In this thesis we present work on both the further development of the ARPES technique itself and the results of two experiments on the high temperature superconductor Bi2Sr2CaCu2O8+delta (BSCCO)---the drosophila of copper oxide superconductors---based upon these analytical and experimental advances. On the analytical side we have shown that the precision of any ARPES experiment can be radically enhanced by using the Lucy-Richardson method (LRM) of iterative deconvolution to remove the worst effects of experimental resolution broadening present in all ARPES spectra. On the experimental side we have constructed a deep ultraviolet laser system capable of increasing our data acquisition rate by more than an order of magnitude compared to what is possible using traditional synchrotron radiation sources at the same momentum and energy resolutions. Using the LRM, in conjunction with synchrotron radiation, spectroscopic evidence was found for the existence of incoherent Cooper pairs in underdoped BSCCO in the normal pseudogap state (above Tc). At the same time an asymmetry between the particle and hole states of BSCCO was found, implying that doped Mott insulators, of which BSCCO is a primordial example, are characterized by the presence of a Fermi-Luttinger surface, rather than a Fermi surface, as would be the case for a simple metal. This study provided the first spectroscopic evidence for either phenomenon. In our second experiment we were able to use the LRM on data acquired with the laser ARPES

  1. Synchrotron Radiation Photoemission Spectroscopic Study of Band Offsets and Interface Self-cleaning by Atomic Layer Deposited HfO2 on In0.53Ga0.47As and In0.52Al0.48As

    SciTech Connect

    Kobayashi, Masaharu; Chen, P.T.; Sun, Y.; Goel, N.; Majhi, P.; Garner, M; Tsai, W.; Pianetta, P.; Nishi, Y.; /SLAC, SSRL

    2008-10-31

    The Synchrotron Radiation Photoemission Spectroscopic (SRPES) study was conducted to (a) investigate the surface chemistry of In{sub 0.53}Ga{sub 0.47}As and In{sub 0.52}Al{sub 0.48}As post chemical and thermal treatments, (b) construct band diagram and (c) investigate the interface property of HfO{sub 2}/In{sub 0.53}Ga{sub 0.47}As and HfO{sub 2}/In{sub 0.52}Al{sub 0.48}As. Dilute HCl and HF etch remove native oxides on In{sub 0.53}Ga{sub 0.47}As and In{sub 0.52}Al{sub 0.47}As, whereas in-situ vacuum annealing removes surface arsenic pile-up. After the atomic layer deposition of HfO{sub 2}, native oxides were considerably reduced compared to that in as-received epi-layers, strongly suggesting the self-clean mechanism. Valence and conduction band offsets are measured to be 3.37 {+-} 0.1eV, 1.80 {+-} 0.3eV for In{sub 0.53}Ga{sub 0.47}As and 3.00 {+-} 0.1eV, 1.47 {+-} 0.3eV for In{sub 0.52}Al{sub 0.47}As, respectively.

  2. Electronic structure of Ce2RhIn8: A two-dimensional heavy-fermion system studied by angle-resolved photoemission spectroscopy

    SciTech Connect

    Jiang, Rui; Mou, Daixing; Liu, Chang; Zhao, Xin; Yao, Yongxin; Ryu, Hyejin; Petrovic, C.; Ho, Kai -Ming; Kaminski, Adam

    2015-04-01

    We use angle-resolved photoemission spectroscopy (ARPES) to study the 2D heavy fermion superconductor, Ce₂RhIn₈. The Fermi surface is rather complicated and consists of several hole and electron pockets with one of the sheets displaying strong nesting properties with a q-vector of (0.32, 0.32) π/a. We do not observe kz dispersion of the Fermi sheets, which is consistent with the expected 2D character of the electronic structure. Comparison of the ARPES data to band structure calculations suggests that a localized picture of the f-electrons works best. While there is some agreement in the overall band dispersion and location of the Fermi sheets, the model does not reproduce all observed bands and is not completely accurate for those it does. As a result, our data paves the way for improving the band structure calculations and the general understanding of the transport and thermodynamical properties of this material.

  3. Interface states and internal photoemission in p-type GaAs metal-oxide-semiconductor surfaces

    NASA Technical Reports Server (NTRS)

    Kashkarov, P. K.; Kazior, T. E.; Lagowski, J.; Gatos, H. C.

    1983-01-01

    An interface photodischarge study of p-type GaAs metal-oxide-semiconductor (MOS) structures revealed the presence of deep interface states and shallow donors and acceptors which were previously observed in n-type GaAs MOS through sub-band-gap photoionization transitions. For higher photon energies, internal photoemission was observed, i.e., injection of electrons to the conduction band of the oxide from either the metal (Au) or from the GaAs valence band; the threshold energies were found to be 3.25 and 3.7 + or - 0.1 eV, respectively. The measured photoemission current exhibited a thermal activation energy of about 0.06 eV, which is consistent with a hopping mechanism of electron transport in the oxide.

  4. Systematics of the 4f energies in a series of rare-earth organic complexes determined by resonant photoemission

    NASA Astrophysics Data System (ADS)

    Thompson, J.; Arima, V.; Zou, Y.; Fink, R.; Umbach, E.; Cingolani, R.; Blyth, R. I. R.

    2004-10-01

    We report a photoemission study of the systematics of the 4f electronic structure of a family of rare-earth organic compounds. Resonant photoemission has been used to determine the binding energies of the 4fN-1 ground states, relative to those of the ligand orbitals, of a number of rare-earth tris-8-hydroxyquinolines ( REQ3 ’s). Using an empirical model these results have been extrapolated to the full series (Ce-Lu) of REQ3 ’s. It is found that in all cases, with the possible exception of Ce, the energy of the 4fN-1 ground state is less than that of the highest occupied molecular orbital, and therefore individual holes on lanthanide sites will not be stable.

  5. Recent Photoemission Results for the Electron-Doped Superconductors

    NASA Astrophysics Data System (ADS)

    Matsui, Hiroaki

    2006-03-01

    Recent improvement in the energy and angular resolution of angle-resolved photoemission spectroscopy (ARPES) enabled us to investigate the detailed electronic structure in electron-doped high-temperature superconductors (HTSC), which have a relatively smaller energy-scale of superconductivity compared to hole-doped systems. In this talk, we report our recent ARPES results1,2 focusing on the many-body interaction and the superconducting-gap symmetry in electron-doped HTSC. We have performed high-resolution ARPES measurements on Nd2-xCexCuO4 and observed that the quasiparticle (QP) effective mass around oπ sg&_slash;p is strongly enhanced due to opening of an antiferromagnetic (AF) pseudogap. Both the QP effective mass and the AF pseudogap are strongly anisotropic with the largest magnitude near the hot spot, which is defined as an intersection point of the Fermi surface and the AF zone boundary. Temperature-dependent measurements have revealed that the AF pseudogap survives at temperatures much higher than TN (N'{e}el temperature), possibly due to the short-range AF correlation remaining even above TN. The AF pseudogap gradually decreases with doping and is abruptly filled up near the boundary between the AF and superconducting phases. To study the anisotropy of superconducting gap in electron-doped HTSC, we have performed high-resolution ARPES on Pr0.89LaCe0.11CuO4. We observed that the momentum dependence of superconducting gap is basically consistent with the dx2-y2-wave symmetry, but it obviously deviates from the simple dx2-y2 gap function. The maximum superconducting gap is not observed at the zone boundary as expected from the simple dx2-y2 gap symmetry, but it is located around the hot spot where electrons are thought to be strongly coupled to the AF spin fluctuation. All these ARPES results suggest that the electronic stricture and the superconducting behavior are strongly dominated by the AF interaction in electron-doped HTSC. 1) H. Matsui, K. Terashima

  6. Probing the electronic and spintronic properties of buried interfaces by extremely low energy photoemission spectroscopy

    PubMed Central

    Fetzer, Roman; Stadtmüller, Benjamin; Ohdaira, Yusuke; Naganuma, Hiroshi; Oogane, Mikihiko; Ando, Yasuo; Taira, Tomoyuki; Uemura, Tetsuya; Yamamoto, Masafumi; Aeschlimann, Martin; Cinchetti, Mirko

    2015-01-01

    Ultraviolet photoemission spectroscopy (UPS) is a powerful tool to study the electronic spin and symmetry features at both surfaces and interfaces to ultrathin top layers. However, the very low mean free path of the photoelectrons usually prevents a direct access to the properties of buried interfaces. The latter are of particular interest since they crucially influence the performance of spintronic devices like magnetic tunnel junctions (MTJs). Here, we introduce spin-resolved extremely low energy photoemission spectroscopy (ELEPS) to provide a powerful way for overcoming this limitation. We apply ELEPS to the interface formed between the half-metallic Heusler compound Co2MnSi and the insulator MgO, prepared as in state-of-the-art Co2MnSi/MgO-based MTJs. The high accordance between the spintronic fingerprint of the free Co2MnSi surface and the Co2MnSi/MgO interface buried below up to 4 nm MgO provides clear evidence for the high interface sensitivity of ELEPS to buried interfaces. Although the absolute values of the interface spin polarization are well below 100%, the now accessible spin- and symmetry-resolved wave functions are in line with the predicted existence of non-collinear spin moments at the Co2MnSi/MgO interface, one of the mechanisms evoked to explain the controversially discussed performance loss of Heusler-based MTJs at room temperature. PMID:25702631

  7. Two-photon photoemission from image-potential states of epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Gugel, Dieter; Niesner, Daniel; Eickhoff, Christian; Wagner, Stefanie; Weinelt, Martin; Fauster, Thomas

    2015-12-01

    Using angle- and time-resolved two-photon photoelectron spectroscopy we observe a single series of image-potential states of graphene on monolayer (MLG) and bilayer graphene (BLG) on SiC(0001). The first image-potential state on MLG (BLG) has a binding energy of 0.93 eV (0.84 eV). Lifetimes of the first three image-potential states of MLG are 9, 44 and 110 fs. On hydrogen-intercalated, quasi-freestanding graphene no unoccupied states are observed. We attribute this to the absence of occupied initial states for direct transitions into image-potential states at photon energies below the work function used in two-photon photoemission. The work function varies between 4.14 and 4.79 eV, but the vacuum level stays ∼4.5 eV above the Dirac point for all surfaces studied. This finding suggests that direct excitation of image-potential states cannot be achieved by doping and the electron dynamics for free-standing graphene is not accessible by two-photon photoemission using photon energies below the work function.

  8. Rotatable spin-polarized electron source for inverse-photoemission experiments

    SciTech Connect

    Stolwijk, S. D. Wortelen, H.; Schmidt, A. B.; Donath, M.

    2014-01-15

    We present a ROtatable Spin-polarized Electron source (ROSE) for the use in spin- and angle-resolved inverse-photoemission (SR-IPE) experiments. A key feature of the ROSE is a variable direction of the transversal electron beam polarization. As a result, the inverse-photoemission experiment becomes sensitive to two orthogonal in-plane polarization directions, and, for nonnormal electron incidence, to the out-of-plane polarization component. We characterize the ROSE and test its performance on the basis of SR-IPE experiments. Measurements on magnetized Ni films on W(110) serve as a reference to demonstrate the variable spin sensitivity. Moreover, investigations of the unoccupied spin-dependent surface electronic structure of Tl/Si(111) highlight the capability to analyze complex phenomena like spin rotations in momentum space. Essentially, the ROSE opens the way to further studies on complex spin-dependent effects in the field of surface magnetism and spin-orbit interaction at surfaces.

  9. Modeling Photoemission of Spin-Polarized Electrons from NEA GaAs Photocathodes

    NASA Astrophysics Data System (ADS)

    Chubenko, Oksana; Afanasev, Andrei

    2015-04-01

    At present, photoemission from strained GaAs activated to negative electron affinity (NEA) is a main source of polarized electrons for modern nuclear-physics and particle-physics facilities. Future experiments at advanced electron colliders will require high-current polarized electron beams, which could provide high polarization and luminosity. This sets new requirements for photocathodes in terms of high quantum efficiency (QE) (>>1%) and spin polarization (~85%). Detailed simulation and modeling of physics processes in photocathodes is important for optimization of their design in order to achieve high QE and reduce depolarization mechanisms. The purpose of the present work was to develop a semi-phenomenological model, which could predict photoemission and electron spin polarization from NEA GaAs photocathodes. Effect of the presence of nanostructures was also studied. Simulation results were compared to the experimental results obtained by the polarized electron source group at Thomas Jefferson National Accelerator Facility. Work supported by Thomas Jefferson Accelerator Facility and George Washington University.

  10. Probing the electronic and spintronic properties of buried interfaces by extremely low energy photoemission spectroscopy.

    PubMed

    Fetzer, Roman; Stadtmüller, Benjamin; Ohdaira, Yusuke; Naganuma, Hiroshi; Oogane, Mikihiko; Ando, Yasuo; Taira, Tomoyuki; Uemura, Tetsuya; Yamamoto, Masafumi; Aeschlimann, Martin; Cinchetti, Mirko

    2015-01-01

    Ultraviolet photoemission spectroscopy (UPS) is a powerful tool to study the electronic spin and symmetry features at both surfaces and interfaces to ultrathin top layers. However, the very low mean free path of the photoelectrons usually prevents a direct access to the properties of buried interfaces. The latter are of particular interest since they crucially influence the performance of spintronic devices like magnetic tunnel junctions (MTJs). Here, we introduce spin-resolved extremely low energy photoemission spectroscopy (ELEPS) to provide a powerful way for overcoming this limitation. We apply ELEPS to the interface formed between the half-metallic Heusler compound Co2MnSi and the insulator MgO, prepared as in state-of-the-art Co2MnSi/MgO-based MTJs. The high accordance between the spintronic fingerprint of the free Co2MnSi surface and the Co2MnSi/MgO interface buried below up to 4 nm MgO provides clear evidence for the high interface sensitivity of ELEPS to buried interfaces. Although the absolute values of the interface spin polarization are well below 100%, the now accessible spin- and symmetry-resolved wave functions are in line with the predicted existence of non-collinear spin moments at the Co2MnSi/MgO interface, one of the mechanisms evoked to explain the controversially discussed performance loss of Heusler-based MTJs at room temperature.

  11. Ce Core-Level Spectroscopy, and Magnetic and Electrical Transport Properties of Lightly Ce-Doped YCoO3

    NASA Astrophysics Data System (ADS)

    Kobayashi, Yoshihiko; Koike, Tsuyoshi; Okawa, Mario; Takayanagi, Ryohei; Takei, Shohei; Minohara, Makoto; Kobayashi, Masaki; Horiba, Koji; Kumigashira, Hiroshi; Yasui, Akira; Ikenaga, Eiji; Saitoh, Tomohiko; Asai, Kichizo

    2016-11-01

    We have investigated the Ce and Co core level spectroscopy, and the magnetic and electrical transport properties of lightly Ce-doped YCoO3. We have successfully synthesized single-phase Y1-xCexCoO3 for 0.0 ≤ x ≤ 0.1 by the sol-gel method. Hard X-ray photoelectron and X-ray absorption spectroscopy experiments reveal that the introduced Ce ions are tetravalent, which is considered to be the first case of electron doping into bulk trivalent Co oxides with perovskite RECoO3 (RE: rare-earth element or Y) caused by RE site substitution. The magnitude of the effective magnetic moment peff obtained from the temperature dependence of magnetic susceptibility χ(T) at higher temperatures is close to that for high-spin Co2+ introduced by the Ce doping, implying that the electrons doped into the Co site induce Co2+ with a high-spin state. For x = 0.1, ferromagnetic ordering is observed below about 7 K. Electrical transport properties such as resistivity and thermoelectric power show that negative electron-like carriers are introduced by Ce substitution.

  12. Skin-depth lattice strain, core-level trap depression and valence charge polarization of Al surfaces

    NASA Astrophysics Data System (ADS)

    Wang, Yan; Bo, Maolin; Liu, Yonghui; Guo, Yongling; Wang, Haibin; Yue, Jian; Huang, Yongli

    2016-01-01

    Clarifying the origin for surface core-level shift (SCLS) and gaining quantitative information regarding the coordination-resolved local strain, binding energy (BE) shift and cohesive energy change have been a challenge. Here, we show that a combination of the bond order-length-strength (BOLS) premise, X-ray photoelectron spectroscopy (XPS) and the ab initio density functional theory (DFT) calculations of aluminum (Al) 2p3/2 energy shift of Al surfaces has enabled us to derive such information, namely, (i) the 2p3/2 energy of an isolated Al atom (72.146 ± 0.003eV) and its bulk shift (0.499 eV); (ii) the skin lattice contracts by up to 12.5% and the BE density increases by 70%; and (iii) the cohesive energy drops up to 38%. It is affirmed that the shorter and stronger bonds between under-coordinated atoms provide a perturbation to the Hamiltonian and hence lead to the local strain, quantum entrapment and valence charge polarization. Findings should help in understanding the phenomena of surface pre-melting and skin-high elasticity, in general.

  13. Photoemission spectra of charge density wave states in cuprates

    NASA Astrophysics Data System (ADS)

    Tu, Wei-Lin; Chen, Peng-Jen; Lee, Ting-Kuo

    Angle-resolved photoemission spectroscopy(ARPES) experiments have reported many exotic properties of cuprates, such as Fermi arc at normal state, two gaps at superconducting state and particle-hole asymmetry at the antinodal direction. On the other hand, a number of inhomogeneous states or so-called charge density waves(CDW) states have also been discovered in cuprates by many experimental groups. The relation between these CDW states and ARPES spectra is unclear. With the help of Gutzwiller projected mean-field theory, we can reproduce the quasiparticle spectra in momentum space. The spectra show strong correspondence to the experimental data with afore-mentioned exotic features in it.

  14. Resonant photoemission of oxidized Yb: Experiment and theory

    NASA Astrophysics Data System (ADS)

    Schmidt-May, J.; Gerken, F.; Nyholm, R.; Davis, L. C.

    1984-11-01

    The oxidation-induced valence change of Yb leads to a single 4f hole in the ground state. The creation of the 4f13 configuration which does not exist for any pure rare-earth metal makes it possible to analyze the 4d-->4f Fano resonance for a simple system experimentally as well as theoretically. Calculated Fano profiles for the 4f12 final-state multiplets are in good agreement with photoemission measurements taken with the FLIPPER monochromator at Hamburger Synchrotron-strahlungslabor, Deutsches Elektronen-Synchrotron, using synchrotron radiation from the storage ring DORIS.

  15. Photon Detector For Inverse Photoemission Spectroscopy With Improved Energy Resolution

    SciTech Connect

    Maniraj, M.; D'Souza, S. W.; Barman, S. R.

    2011-07-15

    We present the results from newly designed and fabricated double window photon detector to improve the overall energy resolution for inverse photoemission spectroscopy (IPES). This simple design allows us to introduce an absorption gas (Krypton) to decrease the band-width of the energy selective photon detector and thus improve the resolution. Resonance absorption line of Kr of wavelength of 123.6 nm was used. By fitting the Fermi edge of the IPES spectrum of silver, we find an overall energy resolution improved by 73 meV. The design is modular and ensures ease and safety of handling.

  16. Core-level positive-ion and negative-ion fragmentation of gaseous and condensed HCCl3 using synchrotron radiation

    NASA Astrophysics Data System (ADS)

    Lu, K. T.; Chen, J. M.; Lee, J. M.; Haw, S. C.; Liang, Y. C.; Deng, M. J.

    2011-07-01

    We investigated the dissociation dynamics of positive-ion and negative-ion fragments of gaseous and condensed HCCl3 following photoexcitation of Cl 2p electrons to various resonances. Based on ab initio calculations at levels HF/cc-pVTZ and QCISD/6-311G*, the first doublet structures in Cl L-edge x-ray absorption spectrum of HCCl3 are assigned to transitions from the Cl (2P3/2,1/2) initial states to the 10a1* orbitals. The Cl 2p → 10a1* excitation of HCCl3 induces a significant enhancement of the Cl+ desorption yield in the condensed phase and a small increase in the HCCl+ yield in the gaseous phase. Based on the resonant photoemission of condensed HCCl3, excitations of Cl 2p electrons to valence orbitals decay predominantly via spectator Auger transitions. The kinetic energy distributions of Cl+ ion via the Cl 2p → 10a1* excitation are shifted to higher energy ˜0.2 eV and ˜0.1 eV relative to those via the Cl 2p → 10e* excitation and Cl 2p → shape resonance excitation, respectively. The enhancement of the yields of ionic fragments at specific core-excited resonance states is assisted by a strongly repulsive surface that is directly related to the spectator electrons localized in the antibonding orbitals. The Cl- anion is significantly reinforced in the vicinity of Cl 2p ionization threshold of gaseous HCCl3, mediated by photoelectron recapture through post-collision interaction.

  17. The influence of oxygen adsorption on the NEXAFS and core-level XPS spectra of the C{sub 60} derivative PCBM

    SciTech Connect

    Brumboiu, Iulia Emilia Eriksson, Olle; Brena, Barbara; Ericsson, Leif; Hansson, Rickard; Moons, Ellen

    2015-02-07

    Fullerenes have been a main focus of scientific research since their discovery due to the interesting possible applications in various fields like organic photovoltaics (OPVs). In particular, the derivative [6,6]-phenyl-C{sub 60}-butyric acid methyl ester (PCBM) is currently one of the most popular choices due to its higher solubility in organic solvents compared to unsubstituted C{sub 60}. One of the central issues in the field of OPVs is device stability, since modules undergo deterioration (losses in efficiency, open circuit voltage, and short circuit current) during operation. In the case of fullerenes, several possibilities have been proposed, including dimerization, oxidation, and impurity related deterioration. We have studied by means of density functional theory the possibility of oxygen adsorption on the C{sub 60} molecular moiety of PCBM. The aim is to provide guidelines for near edge X-ray absorption fine structure (NEXAFS) and X-ray photoelectron spectroscopy (XPS) measurements which can probe the presence of atomic or molecular oxygen on the fullerene cage. By analysing several configurations of PCBM with one or more adsorbed oxygen atoms, we show that a joint core level XPS and O1s NEXAFS investigation could be effectively used not only to confirm oxygen adsorption but also to pinpoint the bonding configuration and the nature of the adsorbate.

  18. Two-photon photoemission investigation of electronic and dynamical properties of alkali atoms adsorbed on noble metal surfaces

    NASA Astrophysics Data System (ADS)

    Sametoglu, Vahit

    We present a systematic time-resolved two-photon photoemission study of the electronic and dynamical properties of Li through Cs adsorbed on Cu(111) and Ag(111) surfaces. A fundamental problem in surface science is how to describe the electronic structure of a chemisorption interface based on the intrinsic properties of the interacting materials. Because of their simple s-electron structure, elements of the alkali atom group comprise paradigmatic adsorbates in many theories of chemisorption, whereas the complementary experimental studies are sparse and incomplete. Through a combination of spectroscopic and femtosecond time-resolved surface measurements, we are able to probe systematically the binding energies, symmetries, and electron and nuclear relaxation dynamics of the initially unoccupied alkali atom resonances. As a prelude, we study the two-photon photoemission process occurring at the bare Ag(111) surface. We develop a quantitative model for two-photon photoemission process, where the nonresonant and k-dependent two-photon absorption between the lower and upper sp-bands is modeled by the optical Bloch equations, and the angle-dependent intensities are described by the Fresnel equations. Our two-photon photoemission spectra of Li through Cs chemisorbed Cu(111) and Ag(111) surfaces reveal two resonances with the m = 0 and m = +/-1 symmetry ('m' is the projection of the orbital angular momentum 'l' onto the surface plane). For the m = 0 resonance, which is derived from the hybridization of the ns and npz orbitals of alkali atoms, we find a binding energy of 1.84--1.99 eV below the vacuum level, which is independent of the alkali atom period, and tunes with coverage in a universal manner. At 0.3--0.7 eV higher energy, we discover and identify the m = +/-1 resonance by its characteristic angular intensity distribution, which derives from the antisymmetry of the npx and npy orbitals. We implement a quantitative model for the alkali atom chemisorption based on the

  19. One-Step Model of Photoemission for Nonlocal Potentials

    NASA Astrophysics Data System (ADS)

    Potthoff, M.; Lachnitt, J.; Nolting, W.; Braun, J.

    1997-10-01

    The one-step model of valence-band photoemission and inverse photoemission from single-crystal surfaces is reformulated for generalized (nonlocal, complex and energy-dependent) potentials. Thereby, it becomes possible to account for self-energy corrections taken from many-body electronic-structure calculations. The original formulation due to Pendry and coworkers employs the KKR multiple-scattering theory for the calculation of the initial state. This prevents a straightforward generalization of the one-step model to nonlocal potentials. We therefore consider the Dyson equation which is set up within a muffin-tin-orbital representation as an alternative to obtain the initial-state Green function. This approach requires a revision of the transition-matrix elements which is carried out in detail. The final state is considered as a time-reversed LEED state as usual. The proposed generalization of the one-step model allows to distinguish between the bare photocurrent reflecting the (quasi-particle) band structure and the secondary effects due to the (dipole) selection rules and due to the wave-vector and energy dependence of the transition-matrix elements.

  20. The intrinsic electronic structure of bilayer manganites from Angle Resolved Photoemission

    NASA Astrophysics Data System (ADS)

    de Jong, Sanne; Kukreja, R.; Hossain, M. A.; Golden, M. S.; van Heumen, E.; Massee, F.; Huang, Y.; Boothroyd, A. T.; Pabhakaran, P.; Walter, A.; Bostwick, A.; Rotenberg, E.; Durr, H. A.

    2012-02-01

    The Colossal MagnetoResistant (CMR) manganites are one of the most studied condensed matter physics systems since decades. Yet, the mechanism behind the CMR effect and their electronic structure are still under hot debate. Recent angle resolved photoemission (ARPES) studies on the bilayer manganite La(2-2x)Sr(1+2x)Mn3O7, LSMO327, reported contradictory results [1]. Here we present an ARPES study unveiling the intrinsic k-- and temperature dependent electronic structure of LSMO327, while carefully steering away from the recently reported sample inhomogeneities [2] that have caused all the confusion. [4pt] [1] N. Mannella, Nature (2005); S. Sun Nature Phys. (2007); S. de Jong, PRB (2007)[0pt] [2] F. Massee, Nature Phys(2011)

  1. Dirac Fermions in graphene and graphite---a view from angle-resolved photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Zhou, Shuyun

    The research in graphene has exploded in the past few years, due to its intriguing physics as an emerging paradigm for relativistic condensed matter physics as well as its great promise for application in next generation electronics. Understanding the low energy electronic structure of graphene is fundamental as most of the intriguing properties of graphene arise from its peculiar electronic dispersion, which resembles that of relativistic Dirac Fermions. This thesis presents a detailed study of the low energy electronic structure of graphene and its related three dimensional material - graphite - by using angle-resolved photoemission spectroscopy (ARPES), a direct probe of the electronic structure. In particular, the evolution of the Dirac Fermions in graphene and graphite as well as the effect of impurities is the focus of this thesis. This thesis is organized as follows. The first chapter is an introduction of the electronic structure of graphene and graphite, and the specialty of Dirac fermions compared to quasiparticles in conventional condensed matter systems. Chapter 2 is an introduction of the techniques used throughout this thesis - angle resolved photoemission spectroscopy (ARPES), X-ray photoemission spectroscopy (XPS) and low energy electron microscopy (LEEM). Chapter 3 discusses the growth and characterization of epitaxial graphene on SiC wafers. Chapters 4 and 5 present the ARPES results on epitaxial graphene, the evolution of the low energy electronic dynamics as a function of sample thickness and how to make graphene a finite band gap semiconductor. More specifically, chapter 4 discusses how a gap is induced between the valence and conduction bands by graphene-substrate interaction and chapter 6 shows how a reversible metal-insulator transition can be possibly induced in epitaxial graphene by hole doping. Chapters 6 and 7 show the ARPES results on three dimensional graphite samples. Chapter 6 shows the coexistence of Dirac fermions with massive

  2. Revisiting photoemission and inverse photoemission spectra of nickel oxide from first principles: implications for solar energy conversion.

    PubMed

    Alidoust, Nima; Toroker, Maytal Caspary; Carter, Emily A

    2014-07-17

    We use two different ab initio quantum mechanics methods, complete active space self-consistent field theory applied to electrostatically embedded clusters and periodic many-body G0W0 calculations, to reanalyze the states formed in nickel(II) oxide upon electron addition and ionization. In agreement with interpretations of earlier measurements, we find that the valence and conduction band edges consist of oxygen and nickel states, respectively. However, contrary to conventional wisdom, we find that the oxygen states of the valence band edge are localized whereas the nickel states at the conduction band edge are delocalized. We argue that these characteristics may lead to low electron-hole recombination and relatively efficient electron transport, which, coupled with band gap engineering, could produce higher solar energy conversion efficiency compared to that of other transition-metal oxides. Both methods find a photoemission/inverse-photoemission gap of 3.6-3.9 eV, in good agreement with the experimental range, lending credence to our analysis of the electronic structure of NiO.

  3. Revisiting Photoemission and Inverse Photoemission Spectra of Nickel Oxide from First Principles: Implications for Solar Energy Conversion

    SciTech Connect

    Alidoust, Nima; Toroker, Maytal; Carter, Emily A.

    2014-07-17

    We use two different ab initio quantum mechanics methods, complete active space self-consistent field theory applied to electrostatically embedded clusters and periodic many-body G₀W₀ calculations, to reanalyze the states formed in nickel(II) oxide upon electron addition and ionization. In agreement with interpretations of earlier measurements, we find that the valence and conduction band edges consist of oxygen and nickel states, respectively. However, contrary to conventional wisdom, we find that the oxygen states of the valence band edge are localized whereas the nickel states at the conduction band edge are delocalized. We argue that these characteristics may lead to low electron-hole recombination and relatively efficient electron transport, which, coupled with band gap engineering, could produce higher solar energy conversion efficiency compared to that of other transition-metal oxides. Both methods find a photoemission/inverse-photoemission gap of 3.6-3.9 eV, in good agreement with the experimental range, lending credence to our analysis of the electronic structure of NiO.

  4. Observation of strontium segregation in LaAlO{sub 3}/SrTiO{sub 3} and NdGaO{sub 3}/SrTiO{sub 3} oxide heterostructures by X-ray photoemission spectroscopy

    SciTech Connect

    Treske, Uwe; Heming, Nadine; Knupfer, Martin; Büchner, Bernd; Koitzsch, Andreas; Di Gennaro, Emiliano; Scotti di Uccio, Umberto; Miletto Granozio, Fabio; Krause, Stefan

    2014-01-01

    LaAlO{sub 3} and NdGaO{sub 3} thin films of different thicknesses have been grown by pulsed laser deposition on TiO{sub 2}-terminated SrTiO{sub 3} single crystals and investigated by soft X-ray photoemission spectroscopy. The surface sensitivity of the measurements has been tuned by varying photon energy hν and emission angle Θ. In contrast to the core levels of the other elements, the Sr 3d line shows an unexpected splitting for higher surface sensitivity, signaling the presence of a second strontium component. From our quantitative analysis we conclude that during the growth process Sr atoms diffuse away from the substrate and segregate at the surface of the heterostructure, possibly forming strontium oxide.

  5. Observation of strontium segregation in LaAlO3/SrTiO3 and NdGaO3/SrTiO3 oxide heterostructures by X-ray photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Treske, Uwe; Heming, Nadine; Knupfer, Martin; Büchner, Bernd; Koitzsch, Andreas; Di Gennaro, Emiliano; Scotti di Uccio, Umberto; Miletto Granozio, Fabio; Krause, Stefan

    2014-01-01

    LaAlO3 and NdGaO3 thin films of different thicknesses have been grown by pulsed laser deposition on TiO2-terminated SrTiO3 single crystals and investigated by soft X-ray photoemission spectroscopy. The surface sensitivity of the measurements has been tuned by varying photon energy hν and emission angle Θ. In contrast to the core levels of the other elements, the Sr 3d line shows an unexpected splitting for higher surface sensitivity, signaling the presence of a second strontium component. From our quantitative analysis we conclude that during the growth process Sr atoms diffuse away from the substrate and segregate at the surface of the heterostructure, possibly forming strontium oxide.

  6. Unoccupied electronic resonances of Sc adsorbed on W(001) by k-resolved inverse photoemission

    NASA Technical Reports Server (NTRS)

    Lamouri, A.; Krainsky, I. L.; Petukhov, A. G.; Lambrecht, W. R. L.; Segall, B.

    1995-01-01

    Scandium adsorbed on the (001) face of tungsten has been studied using Auger-electron spectroscopy, low-energy electron diffraction, k-resolved inverse photoelectron spectroscopy, work-function measurements, and relativistic-electronic-structure calculations. We find that the work function of W(001) does not decrease monotonically as a function of scandium adsorption but reaches a minimum value of Phi = 3.25 eV at 50% coverage. For a complete monolayer, an order 1 X 1 Sc overlayer is formed. Inverse photoemission in the isochromat mode was used to map the unoccupied energy levels of this overlayer along the bar-Gamma(bar-Mu) symmetry direction of the surface Brillouin zone. Local-density-functional calculations using the muffin-tin orbital method were performed for a 1 X 1 Sc overlayer on W and are compared with the experimental two-dimensional band structure.

  7. Spin- and angle-resolved photoemission on the topological Kondo insulator candidate: SmB6.

    PubMed

    Xu, Nan; Ding, Hong; Shi, Ming

    2016-09-14

    Topological Kondo insulators are a new class of topological insulators in which metallic surface states protected by topological invariants reside in the bulk band gap at low temperatures. Unlike other 3D topological insulators, a truly insulating bulk state, which is critical for potential applications in next-generation electronic devices, is guaranteed by many-body effects in the topological Kondo insulator. Furthermore, the system has strong electron correlations that can serve as a testbed for interacting topological theories. This topical review focuses on recent advances in the study of SmB6, the most promising candidate for a topological Kondo insulator, from the perspective of spin- and angle-resolved photoemission spectroscopy with highlights of some important transport results.

  8. X-ray photoemission electron microscopy, a tool for the investigation of complex magnetic structures.

    SciTech Connect

    Scholl, Andreas; Ohldag, Hendrik; Nolting, Frithjof; Stohr, Joachim; Padmore, Howard A.

    2001-08-30

    X-ray Photoemission Electron Microscopy unites the chemical specificity and magnetic sensitivity of soft x-ray absorption techniques with the high spatial resolution of electron microscopy. The discussed instrument possesses a spatial resolution of better than 50 nm and is located at a bending magnet beamline at the Advanced Light Source, providing linearly and circularly polarized radiation between 250 and 1300 eV. We will present examples which demonstrate the power of this technique applied to problems in the field of thin film magnetism. The chemical and elemental specificity is of particular importance for the study of magnetic exchange coupling because it allows separating the signal of the different layers and interfaces in complex multi-layered structures.

  9. Interband quasiparticle scattering in superconducting LiFeAs reconciles photoemission and tunneling measurements.

    PubMed

    Hess, Christian; Sykora, Steffen; Hänke, Torben; Schlegel, Ronny; Baumann, Danny; Zabolotnyy, Volodymyr B; Harnagea, Luminita; Wurmehl, Sabine; van den Brink, Jeroen; Büchner, Bernd

    2013-01-01

    Several angle-resolved photoemission spectroscopy (ARPES) studies reveal a poorly nested Fermi surface of LiFeAs, far away from a spin density wave instability, and clear-cut superconducting gap anisotropies. On the other hand a very different, more nested Fermi surface and dissimilar gap anisotropies have been obtained from quasiparticle interference (QPI) data, which were interpreted as arising from intraband scattering within holelike bands. Here we show that this ARPES-QPI paradox is completely resolved by interband scattering between the holelike bands. The resolution follows from an excellent agreement between experimental quasiparticle scattering data and T-matrix QPI calculations (based on experimental band structure data), which allows disentangling interband and intraband scattering processes.

  10. A brief update of angle-resolved photoemission spectroscopy on a correlated electron system

    SciTech Connect

    Lee, W.S.

    2010-02-24

    In this paper, we briefly summarize the capabilities of state-of-the-art angle-resolved photoemission spectroscopy (ARPES) in the field of experimental condensed matter physics. Due to the advancement of the detector technology and the high flux light sources, ARPES has become a powerful tool to study the low energy excitations of solids, especially those novel quantum materials in which many-body physics are at play. To benchmark today's state-of-the-art ARPES technique, we demonstrate that the precision of today's ARPES has advanced to a regime comparable to the bulk-sensitive de Haas-van Alphen (dHvA) measurements. Finally, as an example of new discoveries driven by the advancement of the ARPES technique, we summarize some of our recent ARPES measurements on underdoped high-T{sub c} superconducting cuprates, which have provided further insight into the complex pseudogap problem.

  11. Complete momentum and energy resolved TOF electron spectrometerfor time-resolved photoemission spectroscopy

    SciTech Connect

    Hussain, Zahid; Lebedev, G.; Tremsin, A.; Siegmund, O.; Chen, Y.; Shen, Z.X.; Hussain, Z.

    2007-08-12

    Over the last decade, high-resolution Angle-Resolved Photoemission Spectroscopy (ARPES) has emerged as a tool of choice for studying the electronic structure of solids, in particular, strongly correlated complex materials such as cuprate superconductors. In this paper we present the design of a novel time-of-flight based electron analyzer with capability of 2D in momentum space (kx and ky) and all energies (calculated from time of flight) in the third dimension. This analyzer will utilize an improved version of a 2D delay linedetector capable of imaging with<35 mm (700x700 pixels) spatial resolution and better than 120 ps FWHM timing resolution. Electron optics concepts and optimization procedure are considered for achieving an energy resolution less than 1 meV and an angular resolution better than 0.11.

  12. Imaging and characterization of conducting ferroelectric domain walls by photoemission electron microscopy

    SciTech Connect

    Schaab, J.; Meier, D.; Krug, I. P.; Nickel, F.; Gottlob, D. M.; Doğanay, H.; Schneider, C. M.; Cano, A.; Hentschel, M.; Yan, Z.; Bourret, E.; Ramesh, R.

    2014-06-09

    High-resolution X-ray photoemission electron microscopy (X-PEEM) is a well-established method for imaging ferroelectric domain structures. Here, we expand the scope of application of X-PEEM and demonstrate its capability for imaging and investigating domain walls in ferroelectrics with high spatial resolution. Using ErMnO{sub 3} as test system, we show that ferroelectric domain walls can be visualized based on photo-induced charging effects and local variations in their electronic conductance can be mapped by analyzing the energy distribution of photoelectrons. Our results open the door for non-destructive, contact-free, and element-specific studies of the electronic and chemical structure at domain walls in ferroelectrics.

  13. Spin- and angle-resolved photoemission on the topological Kondo insulator candidate: SmB6

    NASA Astrophysics Data System (ADS)

    Xu, Nan; Ding, Hong; Shi, Ming

    2016-09-01

    Topological Kondo insulators are a new class of topological insulators in which metallic surface states protected by topological invariants reside in the bulk band gap at low temperatures. Unlike other 3D topological insulators, a truly insulating bulk state, which is critical for potential applications in next-generation electronic devices, is guaranteed by many-body effects in the topological Kondo insulator. Furthermore, the system has strong electron correlations that can serve as a testbed for interacting topological theories. This topical review focuses on recent advances in the study of SmB6, the most promising candidate for a topological Kondo insulator, from the perspective of spin- and angle-resolved photoemission spectroscopy with highlights of some important transport results.

  14. Low energy electron microscopy and photoemission electron microscopy investigation of graphene

    NASA Astrophysics Data System (ADS)

    Man, K. L.; Altman, M. S.

    2012-08-01

    Low energy electron microscopy (LEEM) and photoemission electron microscopy (PEEM) are two powerful techniques for the investigation of surfaces, thin films and surface supported nanostructures. In this review, we examine the contributions of these microscopy techniques to our understanding of graphene in recent years. These contributions have been made in studies of graphene on various metal and SiC surfaces and free-standing graphene. We discuss how the real-time imaging capability of LEEM facilitates a deeper understanding of the mechanisms of dynamic processes, such as growth and intercalation. Numerous examples also demonstrate how imaging and the various available complementary measurement capabilities, such as selected area or micro low energy electron diffraction (μLEED) and micro angle resolved photoelectron spectroscopy (μARPES), allow the investigation of local properties in spatially inhomogeneous graphene samples.

  15. Magnetic linear dichroism of photoemission from ultrathin manganese films on silicon

    NASA Astrophysics Data System (ADS)

    Gomoyunova, M. V.; Grebenyuk, G. S.; Pronin, I. I.; Senkovskiy, B. V.

    2015-09-01

    The magnetic linear dichroism (MLD) effect in photoemission of Mn 3 p electrons was used to study magnetic properties of Mn films (to 2.5 nm thick) grown on the Si(111)-(7 × 7) surface at room temperature and manganese silicide films grown by solid-phase epitaxy. The experiments were performed using linearly polarized light with a photon energy of 130 eV, incident at an angle of 30° to the sample surface. Photoelectron spectra were measured in a narrow solid angle focused along the normal to the surface for two opposite sample magnetization directions in the surface plane, perpendicular to the polarization vector of the light wave. It was shown that the MLD effect characteristic of films with high-temperature ferromagnetism appears after depositing ˜2 nm Mn. The formation of manganese silicides upon annealings of the sample with deposited 2.5 nm Mn results in the disappearance of the MLD effect.

  16. An aberration corrected photoemission electron microscope at the advanced light source

    SciTech Connect

    Feng, J.; MacDowell, A.A.; Duarte, R.; Doran, A.; Forest, E.; Kelez, N.; Marcus, M.; Munson, D.; Padmore, H.; Petermann, K.; Raoux, S.; Robin, D.; Scholl, A.; Schlueter, R.; Schmid, P.; Stohr, J.; Wan, W.; Wei, D.H.; Wu, Y.

    2003-11-01

    Design of a new aberration corrected Photoemission electron microscope PEEM3 at the Advanced Light Source is outlined. PEEM3 will be installed on an elliptically polarized undulator beamline and will be used for the study of complex materials at high spatial and spectral resolution. The critical components of PEEM3 are the electron mirror aberration corrector and aberration-free magnetic beam separator. The models to calculate the optical properties of the electron mirror are discussed. The goal of the PEEM3 project is to achieve the highest possible transmission of the system at resolutions comparable to our present PEEM2 system (50 nm) and to enable significantly higher resolution, albeit at the sacrifice of intensity. We have left open the possibility to add an energy filter at a later date, if it becomes necessary driven by scientific need to improve the resolution further.

  17. Laser-induced electron emission from a tungsten nanotip: identifying above threshold photoemission using energy-resolved laser power dependencies

    NASA Astrophysics Data System (ADS)

    Bionta, M. R.; Chalopin, B.; Champeaux, J. P.; Faure, S.; Masseboeuf, A.; Moretto-Capelle, P.; Chatel, B.

    2014-06-01

    We present an experiment studying the interaction of a strongly focused 25 fs laser pulse with a tungsten nanotip, investigating the different regimes of laser-induced electron emission. We study the dependence of the electron yield with respect to the static electric field applied to the tip. Photoelectron spectra are recorded using a retarding field spectrometer and peaks separated by the photon energy are observed with a 45% contrast. They are a clear signature of above threshold photoemission (ATP), and are confirmed by extensive spectrally resolved studies of the laser power dependence. Understanding these mechanisms opens the route to control experiment in the strong-field regime on nanoscale objects.

  18. Multi-atom resonant photoemission and the development of next-generation software and high-speed detectors for electron spectroscopy

    SciTech Connect

    Kay, Alexander William

    2000-09-01

    This dissertation has involved the exploration of a new effect in photoelectron emission, multi-atom resonant photoemission (MARPE), as well as the development of new software, data analysis techniques, and detectors of general use in such research. We present experimental and theoretical results related to MARPE, in which the photoelectron intensity from a core level on one atom is influenced by a core-level absorption resonance on another. We point out that some of our and others prior experimental data has been strongly influenced by detector non-linearity and that the effects seen in new corrected data are smaller and of different form. Corrected data for the MnO(001) system with resonance between the O 1s and Mn 2p energy levels are found to be well described by an extension of well-known intraatomic resonant photoemission theory to the interatomic case, provided that interactions beyond the usual second-order Kramers-Heisenberg treatment are included. This theory is also found to simplify under certain conditions so as to yield results equivalent to a classical x-ray optical approach, with the latter providing an accurate and alternative, although less detailed and general, physical picture of these effects. Possible future applications of MARPE as a new probe of near-neighbor identities and bonding and its relationship to other known effects are also discussed. We also consider in detail specially written data acquisition software that has been used for most of the measurements reported here. This software has been used with an existing experimental system to develop the method of detector characterization and then data correction required for the work described above. The development of a next generation one-dimensional, high-speed, electron detector is also discussed. Our goal has been to design, build and test a prototype high-performance, one-dimensional pulse-counting detector that represents a significant advancement in detector technology and is well

  19. 48-Channel electron detector for photoemission spectroscopy and microscopy

    NASA Astrophysics Data System (ADS)

    Gregoratti, L.; Barinov, A.; Benfatto, E.; Cautero, G.; Fava, C.; Lacovig, P.; Lonza, D.; Kiskinova, M.; Tommasini, R.; Mähl, S.; Heichler, W.

    2004-01-01

    We show that it is possible to use a multichannel electron detector in a zone plate based photoemission spectromicroscopy in a snap shot mode to reduce the total acquisition time for a given counting time by 50% relative to the standard scanning mode while preserving the feature of the spectra. We describe the result of tests performed at Elettra using its microbeam (150 nm) together with a 48-channel detector designed for the PHOIBOS 100 analyzer optimized for extremely small x-ray sources. We also give a short summary of the technical features of the detector and describe one possible calibration procedure for its use in the snap shot mode. We show initial results from using this device to perform chemical maps of surfaces at a resolution of 150 nm.

  20. Photoemission characteristics of thin GaAs-based heterojunction photocathodes

    SciTech Connect

    Feng, Cheng; Zhang, Yijun Qian, Yunsheng; Shi, Feng; Zou, Jijun; Zeng, Yugang

    2015-01-14

    To better understand the different photoemission mechanism of thin heterojunction photocathodes, the quantum efficiency models of reflection-mode and transmission-mode GaAs-based heterojunction photocathodes are revised based on one-dimensional continuity equations, wherein photoelectrons generated from both the emission layer and buffer layer are taken into account. By comparison of simulated results between the revised and conventional models, it is found that the electron contribution from the buffer layer to shortwave quantum efficiency is closely related to some factors, such as the thicknesses of emission layer and buffer layer and the interface recombination velocity. Besides, the experimental quantum efficiency data of reflection-mode and transmission-mode AlGaAs/GaAs photocathodes are well fitted to the revised models, which confirm the applicability of the revised quantum efficiency models.

  1. Widespread spin polarization effects in photoemission from topological insulators

    SciTech Connect

    Jozwiak, C.; Chen, Y. L.; Fedorov, A. V.; Analytis, J. G.; Rotundu, C. R.; Schmid, A. K.; Denlinger, J. D.; Chuang, Y.-D.; Lee, D.-H.; Fisher, I. R.; Birgeneau, R. J.; Shen, Z.-X.; Hussain, Z.; Lanzara, A.

    2011-06-22

    High-resolution spin- and angle-resolved photoemission spectroscopy (spin-ARPES) was performed on the three-dimensional topological insulator Bi{sub 2}Se{sub 3} using a recently developed high-efficiency spectrometer. The topological surface state's helical spin structure is observed, in agreement with theoretical prediction. Spin textures of both chiralities, at energies above and below the Dirac point, are observed, and the spin structure is found to persist at room temperature. The measurements reveal additional unexpected spin polarization effects, which also originate from the spin-orbit interaction, but are well differentiated from topological physics by contrasting momentum and photon energy and polarization dependencies. These observations demonstrate significant deviations of photoelectron and quasiparticle spin polarizations. Our findings illustrate the inherent complexity of spin-resolved ARPES and demonstrate key considerations for interpreting experimental results.

  2. Electric field stimulation setup for photoemission electron microscopes.

    PubMed

    Buzzi, M; Vaz, C A F; Raabe, J; Nolting, F

    2015-08-01

    Manipulating magnetisation by the application of an electric field in magnetoelectric multiferroics represents a timely issue due to the potential applications in low power electronics and the novel physics involved. Thanks to its element sensitivity and high spatial resolution, X-ray photoemission electron microscopy is a uniquely suited technique for the investigation of magnetoelectric coupling in multiferroic materials. In this work, we present a setup that allows for the application of in situ electric and magnetic fields while the sample is analysed in the microscope. As an example of the performances of the setup, we present measurements on Ni/Pb(Mg(0.66)Nb(0.33))O3-PbTiO3 and La(0.7)Sr(0.3)MnO3/PMN-PT artificial multiferroic nanostructures.

  3. Electric field stimulation setup for photoemission electron microscopes

    SciTech Connect

    Buzzi, M.; Vaz, C. A. F.; Raabe, J.; Nolting, F.

    2015-08-15

    Manipulating magnetisation by the application of an electric field in magnetoelectric multiferroics represents a timely issue due to the potential applications in low power electronics and the novel physics involved. Thanks to its element sensitivity and high spatial resolution, X-ray photoemission electron microscopy is a uniquely suited technique for the investigation of magnetoelectric coupling in multiferroic materials. In this work, we present a setup that allows for the application of in situ electric and magnetic fields while the sample is analysed in the microscope. As an example of the performances of the setup, we present measurements on Ni/Pb(Mg{sub 0.66}Nb{sub 0.33})O{sub 3}-PbTiO{sub 3} and La{sub 0.7}Sr{sub 0.3}MnO{sub 3}/PMN-PT artificial multiferroic nanostructures.

  4. Electric field stimulation setup for photoemission electron microscopes.

    PubMed

    Buzzi, M; Vaz, C A F; Raabe, J; Nolting, F

    2015-08-01

    Manipulating magnetisation by the application of an electric field in magnetoelectric multiferroics represents a timely issue due to the potential applications in low power electronics and the novel physics involved. Thanks to its element sensitivity and high spatial resolution, X-ray photoemission electron microscopy is a uniquely suited technique for the investigation of magnetoelectric coupling in multiferroic materials. In this work, we present a setup that allows for the application of in situ electric and magnetic fields while the sample is analysed in the microscope. As an example of the performances of the setup, we present measurements on Ni/Pb(Mg(0.66)Nb(0.33))O3-PbTiO3 and La(0.7)Sr(0.3)MnO3/PMN-PT artificial multiferroic nanostructures. PMID:26329198

  5. Electric field stimulation setup for photoemission electron microscopes

    NASA Astrophysics Data System (ADS)

    Buzzi, M.; Vaz, C. A. F.; Raabe, J.; Nolting, F.

    2015-08-01

    Manipulating magnetisation by the application of an electric field in magnetoelectric multiferroics represents a timely issue due to the potential applications in low power electronics and the novel physics involved. Thanks to its element sensitivity and high spatial resolution, X-ray photoemission electron microscopy is a uniquely suited technique for the investigation of magnetoelectric coupling in multiferroic materials. In this work, we present a setup that allows for the application of in situ electric and magnetic fields while the sample is analysed in the microscope. As an example of the performances of the setup, we present measurements on Ni/Pb(Mg0.66Nb0.33)O3-PbTiO3 and La0.7Sr0.3MnO3/PMN-PT artificial multiferroic nanostructures.

  6. Electronic Structure of HgBa2CaCu2O(6+delta) Epitaxial films measured by x-ray Photoemission

    NASA Technical Reports Server (NTRS)

    Vasquez, R. P.; Rupp, M.; Gupta, A.; Tsuei, C. C.

    1995-01-01

    The electronic structure and chemical states of HgBa2CaCu20(sub 6 + delta), epitaxial films have been studied with x-ray photelectron spectroscopy. Signals from the superconducting phase dominate all the core-level spectra, and a clear Fermi edge is observed in the valence-band region. The Ba, Ca, Cu, and O core levels are similar to those of Tl2Ba2CaCu208(+)O(sub 6 + delta), but distinct differences are observed in the valence bands which are consistent with differences in the calculated densities of states.

  7. Photoemission from solids: the transition from solid-state to atomic physics

    SciTech Connect

    Shirley, D.A.

    1980-08-01

    As the photon energy is increased, photoemission from solids undergoes a slow transition from solid-state to atomic behavior. However, throughout the energy range h..nu.. = 10 to 1000 eV or higher both types of phenomena are present. Thus angle-resolved photoemission can only be understood quantitatively if each experimenter recognizes the presence of band-structure, photoelectron diffraction, and photoelectron asymmetry effects. The quest for this understanding will build some interesting bridges between solid-state and atomic physics and should also yield important new insights about the phenomena associated with photoemission.

  8. Vacuum space charge effect in laser-based solid-state photoemission spectroscopy

    SciTech Connect

    Graf, Jeff; Hellmann, Stefan; Jozwiak, Chris; Smallwood, Christopher; Hussain, Zahid; Kaindl, Robert; Kipp, Lutz; Rossnagel, Kai; Lanzara, Alessandra

    2009-08-05

    We report a systematic measurement of the space charge effect observed in the few-ps laser pulse regime in laser-based solid-state photoemission spectroscopy experiments. The broadening and the shift of a gold Fermi edge as a function of spot size, laser power, and emission angle are characterized for pulse lengths of 6 ps and 6 eV photon energy. The results are used as a benchmark for an N-body numerical simulation and are compared to different regimes used in photoemission spectroscopy. These results provide an important reference for the design of time and angle-resolved photoemission spectroscopy setups and next-generation light sources.

  9. An Angle Resolved Photoemission Survey of the Band Structure of the Heavy Fermion Superconductor, CeCoIn5

    NASA Astrophysics Data System (ADS)

    Reber, Theodore; Rameau, Jonathon; Hu, Rongwei; Petrovic, Cedomir; Johnson, Peter

    2015-03-01

    With the highest Tc of the non-radioactive heavy fermion materials, CeCoIn5 has been extensively studied by a host of techniques. However direct measurements of the band structure via angle resolved photo-emission spectroscopy has been limited to just a few experiments. We will present our studies of the momentum, temperature, photon energy and polarization dependence of the band structure of CeCoIn5. We will compare our results with theory and other experimental results. Present address: Rutgers Center for Emergent Materials and Department of Physics and Astronomy, Rutgers University

  10. Electronic structure investigation of atomic layer deposition ruthenium(oxide) thin films using photoemission spectroscopy

    SciTech Connect

    Schaefer, Michael E-mail: schlaf@mail.usf.edu; Schlaf, Rudy E-mail: schlaf@mail.usf.edu

    2015-08-14

    Analyzing and manipulating the electronic band line-up of interfaces in novel micro- and nanoelectronic devices is important to achieve further advancement in this field. Such band alignment modifications can be achieved by introducing thin conformal interfacial dipole layers. Atomic layer deposition (ALD), enabling angstrom-precise control over thin film thickness, is an ideal technique for this challenge. Ruthenium (Ru{sup 0}) and its oxide (RuO{sub 2}) have gained interest in the past decade as interfacial dipole layers because of their favorable properties like metal-equivalent work functions, conductivity, etc. In this study, initial results of the electronic structure investigation of ALD Ru{sup 0} and RuO{sub 2} films via photoemission spectroscopy are presented. These experiments give insight into the band alignment, growth behavior, surface structure termination, and dipole formation. The experiments were performed in an integrated vacuum system attached to a home-built, stop-flow type ALD reactor without exposing the samples to the ambient in between deposition and analysis. Bis(ethylcyclopentadienyl)ruthenium(II) was used as precursor and oxygen as reactant. The analysis chamber was outfitted with X-ray photoemission spectroscopy (LIXPS, XPS). The determined growth modes are consistent with a strong growth inhibition situation with a maximum average growth rate of 0.21 Å/cycle for RuO{sub 2} and 0.04 Å/cycle for Ru.{sup 0} An interface dipole of up to −0.93 eV was observed, supporting the assumption of a strongly physisorbed interface. A separate experiment where the surface of a RuO film was sputtered suggests that the surface is terminated by an intermediate, stable, non-stoichiometric RuO{sub 2}/OH compound whose surface is saturated with hydroxyl groups.

  11. Electronic structure investigation of atomic layer deposition ruthenium(oxide) thin films using photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Schaefer, Michael; Schlaf, Rudy

    2015-08-01

    Analyzing and manipulating the electronic band line-up of interfaces in novel micro- and nanoelectronic devices is important to achieve further advancement in this field. Such band alignment modifications can be achieved by introducing thin conformal interfacial dipole layers. Atomic layer deposition (ALD), enabling angstrom-precise control over thin film thickness, is an ideal technique for this challenge. Ruthenium (Ru0) and its oxide (RuO2) have gained interest in the past decade as interfacial dipole layers because of their favorable properties like metal-equivalent work functions, conductivity, etc. In this study, initial results of the electronic structure investigation of ALD Ru0 and RuO2 films via photoemission spectroscopy are presented. These experiments give insight into the band alignment, growth behavior, surface structure termination, and dipole formation. The experiments were performed in an integrated vacuum system attached to a home-built, stop-flow type ALD reactor without exposing the samples to the ambient in between deposition and analysis. Bis(ethylcyclopentadienyl)ruthenium(II) was used as precursor and oxygen as reactant. The analysis chamber was outfitted with X-ray photoemission spectroscopy (LIXPS, XPS). The determined growth modes are consistent with a strong growth inhibition situation with a maximum average growth rate of 0.21 Å/cycle for RuO2 and 0.04 Å/cycle for Ru.0 An interface dipole of up to -0.93 eV was observed, supporting the assumption of a strongly physisorbed interface. A separate experiment where the surface of a RuO film was sputtered suggests that the surface is terminated by an intermediate, stable, non-stoichiometric RuO2/OH compound whose surface is saturated with hydroxyl groups.

  12. Domain imaging on multiferroic BiFeO{sub 3}(001) by linear and circular dichroism in threshold photoemission

    SciTech Connect

    Sander, Anke; Christl, Maik; Chiang, Cheng-Tien; Alexe, Marin; Widdra, Wolf

    2015-12-14

    We demonstrate ferroelectric domain imaging at BiFeO{sub 3}(001) single crystal surfaces with laser-based threshold photoemission electron microscopy (PEEM). Work function differences and linear dichroism allow for the identification of the eight independent ferroelectric domain configurations in the PEEM images. There, the determined domain structure is consistent with piezoresponse force microscopy of the sample surface and can also be related to the circular dichroic PEEM images. Our results provide a method for efficient mapping of complex ferroelectric domains with laser-excited PEEM and may allow lab-based time-resolved studies of the domain dynamics in the future.

  13. Dependence of the band structure of C-60 monolayers on molecularorientations and doping observed by angle resolved photoemission

    SciTech Connect

    Brouet, V.; Yang, W.L.; Zhou, X.J.; Hussain, Z.; Shen, Z.X.

    2008-01-17

    We present angle resolved photoemission studies of C60monolayers deposited on Ag surfaces. The electronic structure of thesemonolayers is derived from the partial filling of the narrow, 6-folddegenerated, C60 conduction band. By comparing the band structure in twomonolayers deposited, respectively, on Ag(111) and Ag(100), we show thatthe molecular degree of freedom, in this case the relative orientationsbetween C60 molecules, is essential to describe the band structure. Wefurther show that the evolution of the band as a function of doping doesnot follow a rigid band-filling picture. Phase separation is observedbetween a metallic and an insulating phase, which might be a result ofstrong correlations.

  14. A synchrotron-based spectroscopic study of the electronic structure of N-doped HOPG and PdY/N-doped HOPG

    NASA Astrophysics Data System (ADS)

    Favaro, M.; Rizzi, G. A.; Nappini, S.; Magnano, E.; Bondino, F.; Agnoli, S.; Granozzi, G.

    2016-04-01

    N-doped Highly Oriented Pyrolytic Graphite (HOPG) (obtained by ion implantation) was used as a model system for mimicking the effect of N-doping in sp2 hybridized carbon based supports. The electronic structure of such system has been careful characterized by means of spectroscopic techniques adopting synchrotron radiation. We demonstrate that it is possible to tailor different functional groups simply by tuning the annealing temperature after ion implantation. On such chemical modified HOPG, PdY catalyst nanoparticles have been deposited under strictly controlled conditions in ultra-high-vacuum (UHV) and the nanoparticle/support interactions studied by photoemission. The formation of the Pd3Y alloy is evidenced by core level shift in Y 3d and Pd 3d states due to charge transfer.

  15. Characterization of Catechins in Water by Photoemission Yield Spectroscopy in Air.

    PubMed

    Yamashita, Daisuke; Ishizaki, Atsushi

    2016-01-01

    Photoemission yield spectroscopy in air (PYSA) was applied for the characterization of catechins in water in ambient conditions. According to the results of measurements on aqueous solutions of epigallocatechin gallate (EGCg) of various concentrations, the photoemission yield is almost proportional to the concentration of EGCg. Contrarily, the threshold energy of photoemission, EPET, is almost constant at 5.46 ± 0.02 eV. Moreover, we measured aqueous solutions of epicatechin (EC), epigallocatechin (EGC), and epicatechin gallate (ECg). The values of EPET of EC, EGC, ECg were estimated to be 5.72 ± 0.02, 5.68 ± 0.01, and 5.45 ± 0.02 eV, respectively, and a dependence on the molecular structure was found. Furthermore, changes in the photoemission yield spectra of heated EGCg were well explained by molecular orbital calculations on the basis of an assumption of epimerization. PMID:27169659

  16. What angle-resolved photoemission experiments tell about the microscopic theory for high-temperature superconductors

    PubMed Central

    Abrahams, Elihu; Varma, C. M.

    2000-01-01

    Recent angular-resolved photoemission experiments on high-temperature superconductors are consistent with a phenomenological description of the normal state of these materials as marginal Fermi liquids. The experiments also provide constraints on microscopic theories. PMID:10811895

  17. Observation of Two-Photon Photoemission Optogalvanic Effect Using Copper Target Electrode

    NASA Astrophysics Data System (ADS)

    Ajithprasad, K. C.; Sasikumar, P. R.; Harilal, S. S.; Nampoori, V. P. N.; Vallabhan, C. P. G.

    Two-photon-induced photoemission optogalvanic effect using copper as the target electrode has been observed in a nitrogen discharge cell using 532 nm radiation from a frequency-doubled Nd:YAG laser as the pump source.

  18. Predicting photoemission intensities and angular distributions with real-time density-functional theory

    NASA Astrophysics Data System (ADS)

    Dauth, M.; Kümmel, S.

    2016-02-01

    Photoemission spectroscopy is one of the most frequently used tools for characterizing the electronic structure of condensed matter systems. We discuss a scheme for simulating photoemission from finite systems based on time-dependent density-functional theory. It allows for the first-principles calculation of relative electron binding energies, ionization cross sections, and anisotropy parameters. We extract these photoemission spectroscopy observables from Kohn-Sham orbitals propagated in real time. We demonstrate that the approach is capable of estimating photoemission intensities, i.e., peak heights. It can also reliably predict the angular distribution of photoelectrons. For the example of benzene we contrast calculated angular distribution anisotropy parameters to experimental reference data. Self-interaction free Kohn-Sham theory yields meaningful outer valence single-particle states in the right energetic order. We discuss how to properly choose the complex absorbing potential that is used in the simulations.

  19. Copper-ceria interaction: A combined photoemission and DFT study

    NASA Astrophysics Data System (ADS)

    Szabová, Lucie; Skála, Tomáš; Matolínová, Iva; Fabris, Stefano; Farnesi Camellone, Matteo; Matolín, Vladimír

    2013-02-01

    Stoichiometric and partially reduced ceria films were deposited on preoxidized Ru(0 0 0 1) crystal by Ce evaporation in oxygen atmosphere of different pressures at 700 K. Copper-ceria interaction was investigated by deposition of metalic copper on both types of substrate. The samples were characterized by low energy electron diffraction (LEED), X-ray photoelectron spectroscopy (XPS) of core states and resonant photoelectron spectroscopy (RPES) of the valence bands. Copper adsorption on stoichiometric ceria caused reduction of CeO2, while on the oxygen-defficient ceria it partially reoxidized the substrate. This is in agreement with DFT+U calculations of copper adsorption on stoichiometric and defective ceria surfaces.

  20. Attosecond photoemission dynamics encoded in real-valued continuum wave functions

    NASA Astrophysics Data System (ADS)

    Gaillac, Romain; Vacher, Morgane; Maquet, Alfred; Taïeb, Richard; Caillat, Jérémie

    2016-01-01

    The dynamics of photoemission is fully encoded in the continuum wave functions selected by the transitions. Using numerical simulations on simple benchmark models, we show how scattering phase shifts and photoemission delays can be retrieved from this unambiguously defined class of wave functions. In contrast with standard scattering waves inherited from collision theory, they are real-valued for one-photon transitions and provide a clear-cut interpretation of the delays recently discussed in the framework of attosecond science.

  1. High-harmonic XUV source for time- and angle-resolved photoemission spectroscopy

    SciTech Connect

    Dakovski, Georgi L; Li, Yinwan; Durakiewicz, Tomasz; Rodriguez, George

    2009-01-01

    We present a laser-based apparatus for visible pump/XUV probe time- and angle-resolved photoemission spectroscopy (TRARPES) utilizing high-harmonic generation from a noble gas. Femtosecond temporal resolution for each selected harmonic is achieved by using a time-delay-compensated monochromator (TCM). The source has been used to obtain photoemission spectra from insulators (UO{sub 2}) and ultrafast pump/probe processes in semiconductors (GaAs).

  2. Low-Temperature and High-Energy-Resolution Laser Photoemission Spectroscopy

    NASA Astrophysics Data System (ADS)

    Shimojima, Takahiro; Okazaki, Kozo; Shin, Shik

    2015-07-01

    We present a review on the developments in the photoemission spectrometer with a vacuum ultraviolet laser at Institute for Solid State Physics at the University of Tokyo. The advantages of high energy resolution, high cooling ability, and bulk sensitivity enable applications with a wide range of materials. We introduce some examples of fine electronic structures detected by laser photoemission spectroscopy and discuss the prospects of research on low-transition-temperature superconductors exhibiting unconventional superconductivity.

  3. Adsorption site and structure determination of c(2x2) N{sub 2}/Ni(100) using angle-resolved photoemission extended fine structure

    SciTech Connect

    Moler, E.J.; Kellar, S.A.; Huff, W.R.A.

    1997-04-01

    The authors have determined the atomic spatial structure of c(2x2) N2Ni(100) with Angle-Resolved Photoemission Extended Fine Structure (ARPEFS) from the nitrogen 1s core level using monochromatized x-rays from beamline 6.1 at SSRL and beamline 9.3.2 at the ALS. The chemically shifted N 1s peak intensities were summed together to obtain ARPEFS curves for both nitrogen atoms in the molecule. They used a new, highly-optimized program based on the Rehr-Albers scattering matrix formalism to find the adsorption site and to quantitatively determine the bond-lengths. The nitrogen molecule stands upright at an atop site, with a N-Ni bond length of 2.25(1) {angstrom}, a N-N bond length of 1.10(7) {angstrom}, and a first layer Ni-Ni spacing of 1.76(4) {angstrom}. The shake-up peak shows an identical ARPEFS diffraction pattern, confirming its intrinsic nature and supporting a previous use of this feature to decompose the peak into contributions from the chemically inequivalent nitrogen atoms. Comparison to a previously published theoretical treatment of N-N-Ni and experimental structures of analogous adsorbate systems demonstrates the importance of adsorbate-adsorbate interactions in weakly chemisorbed systems.

  4. Design of an ultrahigh vacuum transfer mechanism to interconnect an oxide molecular beam epitaxy growth chamber and an x-ray photoemission spectroscopy analysis system

    SciTech Connect

    Rutkowski, M. M.; Zeng Zhaoquan; McNicholas, K. M.; Brillson, L. J.

    2013-06-15

    We designed a mechanism and the accompanying sample holders to transfer between a VEECO 930 oxide molecular beam epitaxy (MBE) and a PHI Versa Probe X-ray photoemission spectroscopy (XPS) chamber within a multiple station growth, processing, and analysis system through ultrahigh vacuum (UHV). The mechanism consists of four parts: (1) a platen compatible with the MBE growth stage, (2) a platen compatible with the XPS analysis stage, (3) a sample coupon that is transferred between the two platens, and (4) the accompanying UHV transfer line. The mechanism offers a robust design that enables transfer back and forth between the growth chamber and the analysis chamber, and yet is flexible enough to allow transfer between standard sample holders for thin film growth and masked sample holders for making electrical contacts and Schottky junctions, all without breaking vacuum. We used this mechanism to transfer a barium strontium titanate thin film into the XPS analysis chamber and performed XPS measurements before and after exposing the sample to the air. After air exposure, a thin overlayer of carbon was found to form and a significant shift ({approx}1 eV) in the core level binding energies was observed.

  5. Angle-resolved photoemission spectroscopy observation of anomalous electronic states in EuFe2As(2-x)P(x).

    PubMed

    Richard, P; Capan, C; Ma, J; Zhang, P; Xu, N; Qian, T; Denlinger, J D; Chen, G-F; Sefat, A S; Fisk, Z; Ding, H

    2014-01-22

    We used angle-resolved photoemission spectroscopy to investigate the electronic structure and the Fermi surface of EuFe2As2, EuFe2As1.4P0.6 and EuFe2P2. We observed doubled core level peaks associated with the pnictide atoms. Using K atoms evaporated at the surface to affect the surface quality, we show that one component of these doubled peaks is related to a surface state. Nevertheless, strong electronic dispersion along the c-axis, especially pronounced in EuFe2P2, is observed for at least one band, thus indicating that the Fe states, albeit probably affected at the surface, do not form pure two-dimensional surface states. We determine the evolution of the Fermi surface as a function of the P content and reveal that the hole Fermi surface pockets enlarge with increasing P content. We also show that the spectral weight near the Fermi level of EuFe2P2 is reduced as compared to that of EuFe2As2 and EuFe2As1.4P0.6. Finally, we identify the electronic states associated with the Eu(2+) f states and show an anomalous jump in EuFe2P2. PMID:24351570

  6. Design of an ultrahigh vacuum transfer mechanism to interconnect an oxide molecular beam epitaxy growth chamber and an x-ray photoemission spectroscopy analysis system

    NASA Astrophysics Data System (ADS)

    Rutkowski, M. M.; McNicholas, K. M.; Zeng, Zhaoquan; Brillson, L. J.

    2013-06-01

    We designed a mechanism and the accompanying sample holders to transfer between a VEECO 930 oxide molecular beam epitaxy (MBE) and a PHI Versa Probe X-ray photoemission spectroscopy (XPS) chamber within a multiple station growth, processing, and analysis system through ultrahigh vacuum (UHV). The mechanism consists of four parts: (1) a platen compatible with the MBE growth stage, (2) a platen compatible with the XPS analysis stage, (3) a sample coupon that is transferred between the two platens, and (4) the accompanying UHV transfer line. The mechanism offers a robust design that enables transfer back and forth between the growth chamber and the analysis chamber, and yet is flexible enough to allow transfer between standard sample holders for thin film growth and masked sample holders for making electrical contacts and Schottky junctions, all without breaking vacuum. We used this mechanism to transfer a barium strontium titanate thin film into the XPS analysis chamber and performed XPS measurements before and after exposing the sample to the air. After air exposure, a thin overlayer of carbon was found to form and a significant shift (˜1 eV) in the core level binding energies was observed.

  7. X-ray Photoemission Spectra and Electronic Structure of Coumarin and its Derivatives.

    PubMed

    Wickrama Arachchilage, Anoja P; Wang, Feng; Feyer, Vitaliy; Plekan, Oksana; Acres, Robert G; Prince, Kevin C

    2016-09-15

    The electronic structures of coumarin and three of its derivatives (7-amino-4-methylcoumarin, 7-amino-4-(trifluoro)methylcoumarin, and 4-hydroxycoumarin) have been studied by theoretical calculations, and compared with experimental valence and core photoelectron spectra to benchmark the predicted spectra. The outer valence band spectra of the first three compounds showed good agreement with theoretical calculations for a single isomer, whereas the spectrum of 4-hydroxycoumarin indicated the presence of more than one tautomer, consistent with published results. Calculations of core level spectra of carbon, nitrogen, oxygen, and fluorine of the first three compounds are also in satisfactory agreement with our measurements. The carbon and oxygen 1s spectra of 4-hydroxycoumarin allow us to identify and quantify the populations of the principle tautomers present. The 4-hydroxy enol form is the most stable isomer at 348 K, followed by the diketo form, with 1.3 kJ·mol(-1) lower energy. PMID:27545582

  8. Adsorption study of copper phthalocyanine on Si(111)(√3 × √3)R30°Ag surface

    NASA Astrophysics Data System (ADS)

    Menzli, S.; Ben Hamada, B.; Arbi, I.; Souissi, A.; Laribi, A.; Akremi, A.; Chefi, C.

    2016-04-01

    The adsorption of copper phthalocyanine (CuPc) molecules on Si(111)(√3 × √3)R30°Ag surface is studied at room temperature under ultra high vacuum. Crystallographic, chemical and electronic properties of the interface are investigated by low energy electron diffraction (LEED), ultraviolet and X-ray photoemission spectroscopies (UPS, XPS) and X-ray photoemission diffraction (XPD). LEED and XPD results indicate that after one monolayer deposition the molecular layer is highly ordered with a flat lying adsorption configuration. The corresponding pattern reveals the coexistence of three symmetrically equivalent orientations of molecules with respect to the substrate. XPS core level spectra of the substrate reveal that there is no discernible chemical interaction between molecules and substrate; however there is evidence of Fermi level movement. During the growth, the work function was found to decrease from 4.90 eV for the clean substrate to 4.35 eV for the highest coverage (60 monolayers). Within a thickness of two monolayer deposition an interface dipole of 0.35 eV and a band bending of 0.2 eV have been found. UPS spectra indicate the existence of a band bending of the highest occupied molecular orbital (HOMO) of 0.55 eV. The changes in the work function, in the Fermi level position and in the HOMO state have been used to determine the energy level alignment at the interface.

  9. Electronic structure of YBa2Cu3O7-δ as a function of δ : determination of the valency of copper atoms by X-ray absorption and photoemission experiments

    NASA Astrophysics Data System (ADS)

    Maurer, M.; Ravet, M. F.; Gourieux, T.; Krill, G.; Fontaine, A.; Tolentino, H.; Dartyge, E.; Tourillon, G.

    The electronic structure of YBa2Cu3O7- δ compounds has been studied in the range 0 < 8 < 1, by performing X-ray Absorption (XAS) on the Cu K edge and X-ray Photoemission experiments (XPS) on the Cu2p and O1s core levels. The absorption experiments have been performed by following continuously the Copper K edge during isothermal cycles of oxy-deoxygenation. Such experiments bring the absolute modifications of the electronic structure, thus minimizing the use of reference compounds in the discussion. An highly correlated mixed-valent ground state in these high Tc materials is suggested. A comparison with the XPS results is made and it confirms this assumption. Les structures électroniques de composés YBa2Cu3O 7-δ ont été étudiées dans la gamme de concentration 0 < δ < 1, à partir d'expériences d'absorption X au seuil K du cuivre et de photoémission X sur les niveaux internes Cu2p et O1 s. Les expériences d'absorption X ont été effectuées en suivant continûment le seuil K du cuivre lors de cycles isothermes d'oxy-désoxygénation des échantillons. Ces expériences nous permettent de discuter les modifications des structures électroniques, en minimisant l'utilisation de composés de référence. L'hypothèse de l'existence d'un état fondamental fortement corrélé, de type valence intermédiaire, est suggérée. Nous discutons également des résultats obtenus par spectroscopie XPS et montrons que ces expériences confortent notre précédente hypothèse.

  10. Probing the energy levels of perovskite solar cells via Kelvin probe and UV ambient pressure photoemission spectroscopy.

    PubMed

    Harwell, J R; Baikie, T K; Baikie, I D; Payne, J L; Ni, C; Irvine, J T S; Turnbull, G A; Samuel, I D W

    2016-07-20

    The field of organo-lead halide perovskite solar cells has been rapidly growing since their discovery in 2009. State of the art devices are now achieving efficiencies comparable to much older technologies like silicon, while utilising simple manufacturing processes and starting materials. A key parameter to consider when optimising solar cell devices or when designing new materials is the position and effects of the energy levels in the materials. We present here a comprehensive study of the energy levels present in a common structure of perovskite solar cell using an advanced macroscopic Kelvin probe and UV air photoemission setup. By constructing a detailed map of the energy levels in the system we are able to predict the importance of each layer to the open circuit voltage of the solar cell, which we then back up through measurements of the surface photovoltage of the cell under white illumination. Our results demonstrate the effectiveness of air photoemission and Kelvin probe contact potential difference measurements as a method of identifying the factors contributing to the open circuit voltage in a solar cell, as well as being an excellent way of probing the physics of new materials.

  11. 4f photoemission from Ce clusters and disordered reaction products at Ce/Si and Ce/GaAs interfaces

    NASA Astrophysics Data System (ADS)

    Fujimori, Atsushi; Grioni, M.; Joyce, J. J.; Weaver, J. H.

    1985-06-01

    Synchrotron radiation photoemission has been used to study the 4f emission from 4f electrons in Ce clusters and disordered reaction products at Ce/GaAs(110) and Ce/Si(111) interfaces. For low Ce coverages on GaAs(110), the reacted interface forms Ce-As local configurations with two 4f-derived features similar to those of bulk CeAs. The shallower 4f peak is located ~1 eV below EF, indicating that it is not due to fully relaxed 4f holes, consistent with the As p-->Ce 4f charge-transfer screening mechanism. For the Ce/Si interface, small Ce clusters formed at low coverage have only a single 4f peak at -3.3 eV, with no evidence of a second peak nearer EF. This is attributed to the reduced number of neighboring Ce 5d orbitals for the clusters, apparent stability of the γ phase relative to the α phase (in the ground state), and reducted 5d-->4f charge-transfer screening probability in the photoemission final state. At high coverages, Ce overlayers cover the reacted interfaces, but our results show that the 4f emission near EF is not established until θ~=20 monolayers, suggesting that the 4f-5d hybridization in metallic Ce is long ranged compared with the short-range Ce-4f/As-p hybridization.

  12. Probing the energy levels of perovskite solar cells via Kelvin probe and UV ambient pressure photoemission spectroscopy.

    PubMed

    Harwell, J R; Baikie, T K; Baikie, I D; Payne, J L; Ni, C; Irvine, J T S; Turnbull, G A; Samuel, I D W

    2016-07-20

    The field of organo-lead halide perovskite solar cells has been rapidly growing since their discovery in 2009. State of the art devices are now achieving efficiencies comparable to much older technologies like silicon, while utilising simple manufacturing processes and starting materials. A key parameter to consider when optimising solar cell devices or when designing new materials is the position and effects of the energy levels in the materials. We present here a comprehensive study of the energy levels present in a common structure of perovskite solar cell using an advanced macroscopic Kelvin probe and UV air photoemission setup. By constructing a detailed map of the energy levels in the system we are able to predict the importance of each layer to the open circuit voltage of the solar cell, which we then back up through measurements of the surface photovoltage of the cell under white illumination. Our results demonstrate the effectiveness of air photoemission and Kelvin probe contact potential difference measurements as a method of identifying the factors contributing to the open circuit voltage in a solar cell, as well as being an excellent way of probing the physics of new materials. PMID:27384817

  13. 1S core-level spectroscopy of graphite: The effects of phonons on emission and absorption and validity of the final-state rule

    NASA Astrophysics Data System (ADS)

    Franck, C. P.; Schnatterly, S. E.; Zutavern, F. J.; Aton, T.; Cafolla, T.; Carson, R. D.

    1985-04-01

    We have used both electron-induced soft x-ray emission and fast inelastic electron scattering to observe 1S core-level emission and absorption in graphite near threshold. Linear phonon coupling with partial relaxation is found to quantitatively explain the absorption linewidth, the emission broadening, and the unusually large difference between emission and absorption threshold energies (Stokes shift). Both emission and absorption line shapes quantitatively obey the final-state rule, which asserts that the best single-particle potential describing these many electron processes is the final-state potential.

  14. Nanoscale morphology and photoemission of arsenic implanted germanium films

    NASA Astrophysics Data System (ADS)

    Petö, G.; Khanh, N. Q.; Horváth, Z. E.; Molnár, G.; Gyulai, J.; Kótai, E.; Guczi, L.; Frey, L.

    2006-04-01

    Germanium films of 140 nm thickness deposited onto Si substrate were implanted with 70 keV arsenic ions with a dose of 2.5×1014 cm-2. The morphology of the implanted films was determined by Rutherford backscattering and cross-sectional transmission electron microscopy. Concentration of oxygen and carbon impurities and their distribution in the implanted layer were detected by secondary-ion-mass spectroscopy and nuclear reaction analysis using the O16(He4,He4)O16 reaction. The depth dependence of the valence band density of states was investigated by measuring the energy distribution curve of photoelectrons using Ar ion etching for profiling. The morphology of As implanted film was dominated by nanosized (10-100 nm) Ge islands separated by empty bubbles at a depth of 20-50 nm under the surface. At depth ranges of 0-20 and 70 to a measured depth of 140 nm, however, morphology of the as-evaporated Ge film was not modified. At a depth of 20-50 nm, photoelectron spectra were similar to those obtained for Ge amorphized with heavy ion (Sb) implantation [implantation induced (I.I.) a-Ge]. The depth profile of the morphology and the photoemission data indicate correlation between the morphology and valence band density of states of the ion I.I. a-Ge. As this regime was formed deep in the evaporated film, i.e., isolated from the environment, any contamination, etc., effect can be excluded. The depth distribution of this I.I. a-Ge layer shows that the atomic displacement process cannot account for its formation.

  15. Performance of the TPSS Functional on Predicting Core Level Binding Energies of Main Group Elements Containing Molecules: A Good Choice for Molecules Adsorbed on Metal Surfaces.

    PubMed

    Pueyo Bellafont, Noèlia; Viñes, Francesc; Illas, Francesc

    2016-01-12

    Here we explored the performance of Hartree-Fock (HF), Perdew-Burke-Ernzerhof (PBE), and Tao-Perdew-Staroverov-Scuseria (TPSS) functionals in predicting core level 1s binding energies (BEs) and BE shifts (ΔBEs) for a large set of 68 molecules containing a wide variety of functional groups for main group elements B → F and considering up to 185 core levels. A statistical analysis comparing with X-ray photoelectron spectroscopy (XPS) experiments shows that BEs estimations are very accurate, TPSS exhibiting the best performance. Considering ΔBEs, the three methods yield very similar and excellent results, with mean absolute deviations of ∼0.25 eV. When considering relativistic effects, BEs deviations drop approaching experimental values. So, the largest mean percentage deviation is of 0.25% only. Linear trends among experimental and estimated values have been found, gaining offsets with respect to ideality. By adding relativistic effects to offsets, HF and TPSS methods underestimate experimental values by solely 0.11 and 0.05 eV, respectively, well within XPS chemical precision. TPSS is posed as an excellent choice for the characterization, by XPS, of molecules on metal solid substrates, given its suitability in describing metal substrates bonds and atomic and/or molecular orbitals.

  16. Final-state diffraction effects in angle-resolved photoemission at an organic-metal interface

    NASA Astrophysics Data System (ADS)

    Bocquet, F. C.; Giovanelli, L.; Amsalem, P.; Petaccia, L.; Topwal, D.; Gorovikov, S.; Abel, M.; Koch, N.; Porte, L.; Goldoni, A.; Themlin, J.-M.

    2011-12-01

    In this paper it is shown that angle-resolved photoemission performed using low-energy photons on an organic-metal interface allows to clearly distinguish genuine interface states from features of substrate photoelectrons diffracted by the molecular lattice. As a model system an ordered monolayer of Zn-phthalocyanine is used as a diffraction lattice to probe the electronic band structure of a Ag(110) substrate. Photoemission close to normal emission geometry reveals strongly dispersive features absent in the pristine substrate spectra. Density functional theory modeling helped identifying these as bulk sp direct transitions undergoing surface-umklapp processes. The present results establish the important role of final-state diffraction effects in photoemission experiments at organic-inorganic interfaces.

  17. Ligand field splittings in core level transitions for transition metal (TM) oxides: Tanabe-Sugano diagrams and (TM) dangling bonds in vacated O-atom defects

    NASA Astrophysics Data System (ADS)

    Lucovsky, Gerry; Wu, Kun; Pappas, Brian; Whitten, Jerry

    2013-04-01

    Defect states in the forbidden band-gap below the conduction band edge are active as electron traps in nano-grain high-) transition metal (TM) oxides with thickness >0.3 nm, e.g., ZrO2 and HfO2. These oxides have received considerable attention as gate-dielectrics in complementary metal oxide semiconductor (CMOS) devices, and more recently are emerging as candidates for charge storage and memory devices. To provide a theoretical basis for device functionality, ab-initio many-electron theory is combined with X-ray absorption spectroscopy (XAS) to study O K edge and TM core level transitions. These studies identify ligand field splittings (ΔLF) for defect state features,. When compared with those obtained from O-atom and TM-atom core spectroscopic transitions, this provides direct information about defect state sun-nm bonding arrangements. comparisons are made for (i) elemental TiO2 and Ti2O3 with different formal ionic charges, Ti4+ and Ti3+ and for (ii) Magneli Phase alloys, TinO2n-1, n is an integer 9>=n>3, and (TiO2)x(HfO2)1-x alloys. The alloys display multi-valent behavior from (i) different ionic-charge states, (ii} local bond-strain, and (iii) metallic hopping transport. The intrinsic bonding defects in TM oxides are identified as pairs of singly occupied dangling bonds. For 6-fold coordinated Ti-oxides defect excited states in 2nd derivative O K pre-edge spectra are essentially the same as single Ti-atom d2 transitions in Tanabe-Sugano (T-S) diagrams. O-vacated site defects in 8-fold coordinated ZrO2 and HfO2 are described by d8 T-S diagrams. T-S defect state ordering and splittings are functions of the coordination and symmetry of vacated site bordering TM atoms. ΔLF values from the analysis of T-S diagrams indicate medium range order (MRO) extending to 3rd and 4th nearest-neighbor (NN) TM-atoms. Values are different for 6-fold Ti, and 8-fold ZrO2 and HfO2, and scale inversely with differences in respective formal ionic radii. O-vacated site bonding

  18. The band structure of VO2 measured by angle-resolved photoemission

    NASA Astrophysics Data System (ADS)

    Moreschini, Luca; Chang, Young Jun; Innocenti, Davide; Walter, Andrew L.; Kim, Young Su; Gaines, Geoffrey; Bostwick, Aaron; Denlinger, Jonathan; Rotenberg, Eli

    2011-03-01

    The origin of the 340K metal-insulator transition (MIT) in VO2 is still under debate. the main reason is that no direct experimental verifications of the electronic structure of VO2 exist up to this point. The quality of the available single crystals is not sufficient for ARPES measurements, so that photoemission is limited to angle-integrated mode. New opportunities are offered by oxide films, on which data of equal or even higher quality have been reported (Saeki et al., PRB 2009). WIth the in situ pulsed-laser-deposition (PLD) system available on beamline 7.0.1 at the Advanced Light Source we have grown VO2(001) films on a TiO2 substrate and measured the Fermi surface of the metallic phase. These results will permit a direct comparison with the existing band calculations and open the way to the study of the MIT as a function, e.g., of film thickness or electron doping with Cr. Work supported by U.S. DOE (DE-AC02-05CH11231 for ALS), the Max Planck Society, and the Swiss National Science Foundation (PBELP2-125484).

  19. Building blocks of an artificial kagome spin ice: Photoemission electron microscopy of arrays of ferromagnetic islands

    NASA Astrophysics Data System (ADS)

    Mengotti, E.; Heyderman, L. J.; Fraile Rodríguez, A.; Bisig, A.; Le Guyader, L.; Nolting, F.; Braun, H. B.

    2008-10-01

    Arrays of dipolar coupled ferromagnetic islands arranged in specific geometries provide ideal systems to directly study frustration. We have examined with photoemission electron microscopy the magnetic configurations in three basic building blocks of an artificial kagome spin ice consisting of one, two, and three rings. The kagome spin ice arrangement is particularly interesting because it is highly frustrated and the three interactions at a vertex are equivalent. Employing dipolar energy calculations, we are able to make a full characterization of the magnetic states and therefore identify the lowest energy states. Experimentally we find that the ice rule is always obeyed even at low dipolar coupling strengths. However, as the number of rings increases there is a drastic decrease in the ability to achieve the low-energy states via demagnetization, a behavior also identified in the magnetization reversal. This carries the implication that the ground state will never be achieved in the infinite system. Finally, we show that at low coupling, the applied field direction governs the resulting states. This work opens the door to a novel class of systems for future spintronic applications.

  20. Mapping of Si/SiC p-n heterojunctions using scanning internal photoemission microscopy

    NASA Astrophysics Data System (ADS)

    Shingo, Masato; Liang, Jianbo; Shigekawa, Naoteru; Arai, Manabu; Shiojima, Kenji

    2016-04-01

    We demonstrated the two-dimensional characterization of p+-Si/n--SiC heterointerfaces by scanning internal photoemission microscopy (SIPM). In internal photoemission spectra, a linear relationship was found between the square root of photoyield (Y) and photon energy, and the threshold energy (qV th) was reasonably obtained to be 1.34 eV. From the SIPM results, Y and qV th maps were successfully obtained, and nanometer-deep gaps in the junction were sensitively visualized as a pattern. These results suggest that this method is a powerful tool for investigating the inhomogeneity of heterojunctions as well as their carrier transport properties.

  1. An XUV source using a femtosecond enhancement cavity for photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Mills, Arthur K.; Zhdanovich, Sergey; Sheyerman, Alex; Levy, Giorgo; Damascelli, Andrea; Jones, David J.

    2015-05-01

    Recent development of extreme ultraviolet (XUV) sources based on high harmonic generation (HHG) in femtosecond enhancement cavities (fsEC) has enabled generation of high photon ux ( ̴ 1013-1014 photons/sec) in the XUV, at high repetition rates (> 50 MHz) and spanning the spectral region from 40 nm - 120 nm. Here we demonstrate the potential offered by this approach for angle-resolved photoemission spectroscopy by measuring the photoemission spectrum of Au using 8.3 and 25 eV photons with excellent resolution at rapid data rates.

  2. The effect of photoemission on the streamer development and propagation in short uniform gaps

    NASA Astrophysics Data System (ADS)

    Georghiou, G. E.; Morrow, R.; Metaxas, A. C.

    2001-01-01

    Results are presented for the time evolution of photoemission in a 0.1 cm parallel-plane gap in atmospheric pressure air when a positive dc voltage is applied at one of the electrodes. The hydrodynamic set of equations is solved using the finite-element flux-corrected transport method in two dimensions. The time evolution of the electron distribution at the cathode and the variation of the spread of the electrons are examined during the avalanche, the avalanche-to-streamer transition and streamer propagation stages. Finally, the effect of the variation of the photoemission coefficient on the field distribution and the current waveform are presented.

  3. Multilayer ReS2 lateral p-n homojunction for photoemission and photodetection

    NASA Astrophysics Data System (ADS)

    Najmzadeh, Mohammad; Ko, Changhyun; Wu, Kedi; Tongay, Sefaattin; Wu, Junqiao

    2016-05-01

    In this paper, a multilayer ReS2 p-n homojunction is fabricated on an oxidized Si substrate, and its photoemission under a forward bias and its photodetection under a reverse bias are reported for the first time. Au nanoparticles were used to make lateral p-n homojunctions. The device shows room temperature photoemission in the IR range, and in the photodetector mode, it shows a 0.41 A/W responsivity under illumination by a 660 nm red laser.

  4. Core-level attosecond transient absorption spectroscopy of laser-dressed solid films of Si and Zr

    NASA Astrophysics Data System (ADS)

    Seres, Enikoe; Seres, Jozsef; Serrat, Carles; Namba, Shinichi

    2016-10-01

    We investigated experimentally as well as theoretically the ultrafast response of the wave function of the conduction band (CB) of Si and Zr to a near-infrared laser field using extreme ultraviolet (XUV) absorption spectroscopy in the spectral range of 80-220 eV. The measured dynamics of the XUV transmission demonstrates that the wave function of the CB follows the electric field of the dressing laser pulse. In these terms, laser dressing was earlier mainly studied on gases. Measurements with two-femtosecond and 200-attosecond temporal steps were performed in the vicinity of the Si L2 ,3 edge near 100 eV, the Si L1 edge near 150 eV, and the Zr M4 ,5 edge near 180 eV. The observed changes were dependent on the core states being excited by the XUV probe pulse. At the 2 p to CB transitions of Si, the XUV transmission increased via the effect of the dressing laser pulse, while at the 2 s to CB transition of Si and the 3 d to CB transition of Zr, the XUV transmission decreased. Furthermore, beats between the transition from 2 p1 /2 and 2 p3 /2 levels of Si and from 3 d3 /2 and 3 d5 /2 levels of Zr were observed with 20.7 fs and 3.6 fs periods.

  5. Two-photon photoemission from a copper cathode in an X -band photoinjector

    NASA Astrophysics Data System (ADS)

    Li, H.; Limborg-Deprey, C.; Adolphsen, C.; McCormick, D.; Dunning, M.; Jobe, K.; Raubenheimer, T.; Vrielink, A.; Vecchione, T.; Wang, F.; Weathersby, S.

    2016-02-01

    This paper presents two-photon photoemission from a copper cathode in an X -band photoinjector. We experimentally verified that the electron bunch charge from photoemission out of a copper cathode scales with laser intensity (I) square for 400 nm wavelength photons. We compare this two-photon photoemission process with the single photon process at 266 nm. Despite the high reflectivity (R ) of the copper surface for 400 nm photons (R =0.48 ) and higher thermal energy of photoelectrons (two-photon at 200 nm) compared to 266 nm photoelectrons, the quantum efficiency of the two-photon photoemission process (400 nm) exceeds the single-photon process (266 nm) when the incident laser intensity is above 300 GW /cm2 . At the same laser pulse energy (E ) and other experimental conditions, emitted charge scales inversely with the laser pulse duration. A thermal emittance of 2.7 mm-mrad per mm root mean square (rms) was measured on our cathode which exceeds by sixty percent larger compared to the theoretical predictions, but this discrepancy is similar to previous experimental thermal emittance on copper cathodes with 266 nm photons. The damage of the cathode surface of our first-generation X -band gun from both rf breakdowns and laser impacts mostly explains this result. Using a 400 nm laser can substantially simplify the photoinjector system, and make it an alternative solution for compact pulsed electron sources.

  6. High-Resolution and Low-Temperature Photoemission Spectroscopy at the Hisor Helical-Undulator Beamline

    NASA Astrophysics Data System (ADS)

    Arita, Masashi; Shimada, Kenya; Namatame, Hirofumi; Taniguchi, Masaki

    We report an experimental system dedicated for high-resolution and low-temperature photoemission spectroscopy installed on the helical-undulator beamline of a compact 700 MeV electron-storage ring (HiSOR) at Hiroshima University. A 3 m off-plane Eagle normal-incidence monochromator at the beamline covers the photon-energy range of hν = 4-40 eV. From the photoemission spectra near the Fermi edge of evaporated Au film, the total energy resolution was estimated to be 4.5 and 7.5 meV at hν = 7.1 and 22.6 eV, respectively. We have also performed photoemission measurements of Yb metal, which demonstrated highly bulk-sensitive spectra for the excitation by low energy photon. The high-resolution photoemission spectra of Y1 - xCaxTiO3 with x = 0.41 in the vicinity of the boundary between the metallic and insulating phases exhibited anomalous temperature dependence in comparison with those of normal metals.

  7. Electron photoemission from platinum and palladium microdeposits on glassy carbon into the solution

    SciTech Connect

    Yakushev, V.V.; Bagotskii, V.S.; Skundin, A.M.

    1984-08-01

    It was of interest to the authors to compare the electrocatalytic and photoemission properties of microdeposits in other systems. Platinum and palladium microdeposits on glassy carbon were selected as such systems in the present work. The procedure used in the photoemission measurements has been previously described. All measurements were conducted in 1 N KOH. A mercury-mercuric oxide electrode served as reference electrode. The true surface areas of the platinum microdeposits were measured potentiodynamically in terms of hydrogen adsorption and oxygen desorption, while that of the palladium microdeposits was measured in terms of oxygen desorption. The results of the present work yield the important conclusion that the changes which occur in the density of electronic states in the microdeposits because of their contact with the support depend on potential, i.e., on the position of the Fermi level. It is found that the enhancement of the photoemission currents is attended by an increase, and the depression of the photoemission currents is attended by a decrease in electrocatalytic activity.

  8. Electronic properties of Mn-phthalocyanine–C{sub 60} bulk heterojunctions: Combining photoemission and electron energy-loss spectroscopy

    SciTech Connect

    Roth, Friedrich; Lupulescu, Cosmin; Darlatt, Erik; Gottwald, Alexander; Eberhardt, Wolfgang

    2015-11-14

    The electronic properties of co-evaporated mixtures (blends) of manganese phthalocyanine and the fullerene C{sub 60} (MnPc:C{sub 60}) have been studied as a function of the concentration of the two constituents using two supplementary electron spectroscopic methods, photoemission spectroscopy (PES) and electron energy-loss spectroscopy (EELS) in transmission. Our PES measurements provide a detailed picture of the electronic structure measured with different excitation energies as well as different mixing ratios between MnPc and C{sub 60}. Besides a relative energy shift, the occupied electronic states of the two materials remain essentially unchanged. The observed energy level alignment is different compared to that of the related CuPc:C{sub 60} bulk heterojunction. Moreover, the results from our EELS investigations show that, despite the rather small interface interaction, the MnPc related electronic excitation spectrum changes significantly by admixing C{sub 60} to MnPc thin films.

  9. Direct Observation of Localized Spin Antiferromagnetic Transition in PdCrO2 by Angle-Resolved Photoemission Spectroscopy

    PubMed Central

    Noh, Han-Jin; Jeong, Jinwon; Chang, Bin; Jeong, Dahee; Moon, Hyun Sook; Cho, En-Jin; Ok, Jong Mok; Kim, Jun Sung; Kim, Kyoo; Min, B. I.; Lee, Han-Koo; Kim, Jae-Young; Park, Byeong-Gyu; Kim, Hyeong-Do; Lee, Seongsu

    2014-01-01

    We report the first case of the successful measurements of a localized spin antiferromagnetic transition in delafossite-type PdCrO2 by angle-resolved photoemission spectroscopy (ARPES). This demonstrates how to circumvent the shortcomings of ARPES for investigation of magnetism involved with localized spins in limited size of two-dimensional crystals or multi-layer thin films that neutron scattering can hardly study due to lack of bulk compared to surface. Also, our observations give direct evidence for the spin ordering pattern of Cr3+ ions in PdCrO2 suggested by neutron diffraction and quantum oscillation measurements, and provide a strong constraint that has to be satisfied by a microscopic mechanism for the unconventional anomalous Hall effect recently reported in this system. PMID:24419488

  10. Progress on PEEM3 - An Aberration Corrected X-Ray PhotoemissionElectron Microscope at the ALS

    SciTech Connect

    MacDowell, Alastair A.; Feng, J.; DeMello, A.; Doran, A.; Duarte,R.; Forest, E.; Kelez, N.; Marcus, M.A.; Miller, T.; Padmore, H.A.; Raoux, S.; Robin, D.; Scholl, A.; Schlueter, R.; Schmid, P.; Stohr, J.; Wan, W.; Wei, D.H.; Wu, Y.

    2006-05-20

    A new ultrahigh-resolution photoemission electron microscope called PEEM3 is being developed and built at the Advanced Light Source (ALS). An electron mirror combined with a much-simplified magnetic dipole separator is to be used to provide simultaneous correction of spherical and chromatic aberrations. It is installed on an elliptically polarized undulator (EPU) beamline, and will be operated with very high spatial resolution and high flux to study the composition, structure, electric and magnetic properties of complex materials. The instrument has been designed and is described. The instrumental hardware is being deployed in 2 phases. The first phase is the deployment of a standard PEEM type microscope consisting of the standard linear array of electrostatic electron lenses. The second phase will be the installation of the aberration corrected upgrade to improve resolution and throughput. This paper describes progress as the instrument enters the commissioning part of the first phase.

  11. Photoemission spectroscopy of magnetic and nonmagnetic impurities on the surface of the Bi2Se3 topological insulator.

    PubMed

    Valla, T; Pan, Z-H; Gardner, D; Lee, Y S; Chu, S

    2012-03-16

    Dirac-like surface states on surfaces of topological insulators have a chiral spin structure that suppresses backscattering and protects the coherence of these states in the presence of nonmagnetic scatterers. In contrast, magnetic scatterers should open the backscattering channel via the spin-flip processes and degrade the state's coherence. We present angle-resolved photoemission spectroscopy studies of the electronic structure and the scattering rates upon the adsorption of various magnetic and nonmagnetic impurities on the surface of Bi2Se3, a model topological insulator. We reveal a remarkable insensitivity of the topological surface state to both nonmagnetic and magnetic impurities in the low impurity concentration regime. Scattering channels open up with the emergence of hexagonal warping in the high-doping regime, irrespective of the impurity's magnetic moment.

  12. Laser intensity effects in carrier-envelope phase-tagged time of flight-photoemission electron microscopy

    NASA Astrophysics Data System (ADS)

    Chew, S. H.; Gliserin, A.; Schmidt, J.; Bian, H.; Nobis, S.; Schertz, F.; Kübel, M.; Yang, Y.-Y.; Loitsch, B.; Stettner, T.; Finley, J. J.; Späth, C.; Ouacha, H.; Azzeer, A. M.; Kleineberg, U.

    2016-04-01

    A time of flight-photoemission electron microscope is combined with a single-shot stereographic above-threshold ionization phase meter for studying attosecond control of electrons in tailored plasmonic nanostructures spatially and energetically via a carrier-envelope phase tagging technique. First carrier-envelope phase-resolved measurements of gold nanoparticles on gold plane and surface roughness from a gold film show an apparent carrier-envelope phase modulation with a period of π. This modulation is found to originate from an intensity dependence of the photoelectron spectra and the carrier-envelope phase measurement rather than from an intrinsic carrier-envelope phase dependence, which is confirmed by simulations. This useful finding suggests that intensity tagging should be considered for phase tagging experiments on plasmonic nanostructures with low carrier-envelope phase sensitivity in order to correct for the intensity-related carrier-envelope phase artifact.

  13. Formation of compensated defects in zinc magnesium oxides assignable from diffusion coefficients and hard x-ray photoemission

    NASA Astrophysics Data System (ADS)

    Ohsawa, Takeo; Sakaguchi, Isao; Ohashi, Naoki; Haneda, Hajime; Ryoken, Haruki; Matsumoto, Kenji; Hishita, Shunichi; Adachi, Yutaka; Ueda, Shigenori; Yoshikawa, Hideki; Kobayashi, Keisuke

    2009-01-01

    We studied metastable (Zn1-xMgx)O alloy films having a high MgO fraction, e.g., x =0.47, in excess of its solubility limit (x ≈0.15). Residual electron concentrations in the metastable films were close to those of the stable films having a smaller MgO fraction (x =0.07). In contrast to the electric conductivity, diffusivities of both cation and anion in the metastable films were surprisingly higher than those in the stable films, indicating that a high concentration of compensated defects were generated in the metastable alloy with a high MgO fraction. Photoemission spectroscopy confirmed the presence of ionized acceptors for charge compensation in the metastable (Zn1-xMgx)O.

  14. Two-photon photoemission of organic semiconductor molecules on silver(111)

    NASA Astrophysics Data System (ADS)

    Yang, Aram

    Angle- and time-resolved two-photon photoemission (2PPE) was used to study systems of organic semiconductors on Ag(111). The 2PPE studies focused on electronic behavior specific to interfaces and ultrathin films. Electron time dynamics and band dispersions were characterized for ultrathin films of a prototypical n-type planar aromatic hydrocarbon, PTCDA, and representatives from a family of p-type oligothiophenes. In PTCDA, electronic behavior was correlated with film morphology and growth modes. Within a few monolayers of the interface, image potential states and a LUMO+1 state were detected. The degree to which the LUMO+1 state exhibited a band mass less than a free electron mass depended on the crystallinity of the layer. Similarly, image potential states were measured to have free electron-like effective masses on ordered surfaces, and the effective masses increased with disorder within the thin film. Electron lifetimes were correlated with film growth modes, such that the lifetimes of electrons excited into systems created by layer-by-layer, amorphous film growth increased by orders of magnitude by only a few monolayers from the surface. Conversely, the decay dynamics of electrons in Stranski-Krastanov systems were limited by interaction with the exposed wetting layer, which limited the barrier to decay back into the metal. Oligothiophenes including monothiophene, quaterthiophene, and sexithiophene were deposited on Ag(111), and their electronic energy levels and effective masses were studied as a function of oligothiophene length. The energy gap between HOMO and LUMO decreased with increasing chain length, but effective mass was found to depend on domains from high- or low-temperature growth conditions rather than chain length. In addition, the geometry of the molecule on the surface, e.g., tilted or planar, substantially affected the electronic structure.

  15. Two-photon Photoemission of Organic Semiconductor Molecules on Ag(111)

    SciTech Connect

    Yang, Aram

    2008-05-01

    Angle- and time-resolved two-photon photoemission (2PPE) was used to study systems of organic semiconductors on Ag(111). The 2PPE studies focused on electronic behavior specific to interfaces and ultrathin films. Electron time dynamics and band dispersions were characterized for ultrathin films of a prototypical n-type planar aromatic hydrocarbon, PTCDA, and representatives from a family of p-type oligothiophenes.In PTCDA, electronic behavior was correlated with film morphology and growth modes. Within a fewmonolayers of the interface, image potential states and a LUMO+1 state were detected. The degree to which the LUMO+1 state exhibited a band mass less than a free electron mass depended on the crystallinity of the layer. Similarly, image potential states were measured to have free electron-like effective masses on ordered surfaces, and the effective masses increased with disorder within the thin film. Electron lifetimes were correlated with film growth modes, such that the lifetimes of electrons excited into systems created by layer-by-layer, amorphous film growth increased by orders of magnitude by only a few monolayers from the surface. Conversely, the decay dynamics of electrons in Stranski-Krastanov systems were limited by interaction with the exposed wetting layer, which limited the barrier to decay back into the metal.Oligothiophenes including monothiophene, quaterthiophene, and sexithiophene were deposited on Ag(111), and their electronic energy levels and effective masses were studied as a function of oligothiophene length. The energy gap between HOMO and LUMO decreased with increasing chain length, but effective mass was found to depend on domains from high- or low-temperature growth conditions rather than chain length. In addition, the geometry of the molecule on the surface, e.g., tilted or planar, substantially affected the electronic structure.

  16. Ultrafast Multiphoton Pump-probe Photoemission Excitation Pathways in Rutile TiO2(110)

    SciTech Connect

    Argondizzo, Adam; Cui, Xuefeng; Wang, Cong; Sun, Huijuan; Shang, Honghui; Zhao, Jin; Petek, Hrvoje

    2015-04-27

    We investigate the spectroscopy and photoinduced electron dynamics within the conduction band of reduced rutile TiO2(110) surface by multiphoton photoemission (mPP) spectroscopy with wavelength tunable ultrafast (!20 fs) laser pulse excitation. Tuning the mPP photon excitation energy between 2.9 and 4.6 eV reveals a nearly degenerate pair of new unoccupied states located at 2.73 ± 0.05 and 2.85 ± 0.05 eV above the Fermi level, which can be analyzed through the polarization and sample azimuthal orientation dependence of the mPP spectra. Based on the calculated electronic structure and optical transition moments, as well as related spectroscopic evidence, we assign these resonances to transitions between Ti 3d bands of nominally t2g and eg symmetry, which are split by crystal field. The initial states for the optical transition are the reduced Ti3+ states of t2g symmetry populated by formation oxygen vacancy defects, which exist within the band gap of TiO2. Furthermore,we studied the electron dynamics within the conduction band of TiO2 by three-dimensional time-resolved pump-probe interferometric mPP measurements. The spectroscopic and time-resolved studies reveal competition between 2PP and 3PP processes where the t2g-eg transitions in the 2PP process saturate, and are overtaken by the 3PP process initiated by the band-gap excitation from the valence band of TiO2.

  17. Nodal Quasiparticle Meltdown in Ultra-High Resolution Pump-Probe Angle-Resolved Photoemission

    SciTech Connect

    Graf, Jeff; Jozwiak, Chris; Smallwood, Chris L.; Eisaki, H.; Kaindl, Robert A.; Lee, Dung-Hai; Lanzara, Alessandra

    2011-06-03

    High-T{sub c} cuprate superconductors are characterized by a strong momentum-dependent anisotropy between the low energy excitations along the Brillouin zone diagonal (nodal direction) and those along the Brillouin zone face (antinodal direction). Most obvious is the d-wave superconducting gap, with the largest magnitude found in the antinodal direction and no gap in the nodal direction. Additionally, while antin- odal quasiparticle excitations appear only below T{sub c}, superconductivity is thought to be indifferent to nodal excitations as they are regarded robust and insensitive to T{sub c}. Here we reveal an unexpected tie between nodal quasiparticles and superconductivity using high resolution time- and angle-resolved photoemission on optimally doped Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8+{delta}} . We observe a suppression of the nodal quasiparticle spectral weight following pump laser excitation and measure its recovery dynamics. This suppression is dramatically enhanced in the superconducting state. These results reduce the nodal-antinodal dichotomy and challenge the conventional view of nodal excitation neutrality in superconductivity. The electronic structures of high-Tc cuprates are strongly momentum-dependent. This is one reason why the momentum-resolved technique of angle-resolved photoemission spectroscopy (ARPES) has been a central tool in the field of high-temperature superconductivity. For example, coherent low energy excitations with momenta near the Brillouin zone face, or antinodal quasiparticles (QPs), are only observed below T{sub c} and have been linked to superfluid density. They have therefore been the primary focus of ARPES studies. In contrast, nodal QPs, with momenta along the Brillouin zone diagonal, have received less attention and are usually regarded as largely immune to the superconducting transition because they seem insensitive to perturbations such as disorder, doping, isotope exchange, charge ordering, and temperature. Clearly

  18. Dirac cones, Floquet side bands, and theory of time-resolved angle-resolved photoemission

    NASA Astrophysics Data System (ADS)

    Farrell, Aaron; Arsenault, A.; Pereg-Barnea, T.

    2016-10-01

    Pump-probe techniques with high temporal resolution allow one to drive a system of interest out of equilibrium and at the same time probe its properties. Recent advances in these techniques open the door to studying new, nonequilibrium phenomena such as Floquet topological insulators and superconductors. These advances also necessitate the development of theoretical tools for understanding the experimental findings and predicting new ones. In the present paper, we provide a theoretical foundation to understand the nonequilibrium behavior of a Dirac system. We present detailed numerical calculations and simple analytic results for the time evolution of a Dirac system irradiated by light. These results are framed by appealing to the recently revitalized notion of side bands [A. Farrell and T. Pereg-Barnea, Phys. Rev. Lett. 115, 106403 (2015), 10.1103/PhysRevLett.115.106403; Phys. Rev. B 93, 045121 (2016), 10.1103/PhysRevB.93.045121], extended to the case of nonperiodic drive where the fast oscillations are modified by an envelope function. We apply this formalism to the case of photocurrent generated by a second probe pulse. We find that, under the application of circularly polarized light, a Dirac point only ever splits into two copies of side bands. Meanwhile, the application of linearly polarized light leaves the Dirac point intact while producing side bands. In both cases the population of the side bands are time dependent through their nonlinear dependence on the envelope of the pump pulse. Our immediate interest in this work is in connection to time- and angle-resolved photoemission experiments, where we find excellent qualitative agreement between our results and those in the literature [Wang et al., Science 342, 453 (2013), 10.1126/science.1239834]. However, our results are general and may prove useful beyond this particular application and should be relevant to other pump-probe experiments.

  19. Internal photoemission from plasmonic nanoparticles: comparison between surface and volume photoelectric effects.

    PubMed

    Uskov, Alexander V; Protsenko, Igor E; Ikhsanov, Renat S; Babicheva, Viktoriia E; Zhukovsky, Sergei V; Lavrinenko, Andrei V; O'Reilly, Eoin P; Xu, Hongxing

    2014-05-01

    We study the emission of photoelectrons from plasmonic nanoparticles into a surrounding matrix. We consider two mechanisms of electron emission from the nanoparticles--surface and volume ones--and use models for these two mechanisms which allow us to obtain analytical results for the photoelectron emission rate from a nanoparticle. Calculations have been carried out for a step potential at the surface of a spherical nanoparticle, and a simple model for the hot electron cooling has been used. We highlight the effect of the discontinuity of the dielectric permittivity at the nanoparticle boundary in the surface mechanism, which leads to a substantial (by ∼5 times) increase of the internal photoelectron emission rate from a nanoparticle compared to the case when such a discontinuity is absent. For a plasmonic nanoparticle, a comparison of the two photoeffect mechanisms was undertaken for the first time which showed that the surface photoeffect can in the general case be larger than the volume one, which agrees with the results obtained for a flat metal surface first formulated by Tamm and Schubin in their pioneering development of a quantum-mechanical theory of photoeffect in 1931. In accordance with our calculations, this possible predominance of the surface effect is based on two factors: (i) effective cooling of hot carriers during their propagation from the volume of the nanoparticle to its surface in the scenario of the volume mechanism and (ii) strengthening of the surface mechanism through the effect of the discontinuity of the dielectric permittivity at the nanoparticle boundary. The latter is stronger at relatively lower photon energies and correspondingly is more substantial for internal photoemission than for an external one. We show that in the general case, it is essential to take both mechanisms into account in the development of devices based on the photoelectric effect and when considering hot electron emission from a plasmonic nanoantenna.

  20. Direct angle resolved photoemission spectroscopy and superconductivity of strained high-Tc films

    NASA Astrophysics Data System (ADS)

    Pavuna, Davor; Ariosa, Daniel; Cloetta, Dominique; Cancellieri, Claudia; Abrecht, Mike

    2008-02-01

    Since 1997 we systematically perform direct angle resolved photoemission spectroscopy (ARPES) on in-situ grown thin (<30 nm) cuprate films. Specifically, we probe low-energy electronic structure and properties of high-T_{c} superconductors (HTSC) under different degrees of epitaxial ({compressive vs. tensile}) strain. In overdoped and underdoped in-plane compressed (the strain is induced by the choice of substrate) ≈15 nm thin La_{2-x}Sr_{x}CuO_{4} (LSCO) films we almost double T_{c} to 40 K, from 20 K and 24 K, respectively. Yet the Fermi surface (FS) remains essentially two-dimensional. In contrast, ARPES data under {tensile} strain exhibit the dispersion that is three-dimensional, yet T_{c} drastically decreases. It seems that the in-plane compressive strain tends to push the apical oxygen far away from the CuO_{2} plane, enhances the two-dimensional character of the dispersion and increases T_{c}, while the tensile strain acts in the opposite direction and the resulting dispersion is three-dimensional. We have established the shape of the FS for both cases, and all our data are consistent with other ongoing studies, like EXAFS. As the actual lattice of cuprates is like a `Napoleon-cake', i.e. rigid CuO_{2 } planes alternating with softer `reservoir', that distort differently under strain, our data rule out all oversimplified two-dimensional (rigid lattice) mean field models. The work is still in progress on optimized La-doped Bi-2201 films with enhanced T_{c}.

  1. Internal photoemission from plasmonic nanoparticles: comparison between surface and volume photoelectric effects

    NASA Astrophysics Data System (ADS)

    Uskov, Alexander V.; Protsenko, Igor E.; Ikhsanov, Renat S.; Babicheva, Viktoriia E.; Zhukovsky, Sergei V.; Lavrinenko, Andrei V.; O'Reilly, Eoin P.; Xu, Hongxing

    2014-04-01

    We study the emission of photoelectrons from plasmonic nanoparticles into a surrounding matrix. We consider two mechanisms of electron emission from the nanoparticles - surface and volume ones - and use models for these two mechanisms which allow us to obtain analytical results for the photoelectron emission rate from a nanoparticle. Calculations have been carried out for a step potential at the surface of a spherical nanoparticle, and a simple model for the hot electron cooling has been used. We highlight the effect of the discontinuity of the dielectric permittivity at the nanoparticle boundary in the surface mechanism, which leads to a substantial (by ~5 times) increase of the internal photoelectron emission rate from a nanoparticle compared to the case when such a discontinuity is absent. For a plasmonic nanoparticle, a comparison of the two photoeffect mechanisms was undertaken for the first time which showed that the surface photoeffect can in the general case be larger than the volume one, which agrees with the results obtained for a flat metal surface first formulated by Tamm and Schubin in their pioneering development of a quantum-mechanical theory of photoeffect in 1931. In accordance with our calculations, this possible predominance of the surface effect is based on two factors: (i) effective cooling of hot carriers during their propagation from the volume of the nanoparticle to its surface in the scenario of the volume mechanism and (ii) strengthening of the surface mechanism through the effect of the discontinuity of the dielectric permittivity at the nanoparticle boundary. The latter is stronger at relatively lower photon energies and correspondingly is more substantial for internal photoemission than for an external one. We show that in the general case, it is essential to take both mechanisms into account in the development of devices based on the photoelectric effect and when considering hot electron emission from a plasmonic nanoantenna.

  2. Photon-impenetrable, electron-permeable: the carbon nanotube forest as a medium for multiphoton thermal-photoemission.

    PubMed

    Vahdani Moghaddam, Mehran; Yaghoobi, Parham; Sawatzky, George A; Nojeh, Alireza

    2015-04-28

    Combining the photoelectric and thermionic mechanisms to generate free electrons has been of great interest since the early days of quantum physics as exemplified by the Fowler-DuBridge theory, and recently proposed for highly efficient solar conversion. We present experimental evidence of this combined effect over the entire range spanning room-temperature photoemission to thermionic emission. Remarkably, the optical stimulus alone is responsible for both heating and photoemission at the same time. Moreover, the current depends on optical intensity quadratically, indicating two-photon photoemission, for intensities of ca. 1-50 W/cm(2), which are orders of magnitude below the intensities required for two-photon photoemission from bulk metals. This surprising behavior appears to be enabled by the internal nanostructure of the carbon nanotube forest, which captures photons effectively, yet allows electrons to escape easily.

  3. Significant relaxation of residual negative carrier in polar Alq3 film directly detected by high-sensitivity photoemission

    NASA Astrophysics Data System (ADS)

    Kinjo, Hiroumi; Lim, Hyunsoo; Sato, Tomoya; Noguchi, Yutaka; Nakayama, Yasuo; Ishii, Hisao

    2016-02-01

    Tris(8-hydroxyquinoline)aluminum (Alq3) has been widely applied as a good electron-injecting layer (EIL) in organic light-emitting diodes. High-sensitivity photoemission measurement revealed a clear photoemission by visible light, although its ionization energy is 5.7 eV. This unusual photoemission is ascribed to Alq3 anions captured by positive polarization charges. The observed electron detachment energy of the anion was about 1 eV larger than the electron affinity reported by inverse photoemission. This difference suggests that the injected electron in the Alq3 layer is energetically relaxed, leading to the reduction in injection barrier. This nature is one of the reasons why Alq3 worked well as the EIL.

  4. Photon-impenetrable, electron-permeable: the carbon nanotube forest as a medium for multiphoton thermal-photoemission.

    PubMed

    Vahdani Moghaddam, Mehran; Yaghoobi, Parham; Sawatzky, George A; Nojeh, Alireza

    2015-04-28

    Combining the photoelectric and thermionic mechanisms to generate free electrons has been of great interest since the early days of quantum physics as exemplified by the Fowler-DuBridge theory, and recently proposed for highly efficient solar conversion. We present experimental evidence of this combined effect over the entire range spanning room-temperature photoemission to thermionic emission. Remarkably, the optical stimulus alone is responsible for both heating and photoemission at the same time. Moreover, the current depends on optical intensity quadratically, indicating two-photon photoemission, for intensities of ca. 1-50 W/cm(2), which are orders of magnitude below the intensities required for two-photon photoemission from bulk metals. This surprising behavior appears to be enabled by the internal nanostructure of the carbon nanotube forest, which captures photons effectively, yet allows electrons to escape easily. PMID:25769341

  5. Radiationless S 1 → S 0 phenyl deactivation pathway: an investigation of iodine-marked bi-phenyl on a silicon surface by means of time resolved core-level photoelectron spectroscopy

    NASA Astrophysics Data System (ADS)

    Michelswirth, Martin; Dachraoui, Hatem; Mattay, Jochen; Heinzmann, Ulrich

    2012-02-01

    The S 1 → S 0 radiationless deactivation of iodine terminated bi-phenyl immobilized on a silicon surface was probed by analysing the I4d signature (BE: 45.6 eV, 47.3 eV) by means of High Harmonic Generation (HHG) based photoelectron spectroscopy. Modifications of the 4d5/2,3/2 spectroscopic contents spanning about 0.2 ps after UV activation (266 nm) were verified as showing a transient molecular response character. A localization to the terminated phenyl substructure in the complex structural environment on the surface was ensured according to the core-level nature of the recorded I4d. The activation of the bi-phenyl achieved by UV irradiation, corresponding to the UV absorption band-edge, was verified as being dominated by a Bπ → Bπ* phenyl excitation. Time-Dependent Density Functional Theory (TD-DFT) modellings were therefore performed. They were matched to Configuration Interaction semi-empirical calculations (CI-MNDO) verifying the Rustagi-Ducuing relation. The simulated singlet-singlet excitation spectrum was referenced to the spectra of an iodine terminated monomer and a linear oligophenyl chain (N = 8). Thus the deactivation response studied was assigned to a conical intersection promoted ? reaction pathway.

  6. Valence electron photoemission spectrum of semiconductors: ab initio description of multiple satellites.

    PubMed

    Guzzo, Matteo; Lani, Giovanna; Sottile, Francesco; Romaniello, Pina; Gatti, Matteo; Kas, Joshua J; Rehr, John J; Silly, Mathieu G; Sirotti, Fausto; Reining, Lucia

    2011-10-14

    The experimental valence band photoemission spectrum of semiconductors exhibits multiple satellites that cannot be described by the GW approximation for the self-energy in the framework of many-body perturbation theory. Taking silicon as a prototypical example, we compare experimental high energy photoemission spectra with GW calculations and analyze the origin of the GW failure. We then propose an approximation to the functional differential equation that determines the exact one-body Green's function, whose solution has an exponential form. This yields a calculated spectrum, including cross sections, secondary electrons, and an estimate for extrinsic and interference effects, in excellent agreement with experiment. Our result can be recast as a dynamical vertex correction beyond GW, giving hints for further developments. PMID:22107408

  7. Shakeup in soft-x-ray emission. II. Plasmon satellites and x-ray photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Livins, Peteris; Schnatterly, S. E.

    1988-04-01

    We report the first observation of a plasmon satellite in the K emission spectrum of diamond. The previously identified plasmon satellites of Al and graphite are also presented, and data is compared with an oscillator model applicable to soft-x-ray emission and photoemission. The graphite satellite is shown to exhibit an anomalous location with respect to the parent emission. We report for the Al LI-LII,III core-core transitions a spin-orbit splitting of 0.42+/-0.02 eV with a Lorentzian width of 0.67+/-0.02 eV. The oscillator model applied to x-ray photoemission predicts a shift of the plasmon satellite with respect to the zero loss line as the final-electron kinetic energy is varied.

  8. TOF Electron Energy Analyzer for Spin and Angular Resolved Photoemission Spectroscopy

    SciTech Connect

    Lebedev, Gennadi; Jozwiak, Chris; Andresen, Nord; Lanzara, Alessandra; Hussain, Zahid

    2008-07-09

    Current pulsed laser and synchrotron x-ray sources provide new opportunities for Time-Of- Flight (TOF) based photoemission spectroscopy to increase photoelectron energy resolution and efficiency compared to current standard techniques. The principals of photoelectron timing front formation, temporal aberration minimization, and optimization of electron beam transmission are presented. We have developed these concepts into a high resolution Electron Optical Scheme (EOS) of a TOF Electron Energy Analyzer (TOF-EEA) for photoemission spectroscopy. The EOS of the analyzer includes an electrostatic objective lens, three columns of transport lenses and a 90 degree energy band pass filter (BPF). The analyzer has two modes of operation: Spectrometer Mode (SM) with straight passage of electrons through the EOS undeflected by the BPF, allowing the entire spectrum to be measured, and Monochromator Mode (MM) in which the BPF defines a certain energy window inside the scope of the electron energy spectrum.

  9. TOF Electron Energy Analyzer for Spin and Angular Resolved Photoemission Spectroscopy

    NASA Astrophysics Data System (ADS)

    Lebedev, Gennadi; Jozwiak, Chris; Andresen, Nord; Hussain, Zahid; Lanzara, Alessandra

    2007-03-01

    Current pulsed laser and synchrotron x-ray sources provide new opportunities for Time-Of- Flight (TOF) based photoemission spectroscopy to increase photoelectron energy resolution and efficiency compared to current standard techniques. The principals of photoelectron timing front formation, temporal aberration minimization, and optimization of electron beam transmission are presented. We have developed these concepts into a high resolution a TOF Electron Energy Analyzer for photoemission spectroscopy. The electron optical scheme of the analyzer includes an electrostatic objective lens, three columns of transport lenses and a 90 degree energy band pass filter (BPF). High efficiency exchange scattering based spin polarimeter [1] is used for electron spin detection. The analyzer support two modes of operation: Spectrometer Mode allowing the entire spectrum to be measured, and Monochromator Mode in which the BPF passes a specified energy window inside the scope of the electron energy spectrum. [1] J. Graf, C. Jozwiak, A. K. Schmid, Z. Hussain, and A. Lanzara, Physical. Rev. B 71, 144429 (2005)

  10. Interference of spin states in resonant photoemission induced by circularly polarized light from magnetized Gd

    SciTech Connect

    Mueller, N.; Khalil, T.; Pohl, M.; Uphues, T.; Heinzmann, U.; Polcik, M.; Rader, O.; Heigl, F.; Starke, K.; Fritzsche, S.; Kabachnik, N. M.

    2006-10-15

    We have observed the spin-state interference by measuring the photoelectron spin polarization in the resonant preedge 4d{yields}4f photoemission from magnetized Gd. The photoemission is induced by circularly polarized light which determines one preferential direction of electron spin orientation due to polarization transfer and spin-orbit interaction. Another direction perpendicular to the first one is determined by the target electron spin orientation connected with the target magnetization. We have measured the component of spin polarization perpendicular to those two directions which can only appear due to spin-state interference which implies coherence of the spin states produced by the two mechanisms of the photoelectron spin polarization.

  11. Quantum-electrodynamic treatment of photoemission by a single-electron wave packet

    NASA Astrophysics Data System (ADS)

    Corson, John P.; Peatross, Justin

    2011-11-01

    A quantum-field-theory description of photoemission by a laser-driven single-electron wave packet is presented. We show that, when the incident light is represented with multimode coherent states then, to all orders of perturbation theory, the relative phases of the electron's constituent momenta have no influence on the amount of scattered light. These results are extended using the Furry picture, where the (unidirectional) arbitrary incident light pulse is treated nonperturbatively with Volkov functions. This analysis increases the scope of our prior results in [Phys. Rev. APLRAAN1050-294710.1103/PhysRevA.84.053831 84, 053831 (2011)], which demonstrate that the spatial size of the electron wave packet does not influence photoemission.

  12. The role of angle-resolved photoemission in understanding the high temperature superconductors.

    SciTech Connect

    Campuzano, J. C.; Kaminski, A.; Fretwell, H.; Mesot, J.; Sato, T.; Takahashi, T.; Norman, M.; Randeria, M.; Kadowaki, K.; Hinks, D.; Univ. of Illinois at Chicago; Tohuku Univ.; Tata Inst.; Tsukuba Univ.

    2001-01-01

    The two-dimensional nature of the high temperature superconductors allows the determination of the energy-momentum relationship of electronic states by angle-resolved photoemission (ARPES). Furthermore, the shape of the ARPES spectra provides information on the many body interactions so prevalent in these materials. In this paper we review some results obtained by our group on the question of the existence of quasiparticles and their interactions.

  13. A sample holder with integrated laser optics for an ELMITEC photoemission electron microscope

    SciTech Connect

    Gierster, L.; Pape, L.; Ünal, A. A.; Kronast, F.

    2015-02-15

    We present a new sample holder compatible with ELMITEC Photoemission Electron Microscopes (PEEMs) containing an optical lens and a mirror. With the integrated optical elements, a laser beam is focused from the back side of the sample at normal incidence, yielding a minimum spot size of about 1 μm. This opens up new possibilities for local laser excitations in PEEM experiments such as imaging all-optical magnetization switching at a small length scale.

  14. Two-photon photoemission and the dynamics of electrons at interfaces

    SciTech Connect

    Padowitz, D.F.; Harris, C.B.; Jordan, R.E.; Lingle, R.L. Jr.; McNeill, J.D.; Merry, W.R.

    1994-01-01

    A new instrument for angle-resolved two-photon photoemission with exceptional sensitivity and energy resolution has allowed a detailed examination of the interaction of image-state electrons with adsorbates. In addition to measuring the electrostatic properties of molecular-thickness films, the technique serves as a probe of adsorbate growth modes, and provides new opportunities to explore the dynamics of electrons in well-controlled two-dimensional systems.

  15. Photoemission and the electronic properties of heavy fermions -- limitations of the Kondo model

    SciTech Connect

    Joyce, J.J.; Arko, A.J.; Andrews, A.B.

    1993-09-01

    The electronic properties of Yb-based heavy fermions have been investigated by means of high resolution synchrotron radiation photoemission and compared with predictions of the Kondo model. The Yb heavy fermion photoemission spectra show massive disagreement with the Kondo model predictions (as calculated within the Gunnarsson-Schonhammer computational method). Moreover, the Yb heavy fermion photoemission spectra give very strong indications of core-like characteristics and compare favorable to purely divalent Yb metal and core-like Lu 4f levels. The heavy fermions YbCu{sub 2}Si{sub 2}, YbAgCu{sub 4} and YbAl{sub 3} were measured and shown to have lineshapes much broader and deeper in binding energy than predicted by the Kondo model. The lineshape of the bulk component of the 4f emission for these three heavy fermion materials was compared with that from Yb metal and the Lu 4f levels in LuAl{sub 3}, the heavy fermion materials show no substantive spectroscopic differences from simple 4f levels observed in Yb metal and LuAl{sub 3}. Also, the variation with temperature of the 4f fineshape was measured for Yb metal and clearly demonstrates that phonon broadening plays a major role in 4f level lineshape analysis and must be accounted for before considerations of correlated electron resonance effects are presumed to be at work.

  16. Plasmonic Field Enhancement of Individual Nanoparticles by Correlated Scanning and Photoemission Electron Microscopy

    SciTech Connect

    Peppernick, Samuel J.; Joly, Alan G.; Beck, Kenneth M.; Hess, Wayne P.

    2011-01-21

    We present results of a combined two-photon photoemission and scanning electron microscopy investigation to determine the electromagnetic enhancement factors of silver-coated spherical nanoparticles deposited on an atomically flat mica substrate. Femtosecond laser excitation, of the nanoparticles, produces intense photoemission, attributed to near-resonant excitation of localized surface plasmons. Enhancement factors are determined by comparing the respective two-photon photoemission yield measured for equal areas between single nanoparticles to that of the surrounding flat surface. For s-polarized, 400 nm (~ 3.1 eV) femtosecond radiation a distribution of enhancement factors are found with a large percentage (77%) of the nanoparticles falling within a median range. A correlated scanning electron microscopy analysis demonstrated that the nanoparticles typifying the median of the distribution were characterized by ideal spherical shapes and defect-free morphologies. The single largest enhancement factors were in contrast produced by a very small percentage (8%) of the total, for which evidence of silver defect anomalies were found that contributed to the overall structure of the nanoparticle. Comparisons are made between the experimentally measured enhancement factors and previously reported theoretical predictions of the localized surface plasmon near-field intensities for isolated nanometer-sized silver spheres.

  17. Photoemission electron microscopy of localized surface plasmons in silver nanostructures at telecommunication wavelengths

    SciTech Connect

    Mårsell, Erik; Larsen, Esben W.; Arnold, Cord L.; Xu, Hongxing; Mauritsson, Johan; Mikkelsen, Anders

    2015-02-28

    We image the field enhancement at Ag nanostructures using femtosecond laser pulses with a center wavelength of 1.55 μm. Imaging is based on non-linear photoemission observed in a photoemission electron microscope (PEEM). The images are directly compared to ultra violet PEEM and scanning electron microscopy (SEM) imaging of the same structures. Further, we have carried out atomic scale scanning tunneling microscopy on the same type of Ag nanostructures and on the Au substrate. Measuring the photoelectron spectrum from individual Ag particles shows a larger contribution from higher order photoemission processes above the work function threshold than would be predicted by a fully perturbative model, consistent with recent results using shorter wavelengths. Investigating a wide selection of both Ag nanoparticles and nanowires, field enhancement is observed from 30% of the Ag nanoparticles and from none of the nanowires. No laser-induced damage is observed of the nanostructures neither during the PEEM experiments nor in subsequent SEM analysis. By direct comparison of SEM and PEEM images of the same nanostructures, we can conclude that the field enhancement is independent of the average nanostructure size and shape. Instead, we propose that the variations in observed field enhancement could originate from the wedge interface between the substrate and particles electrically connected to the substrate.

  18. Quasiparticle energy studies of bulk semiconductors, surfaces and nanotubes

    SciTech Connect

    Blase, X.F.

    1994-12-01

    Effects of many-body effects on electronic excitation energies (quasiparticle band structure) of these materials are explored. GW approximation, including local field effects, for self-energy operator is used to calculate quasi-particle energies. The newly discovered carbon nanotubes are studied; structural stability and band structures are calculated. BN nanotubes are also studied, and their stability is predicted. Unexpected electronic features are predicted for both systems. Filling of carbon nanotubes with metal atoms and the doping of BN nanotubes by carbon and other impurites is also studied. The occupied surface states at H/Si(111)-(1{times}1) surface are studied; it is shown that the electronic structure requires a full quasiparticle calculation even for this simple chemisorption system. The core level shift of the Si 2p levels for atoms near the H/Si(111)-(1{times}1) surface is calculated; a simple first order perturbation theory using pseudopotential and the local density approximation gives good results for the photoemission spectra of the core electrons. The quasiparticle energies of bulk hexagonal BN and those of an isolated BN sheet are studied; this provides an understanding of the quasiparticle band structure of BN nanotubes. A nearly free electron state with a wavefunction in the interlayer or vacuum region composes the bottom of the conduction bands. A mixed-space formalism is presented for calculating the dynamical screening effects and electron self-energy operator in solids; this provides an efficient algorithm to calculate quasiparticle energies for large systems.

  19. Electronic structure of aromatic amino acids studied by soft x-ray spectroscopy

    NASA Astrophysics Data System (ADS)

    Zhang, Wenhua; Carravetta, Vincenzo; Plekan, Oksana; Feyer, Vitaliy; Richter, Robert; Coreno, Marcello; Prince, Kevin C.

    2009-07-01

    The electronic structure of phenylalanine, tyrosine, tryptophan, and 3-methylindole in the gas phase was investigated by x-ray photoemission spectroscopy (XPS) and near edge x-ray absorption fine structure (NEXAFS) spectroscopy at the C, N, and O K-edges. The XPS spectra have been calculated for the four principal conformers of each amino acid, and the spectra weighted by the Boltzmann population ratios calculated from published free energies. Instead of the single peaks expected from the stoichiometry of the compounds, the N 1s core level spectra of phenylalanine and tryptophan show features indicating that more than one conformer is present. The calculations reproduce the experimental features. The C and O 1s spectra do not show evident effects due to conformational isomerism. The calculations predict that such effects are small for carbon, and for oxygen it appears that only broadening occurs. The carbon K-edge NEXAFS spectra of these aromatic amino acids are similar to the published data of the corresponding molecules in the solid state, but show more structure due to the higher resolution in the present study. The N K-edge spectra of tryptophan and 3-methylindole differ from phenylalanine and tyrosine, as the first two both contain a nitrogen atom located in a pyrrole ring. The nitrogen K-edge NEXAFS spectra of aromatic amino acids do not show any measurable effects due to conformational isomerism, in contrast to the photoemission results. Calculations support this result and show that variations of the vertical excitation energies of different conformers are small, and cannot be resolved in the present experiment. The O NEXAFS spectra of these three aromatic compounds are very similar to other, simpler amino acids, which have been studied previously.

  20. Momentum-resolved electronic structure at a buried interface from soft X-ray standing-wave angle-resolved photoemission

    NASA Astrophysics Data System (ADS)

    Gray, A. X.; Minár, J.; Plucinski, L.; Huijben, M.; Bostwick, A.; Rotenberg, E.; Yang, S.-H.; Braun, J.; Winkelmann, A.; Conti, G.; Eiteneer, D.; Rattanachata, A.; Greer, A. A.; Ciston, J.; Ophus, C.; Rijnders, G.; Blank, D. H. A.; Doennig, D.; Pentcheva, R.; Kortright, J. B.; Schneider, C. M.; Ebert, H.; Fadley, C. S.

    2013-10-01

    Angle-resolved photoemission spectroscopy (ARPES) is a powerful technique for the study of electronic structure, but it lacks a direct ability to study buried interfaces between two materials. We address this limitation by combining ARPES with soft X-ray standing-wave (SW) excitation (SWARPES), in which the SW profile is scanned through the depth of the sample. We have studied the buried interface in a prototypical magnetic tunnel junction La0.7Sr0.3MnO3/SrTiO3. Depth-and momentum-resolved maps of Mn 3d eg and t2g states from the central, bulk-like and interface-like regions of La0.7Sr0.3MnO3 exhibit distinctly different behavior consistent with a change in the Mn bonding at the interface. We compare the experimental results to state-of-the-art density-functional and one-step photoemission theory, with encouraging agreement that suggests wide future applications of this technique.

  1. Photoemission from real iron surfaces and its relationship to light penetration of the overlayer

    NASA Astrophysics Data System (ADS)

    Momose, Yoshihiro; Suzuki, Daisuke; Sakurai, Takao; Nakayama, Keiji

    2014-09-01

    We report the photoemission from real iron surfaces at elevated temperatures, called thermally assisted photoemission (TAPE), and its relationship to the X-ray photoelectron spectroscopy (XPS) results. TAPE measurements were carried out using a Geiger counter under a gaseous atmosphere of He containing 1 % isobutane vapor at normal atmospheric pressure. A sample was initially heated to temperatures ranging from 25 to 353 °C under light irradiation at a certain wavelength of 200, 210, 220, and 230 nm, and then, wavelength was scanned from 300 to 170 nm at the final temperature. The values of a constant related to electron photoemission probability, αA, where A is identical with the Richardson constant, and photothreshold (photoelectric work function), ϕ, were obtained from a plot of the square root of the electron photoemission intensity against the photon energy; the αA values increased with temperature, and the ϕ values also increased with temperature. From the Arrhenius plot, the αA was found to have an activation energy ΔE αA = 0.096 eV. The activation energies of the surface oxygen component ratio Z = O2-/(OH + O2-) and the surface elemental composition ratio X = Fe/(O + N + C + Fe) obtained from the XPS data were also determined from their Arrhenius plots: ΔE Z = 0.113 eV and ΔE X = 0.039 eV, respectively. From a close resemblance between the latter activation energies and those of the ΔE αA and the ΔE a = 0.112-0.040 eV for the quantum yields (Momose et al. in Appl Phys A. doi: 10.1007/s00339-014-8589-7, 2014), it was found that the increase in the intensity of the TAPE with temperature was strongly associated with the increase in the values of Z and X with temperature. It was therefore concluded that the ability of the surface overlayer to pass the incident light became a rate-determining step to start the photoemission, which was decisively controlled by the temperature-dependent surface oxygen components and surface compositions. The intensity

  2. Photoemission from real iron surfaces and its relationship to light penetration of the overlayer

    NASA Astrophysics Data System (ADS)

    Momose, Yoshihiro; Suzuki, Daisuke; Sakurai, Takao; Nakayama, Keiji

    2015-02-01

    We report the photoemission from real iron surfaces at elevated temperatures, called thermally assisted photoemission (TAPE), and its relationship to the X-ray photoelectron spectroscopy (XPS) results. TAPE measurements were carried out using a Geiger counter under a gaseous atmosphere of He containing 1 % isobutane vapor at normal atmospheric pressure. A sample was initially heated to temperatures ranging from 25 to 353 °C under light irradiation at a certain wavelength of 200, 210, 220, and 230 nm, and then, wavelength was scanned from 300 to 170 nm at the final temperature. The values of a constant related to electron photoemission probability, αA, where A is identical with the Richardson constant, and photothreshold (photoelectric work function), ϕ, were obtained from a plot of the square root of the electron photoemission intensity against the photon energy; the αA values increased with temperature, and the ϕ values also increased with temperature. From the Arrhenius plot, the αA was found to have an activation energy Δ E αA = 0.096 eV. The activation energies of the surface oxygen component ratio Z = O2-/(OH + O2-) and the surface elemental composition ratio X = Fe/(O + N + C + Fe) obtained from the XPS data were also determined from their Arrhenius plots: Δ E Z = 0.113 eV and Δ E X = 0.039 eV, respectively. From a close resemblance between the latter activation energies and those of the Δ E αA and the Δ E a = 0.112-0.040 eV for the quantum yields (Momose et al. in Appl Phys A. doi: 10.1007/s00339-014-8589-7, 2014), it was found that the increase in the intensity of the TAPE with temperature was strongly associated with the increase in the values of Z and X with temperature. It was therefore concluded that the ability of the surface overlayer to pass the incident light became a rate-determining step to start the photoemission, which was decisively controlled by the temperature-dependent surface oxygen components and surface compositions. The

  3. The Si(100)-Sb 2{times}1 and Ge(100) 2{times}1 surfaces: A multi-technique study

    SciTech Connect

    Richter, M.

    1993-08-01

    The electronic and geometric structures of the clean and Sb terminated Si(100)2{times}1 and Ge(100)-2{times}1 surfaces have been investigated using a multi-technique approach. Low energy electron diffraction (LEED), scanning tunneling microscopy (STM), surface extended X-ray absorption fine structure (SEXAFS) spectroscopy and angle-integrated core-level photoemission electron spectroscopy (PES) were employed to measure the surface symmetry, defect structure, relevant bond lengths, atomic coordination and electronic structure. By employing a multi-technique approach, it is possible to correlate changes in the geometric structure to specific features of the core-level lineshape of the substrate. This allows for the assignment of components of the core-level lineshape to be assigned to specific surface and near-surface atoms.

  4. Photoemission from activated gallium arsenide. II. Spin polarization versus kinetic energy analysis

    NASA Astrophysics Data System (ADS)

    Drouhin, H.-J.; Hermann, C.; Lampel, G.

    1985-03-01

    The spin polarization of the electrons emitted by a GaAs photocathode under circularly polarized light excitation is investigated as a function of the electron kinetic energy. The photocathode is activated by cesium and oxygen coadsorption under ultrahigh-vacuum conditions to achieve a negative electron affinity. The spin polarization is measured by Mott scattering. The study is performed with a very-high-energy resolution (20 meV), at 300 and 120 K, under well-focused Kr+-laser light excitation (photon energy ranging from 1.55 to 2.60 eV). The polarization-versus-energy distribution curves show typical features related to those observed in the energy distribution curves, which are analyzed in detail in the preceding paper [H.-J. Drouhin, C. Hermann, and G. Lampel, Phys. Rev. B 31, 3859 (1985)]. A model is developed to account for the largest measured polarization, which arises from electrons excited from the heavy-hole band and emitted without suffering any collision: A (2/3) maximum value is expected, which is reduced by spin precession in the internal D'yakonov and Perel' (DP) field, due to the absence of space-inversion symmetry in GaAs. An estimation of the hot-electron mean free path (~0.1 μm for photon energy above 1.96 eV) is deduced. The photoemission polarizations of the electrons excited from each of the two other valence bands are also calculated using a nonparabolic Kane band model. The L and X subsidiary minima give rise to polarization plateaus originating from energy relaxation in the band-bending region. The main contribution to the photocurrent is due to electrons which were thermalized in the central minimum of the bulk crystal and have relaxed their energy in the band-bending region prior to emission into vacuum. Their polarization is studied in relation with the luminescence polarization, measured on the same samples, in the framework of a one-dimensional diffusion model. An additional depolarization, occurring during the escape process, is

  5. Concentration and chemical-state profiles at heterogeneous interfaces with sub-nm accuracy from standing-wave ambient-pressure photoemission

    NASA Astrophysics Data System (ADS)

    Nemšák, Slavomír; Shavorskiy, Andrey; Karslioglu, Osman; Zegkinoglou, Ioannis; Rattanachata, Arunothai; Conlon, Catherine S.; Keqi, Armela; Greene, Peter K.; Burks, Edward C.; Salmassi, Farhad; Gullikson, Eric M.; Yang, See-Hun; Liu, Kai; Bluhm, Hendrik; Fadley, Charles S.

    2014-11-01

    Heterogeneous processes at solid/gas, liquid/gas and solid/liquid interfaces are ubiquitous in modern devices and technologies but often difficult to study quantitatively. Full characterization requires measuring the depth profiles of chemical composition and state with enhanced sensitivity to narrow interfacial regions of a few to several nm in extent over those originating from the bulk phases on either side of the interface. We show for a model system of NaOH and CsOH in an ~1-nm thick hydrated layer on α-Fe2O3 (haematite) that combining ambient-pressure X-ray photoelectron spectroscopy and standing-wave photoemission spectroscopy provides the spatial arrangement of the bulk and interface chemical species, as well as local potential energy variations, along the direction perpendicular to the interface with sub-nm accuracy. Standing-wave ambient-pressure photoemission spectroscopy is thus a very promising technique for measuring such important interfaces, with relevance to energy research, heterogeneous catalysis, electrochemistry, and atmospheric and environmental science.

  6. Chemical interaction at the Cu/PPA interface: an X-ray photoemission investigation

    NASA Astrophysics Data System (ADS)

    Polzonetti, G.; Russo, M. V.; Iucci, G.; Furlani, A.

    1993-11-01

    A coverage-dependent XPS investigation of the early stages of interaction between evaporated Cu and polyphenylacetylene (PPA) has been carried out. Copper films have been deposited at 300 K to a final thickness of about 5 monolayers. Overlayer and substrate core-level emission behaviour indicates the layer-by-layer growth of Cu on the PPA surface without interdiffusion. At low copper coverages a chemical interaction between the Cu adatoms and the substrate is observed by monitoring the changes occurring at the π å π∗ satellite feature of the C1s core-level line. We observe a decrease of intensity for this satellite as the copper coverage increases, interpreted in terms of the formation of a Cu-π complex with the phenyl ring. The Cu Auger spectra demonstrated the presence of positively charged metal atoms up to a coverage of ˜ 5 Å. In the submonolayer region the occurence of broadening of the C1s core level on the low binding energy side is observed together with a positive shift for the Cu2p 3/2 emission. Upon completion of the first copper monolayer these phenomena are removed. The observed behaviour can be accounted for in terms of differential charging with injection and trapping of charge into the PPA film from the Cu atoms that have not yet completed the first monolayer.

  7. Soft-x-ray fluorescence study of buried silicides in antiferromagnetically coupled Fe/Si multilayers

    SciTech Connect

    Carlisle, J.A.; Chaiken, A.; Michel, R.P.

    1997-04-01

    Multilayer films made by alternate deposition of two materials play an important role in electronic and optical devices such as quantum-well lasers and x-ray mirrors. In addition, novel phenomena like giant magnetoresistance and dimensional crossover in superconductors have emerged from studies of multilayers. While sophisticated x-ray techniques are widely used to study the morphology of multilayer films, progress in studying the electronic structure has been slower. The short mean-free path of low-energy electrons severely limits the usefulness of photoemission and related electron free path of low-energy electrons severely limit spectroscopies for multilayer studies. Soft x-ray fluorescence (SXF) is a bulk-sensitive photon-in, photon-out method to study valence band electronic states. Near-edge x-ray absorption fine-structure spectroscopy (NEXAFS) measured with partial photon yield can give complementary bulk-sensitive information about unoccupied states. Both these methods are element-specific since the incident x-ray photons excite electrons from core levels. By combining NEXAFS and SXF measurements on buried layers in multilayers and comparing these spectra to data on appropriate reference compounds, it is possible to obtain a detailed picture of the electronic structure. Results are presented for a study of a Fe/Si multilayer system.

  8. Deduction of the chemical state and the electronic structure of Nd{sub 2}Fe{sub 14}B compound from X-ray photoelectron spectroscopy core-level and valence-band spectra

    SciTech Connect

    Wang, Jing; Liang, Le; Zhang, Lanting E-mail: lmsun@sjtu.edu.cn; Sun, Limin E-mail: lmsun@sjtu.edu.cn; Hirano, Shinichi

    2014-10-28

    Characterization of chemical state and electronic structure of the technologically important Nd{sub 2}Fe{sub 14}B compound is attractive for understanding the physical nature of its excellent magnetic properties. X-ray photoelectron spectroscopy (XPS) study of such rare-earth compound is important and also challenging due to the easy oxidation of surface and small photoelectron cross-sections of rare-earth 4f electrons and B 2p electrons, etc. Here, we reported an investigation based on XPS spectra of Nd{sub 2}Fe{sub 14}B compound as a function of Ar ion sputtering time. The chemical state of Fe and that of B in Nd{sub 2}Fe{sub 14}B compound can be clearly determined to be 0 and −3, respectively. The Nd in Nd{sub 2}Fe{sub 14}B compound is found to have the chemical state of close to +3 instead of +3 as compared with the Nd in Nd{sub 2}O{sub 3}. In addition, by comparing the valence-band spectrum of Nd{sub 2}Fe{sub 14}B compound to that of the pure Fe, the contributions from Nd, Fe, and B to the valence-band structure of Nd{sub 2}Fe{sub 14}B compound is made more clear. The B 2p states and B 2s states are identified to be at ∼11.2 eV and ∼24.6 eV, respectively, which is reported for the first time. The contribution from Nd 4f states can be identified both in XPS core-level spectrum and XPS valence-band spectrum. Although Nd 4f states partially hybridize with Fe 3d states, Nd 4f states are mainly localized in Nd{sub 2}Fe{sub 14}B compound.

  9. Photoemission determination of the band diagram of the Te/CdTe interface

    NASA Astrophysics Data System (ADS)

    Niles, David W.; Li, Xiaonan; Sheldon, Peter

    1995-05-01

    A band diagram of the Te/CdTe interface was believed to be a prerequisite in understanding how the Te layer on the CdTe surface lowered the resistance of contacts to CdTe solar cell devices. A two-stage experiment was therefore designed. First, the application of x-ray photoelectron and Auger electron spectroscopies was discussed to comprehend the etching process. Second, the valence-band offset by vacuum deposition of Te on a sputtered CdTe surface was measured employing ultraviolet photoemission spectroscopy.

  10. Measurement of Electron Beam Polarization from Unstrained Bulk GaAs via Two Photon Photoemission

    SciTech Connect

    J L McCarter, T J Gay, J Hansknecht, M Poelker, M L Stutzman

    2011-06-01

    This paper describes measurements of the beam polarization and quantum efficiency for photoemission using two-photon excitation from unstrained bulk GaAs illuminated with pulsed, high intensity 1560nm laser light. Quantum efficiency is linearly proportional to 1560nm peak laser intensity, which was varied in three independent ways, indicating that the emitted electrons are promoted from the valence to the conduction band via two-photon absorption. Beam polarization was measured using a microMott polarimeter, with a value of 16.8(4)% polarization at 1560nm, which is roughly half the measured value of 33.4(8)% using 778 nm light.

  11. X-ray photoemission analysis of chemically modified TlBr surfaces for improved radiation detectors

    DOE PAGES

    Nelson, A. J.; Voss, L. F.; Beck, P. R.; Graff, R. T.; Conway, A. M.; Nikolic, R. J.; Payne, S. A.; Lee, J. -S.; Kim, H.; Cirignano, L.; et al

    2013-01-12

    We subjected device-grade TlBr to various chemical treatments used in room temperature radiation detector fabrication to determine the resulting surface composition and electronic structure. As-polished TlBr was treated separately with HCl, SOCl2, Br:MeOH and HF solutions. High-resolution photoemission measurements on the valence band electronic structure and Tl 4f, Br 3d, Cl 2p and S 2p core lines were used to evaluate surface chemistry and shallow heterojunction formation. Surface chemistry and valence band electronic structure were correlated with the goal of optimizing the long-term stability and radiation response.

  12. Simple surface structure determination from Fourier transforms of angle-resolved photoemission extended fine structure

    SciTech Connect

    Zheng, Y. |; Shirley, D.A.

    1995-02-01

    The authors show by Fourier analyses of experimental data, with no further treatment, that the positions of all the strong peaks in Fourier transforms of angle-resolved photoemission extended fine structure (ARPEFS) from adsorbed surfaces can be explicitly predicted from a trial structure with an accuracy of about {+-} 0.3 {angstrom} based on a single-scattering cluster model together with the concept of a strong backscattering cone, and without any additional analysis. This characteristic of ARPEFS Fourier transforms can be developed as a simple method for determining the structures of adsorbed surfaces to an accuracy of about {+-} 0.1 {angstrom}.

  13. Laser-based spin- and angle-resolved photoemission spectroscopy for rapid, high-resolution measurements

    NASA Astrophysics Data System (ADS)

    Gotlieb, Kenneth; Bostwick, Aaron; Hussain, Zahid; Lanzara, Alessandra; Jozwiak, Christopher

    2014-03-01

    A unique spin-and angle-resolved photoemission spectrometer (spin-ARPES) is coupled with a 6 eV laser to achieve unprecedented measurements of near-EF physics in topological insulators and Rashba systems. The pairing of the spin-ARPES system with the laser allows for energy and angular resolutions never before seen in a spin-ARPES experiment. Most importantly, the high efficiency of the system and high photon flux of the laser make measurements very rapid, permitting exploration of a large experimental phase space.

  14. Orientation-Dependent C60 Electronic Structures Revealed byPhotoemission Spectroscopy

    SciTech Connect

    Brouet, V.; Yang, W.L.; Zhou, X.J.; Choi, H.J.; Louie, S.G.; Cohen, M.L.; Goldoni, A.; Parmigiani, F.; Hussain, Z.; Shen, Z.X.

    2004-11-05

    We observe, with angle-resolved photoemission, a dramatic change in the electronic structure of two C60 monolayers, deposited,respectively, on Ag (111) and (100) substrates, and similarly doped with potassium to half filling of the C60 lowest unoccupied molecular orbital.The Fermi surface symmetry, the bandwidth, and the curvature of the dispersion at Gamma point are different. Orientations of the C60molecules on the two substrates are known to be the main structural difference between the two monolayers, and we present new band-structure calculations for some of these orientations. We conclude that orientations play a key role in the electronic structure of fullerides.

  15. Ultrahigh-resolution spin-resolved photoemission spectrometer with a mini Mott detector.

    PubMed

    Souma, S; Takayama, A; Sugawara, K; Sato, T; Takahashi, T

    2010-09-01

    We have developed an ultrahigh-resolution spin-resolved photoemission spectrometer with a highly efficient mini Mott detector and an intense xenon plasma discharge lamp. The spectrometer achieves the energy resolutions of 0.9 and 8 meV for non-spin-resolved and spin-resolved modes, respectively. Three-dimensional spin-polarization is determined by using a 90° electron deflector situated before the Mott detector. The performance of spectrometer is demonstrated by observation of a clear Rashba splitting of the Bi(111) surface states.

  16. An ultrafast electron microscope gun driven by two-photon photoemission from a nanotip cathode

    SciTech Connect

    Bormann, Reiner; Strauch, Stefanie; Schäfer, Sascha Ropers, Claus

    2015-11-07

    We experimentally and numerically investigate the performance of an advanced ultrafast electron source, based on two-photon photoemission from a tungsten needle cathode incorporated in an electron microscope gun geometry. Emission properties are characterized as a function of the electrostatic gun settings, and operating conditions leading to laser-triggered electron beams of very low emittance (below 20 nm mrad) are identified. The results highlight the excellent suitability of optically driven nano-cathodes for the further development of ultrafast transmission electron microscopy.

  17. Whispering gallery mode photoemission from self-assembled poly-para-phenylenevinylene microspheres

    SciTech Connect

    Kushida, Soh; Yamamoto, Yohei; Braam, Daniel; Lorke, Axel

    2015-12-31

    Poly[2-methoxy-5-(3,7-dimethyloctyloxy)-1,4-phenylenevinylene] (MDMOPPV) self-assembles to form well-defined spheres with several micrometers in diameter upon addition of a methanol vapor into a chloroform solution of MDMOPPV. The single sphere of MDMOPPV with 5.7 µm diameter exhibits whispering gallery mode (WGM) photoemission upon excitation with focused laser beam. The periodic emission lines are characterized by transverse electric and magnetic WGMs, and Q-factor reaches ∼345 at the highest.

  18. Theory of photoemission from cesium antimonide using an alpha-semiconductor model

    NASA Astrophysics Data System (ADS)

    Jensen, Kevin L.; Jensen, Barbara L.; Montgomery, Eric J.; Feldman, Donald W.; O'Shea, Patrick G.; Moody, Nathan

    2008-08-01

    A model of photoemission from cesium antimonide (Cs3Sb) that does not rely on adjustable parameters is proposed and compared to the experimental data of Spicer [Phys. Rev. 112, 114 (1958)] and Taft and Philipp [Phys. Rev. 115, 1583 (1959)]. It relies on the following components for the evaluation of all relevant parameters: (i) a multidimensional evaluation of the escape probability from a step-function surface barrier, (ii) scattering rates determined using a recently developed alpha-semiconductor model, and (iii) evaluation of the complex refractive index using a harmonic oscillator model for the evaluation of reflectivity and extinction coefficient.

  19. Ultrahigh-resolution spin-resolved photoemission spectrometer with a mini Mott detector

    SciTech Connect

    Souma, S.; Sugawara, K.; Takayama, A.; Sato, T.; Takahashi, T.

    2010-09-15

    We have developed an ultrahigh-resolution spin-resolved photoemission spectrometer with a highly efficient mini Mott detector and an intense xenon plasma discharge lamp. The spectrometer achieves the energy resolutions of 0.9 and 8 meV for non-spin-resolved and spin-resolved modes, respectively. Three-dimensional spin-polarization is determined by using a 90 deg. electron deflector situated before the Mott detector. The performance of spectrometer is demonstrated by observation of a clear Rashba splitting of the Bi(111) surface states.

  20. Standing-wave excited soft x-ray photoemission microscopy: application to Co microdot magnetic arrays

    SciTech Connect

    Gray, Alexander; Kronast, Florian; Papp, Christian; Yang, See-Hun; Cramm, Stefan; Krug, Ingo P.; Salmassi, Farhad; Gullikson, Eric M.; Hilken, Dawn L.; Anderson, Erik H.; Fischer, Peter; Durr, Hermann A.; Schneider, Claus M.; Fadley, Charles S.

    2010-10-29

    We demonstrate the addition of depth resolution to the usual two-dimensional images in photoelectron emission microscopy (PEEM), with application to a square array of circular magnetic Co microdots. The method is based on excitation with soft x-ray standing-waves generated by Bragg reflection from a multilayer mirror substrate. Standing wave is moved vertically through sample simply by varying the photon energy around the Bragg condition. Depth-resolved PEEM images were obtained for all of the observed elements. Photoemission intensities as functions of photon energy were compared to x-ray optical calculations in order to quantitatively derive the depth-resolved film structure of the sample.

  1. Low-energy excitations in α- and γ-Ce observed by photoemission

    NASA Astrophysics Data System (ADS)

    Patthey, F.; Delley, B.; Schneider, W.-D.; Baer, Y.

    1985-09-01

    uv-photoemission spectra of the α- and γ-phases of Ce have been measured with an unprecedented resolution (20 meV). A detailed many-body calculation based on the Anderson impurity model and including the 4f1 spin-orbit splitting has been performed. It accounts perfectly for the fine structures observed in the spectra. Within the energy range corresponding to the ground-state lowering by the f-d hybridization, the f contribution to the spectra reveals the density of low-energy excitations culminating at EF.

  2. Photoemission electron microscopy and scanning electron microscopy of Magnetospirillum magnetotacticum's magnetosome chains.

    PubMed

    Keutner, Christoph; von Bohlen, Alex; Berges, Ulf; Espeter, Philipp; Schneider, Claus M; Westphal, Carsten

    2014-10-01

    Magnetotactic bacteria are of great interdisciplinary interest, since a vast field of applications from magnetic recording media to medical nanorobots is conceivable. A key feature for a further understanding is the detailed knowledge about the magnetosome chain within the bacteria. We report on two preparation procedures suitable for UHV experiments in reflective geometry. Further, we present the results of scanning electron microscopy, as well as the first photoemission electron microscopy experiments, both accessing the magnetosomes within intact magnetotactic bacteria and compare these to scanning electron microscopy data from the literature. From the images, we can clearly identify individual magnetosomes within their chains.

  3. Gauge invariance in the theoretical description of time-resolved angle-resolved pump/probe photoemission spectroscopy

    SciTech Connect

    Freericks, J. K.; Krishnamurthy, H. R.; Sentef, M. A.; Devereaux, T. P.

    2015-10-01

    Nonequilibrium calculations in the presence of an electric field are usually performed in a gauge, and need to be transformed to reveal the gauge-invariant observables. In this work, we discuss the issue of gauge invariance in the context of time-resolved angle-resolved pump/probe photoemission. If the probe is applied while the pump is still on, one must ensure that the calculations of the observed photocurrent are gauge invariant. We also discuss the requirement of the photoemission signal to be positive and the relationship of this constraint to gauge invariance. We end by discussing some technical details related to the perturbative derivation of the photoemission spectra, which involve processes where the pump pulse photoexcites electrons due to nonequilibrium effects.

  4. Photoemission and optical properties of C{sub 60} fullerites

    SciTech Connect

    Shirley, E.L.; Louie, S.G. |

    1994-08-01

    A theory is presented for excitations in undoped, solid C{sub 60} involving addition or removal of an electron, as well as creation of an electron-hole pair. Excitation energies are computed using a quasiparticle description of electrons and holes, plus a model for electron-hole interactions. Results are compared with those of direct and inverse photoelectron and optical absorption spectroscopy studies. Reasonable agreement is found in such comparisons, while more complete modeling of experimental spectra might include neglected matrix-element and vibrational effects. These results give values for simple, conceptual parameters, such as a molecular Hubbard U. Some results could also be relevant in doped fullerites.

  5. A combined droplet train and ambient pressure photoemission spectrometer for the investigation of liquid/vapor interfaces

    SciTech Connect

    Starr, David E.; Wong, Ed K.; Worsnop, Douglas R.; Wilson, Kevin R.; Bluhm, Hendrik

    2008-05-01

    We describe a combined ambient pressure photoelectron spectroscopy/droplet train apparatus for investigating the nature and heterogeneous chemistry of liquid/vapor interfaces. In this instrument a liquid droplet train with typical droplet diameters from 50...150 {micro}m is produced by a vibrating orifice aerosol generator (VOAG). The droplets are irradiated by soft X-rays (100...1500 eV) in front of the entrance aperture of a differentially pumped electrostatic lens system that transfers the emitted electrons into a conventional hemispherical electron analyzer. The photoemission experiments are performed at background pressures of up to several Torr, which allows the study of environmentally important liquid/vapor interfaces, in particular aqueous solutions, under equilibrium conditions. The exposure time of the droplet surface to the background gases prior to the XPS measurement can be varied, which will allow future kinetic measurements of gas uptake on liquid surfaces. As an example, a measurement of the surface composition of a {chi} = 0.21 aqueous methanol solution is presented. The concentration of methanol at the vapor/liquid interface is enhanced by a factor of about 3 over the bulk value, while the expected bulk value is recovered at depths larger than about 1.5 nm.

  6. Low-energy inverse photoemission spectroscopy using a high-resolution grating spectrometer in the near ultraviolet range.

    PubMed

    Yoshida, Hiroyuki

    2013-10-01

    An inverse photoemission spectroscopy (IPES) apparatus using a Czerny-Turner grating spectrometer is demonstrated. Previous IPES instruments based on grating spectrometers used a concave grating and operated in the vacuum ultraviolet range. The reflectance of such gratings is lower than 20% and the aberration cannot be finely corrected leading to an energy resolution of up to 0.1 eV. In the present study, employing the low energy IPES regime [H. Yoshida, Chem. Phys. Lett. 539-540, 180 (2012)], incident electrons with a kinetic energy below 5 eV are used, while photon emission in the range of between 250 and 370 nm is analyzed with a 10-cm Czerny-Turner grating spectrometer. The signal intensity is at least 30 times higher than the previous apparatus. The resolution of photon detection is set at 0.07 eV though the ultimate resolution is one order of magnitude higher. The experiment is performed both by sweeping the electron energy (isochromat mode) and by simultaneously analyzing the photon of whole wavelength range (tunable photon energy mode).

  7. Low-energy inverse photoemission spectroscopy using a high-resolution grating spectrometer in the near ultraviolet range

    SciTech Connect

    Yoshida, Hiroyuki

    2013-10-15

    An inverse photoemission spectroscopy (IPES) apparatus using a Czerny-Turner grating spectrometer is demonstrated. Previous IPES instruments based on grating spectrometers used a concave grating and operated in the vacuum ultraviolet range. The reflectance of such gratings is lower than 20% and the aberration cannot be finely corrected leading to an energy resolution of up to 0.1 eV. In the present study, employing the low energy IPES regime [H. Yoshida, Chem. Phys. Lett. 539–540, 180 (2012)], incident electrons with a kinetic energy below 5 eV are used, while photon emission in the range of between 250 and 370 nm is analyzed with a 10-cm Czerny-Turner grating spectrometer. The signal intensity is at least 30 times higher than the previous apparatus. The resolution of photon detection is set at 0.07 eV though the ultimate resolution is one order of magnitude higher. The experiment is performed both by sweeping the electron energy (isochromat mode) and by simultaneously analyzing the photon of whole wavelength range (tunable photon energy mode)

  8. Determination of the Fermi surface in high-T{sub c} superconductors by angle-resolved photoemission spectroscopy

    SciTech Connect

    Mesot, J.; Randeria, M.; Norman, M. R.; Kaminski, A.; Fretwell, H. M.; Campuzano, J. C.; Ding, H.; Takeuchi, T.; Sato, T.; Yokoya, T.

    2001-06-01

    We study the normal-state electronic excitations probed by angle-resolved photoemission spectroscopy (ARPES) in Bi{sub 1.6}Pb{sub 0.4}Sr{sub 2}CuO{sub 6} (Bi2201) and Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8+{delta}} (Bi2212). Our main goal is to establish explicit criteria for determining the Fermi surface from ARPES data on strongly interacting systems where sharply defined quasiparticles do not exist and the dispersion is very weak in parts of the Brillouin zone. Additional complications arise from strong matrix element variations within the zone. We present detailed results as a function of incident photon energy, and show simple experimental tests to distinguish between an intensity drop due to matrix element effects and spectral weight loss due to a Fermi crossing. We reiterate the use of polarization selection rules in disentangling the effect of umklapps due to the BiO superlattice in Bi2212. We conclude that, despite all the complications, the Fermi surface can be determined unambiguously; it is a single large hole barrel centered about ({pi},{pi}) in both materials.

  9. A combined droplet train and ambient pressure photoemission spectrometer for the investigation of liquid/vapor interfaces.

    PubMed

    Starr, David E; Wong, Ed K; Worsnop, Douglas R; Wilson, Kevin R; Bluhm, Hendrik

    2008-06-01

    We describe a combined ambient pressure photoelectron spectroscopy/droplet train apparatus for investigating the nature and heterogeneous chemistry of liquid/vapor interfaces. In this instrument a liquid droplet train with typical droplet diameters from 50-150 mum is produced by a vibrating orifice aerosol generator (VOAG). The droplets are irradiated by soft X-rays (100-1500 eV) in front of the entrance aperture of a differentially pumped electrostatic lens system that transfers the emitted electrons into a conventional hemispherical electron analyzer. The photoemission experiments are performed at background pressures of up to several Torr, which allows the study of environmentally important liquid/vapor interfaces, in particular aqueous solutions, under equilibrium conditions. The exposure time of the droplet surface to the background gases prior to the XPS measurement can be varied, which will allow future kinetic measurements of gas uptake on liquid surfaces. As an example, a measurement of the surface composition of a chi = 0.21 aqueous methanol solution is presented. The concentration of methanol at the vapor/liquid interface is enhanced by a factor of about 3 over the bulk value, while the expected bulk value is recovered at depths larger than about 1.5 nm.

  10. Direct Observation of Localized Spin Antiferromagnetic Transition in PdCrO2 by Angle-Resolved Photoemission Spectroscopy

    NASA Astrophysics Data System (ADS)

    Noh, Han-Jin; Jeong, Jinwon; Chang, Bin; Jeong, Dahee; Moon, Hyun Sook; Cho, En-Jin; Ok, Jong Mok; Kim, Jun Sung; Kim, Kyoo; Min, B. I.; Lee, Han-Koo; Kim, Jae-Young; Park, Byeong-Gyu; Kim, Hyeong-Do; Lee, Seongsu

    2014-03-01

    We report the first case of the successful measurements of a localized spin antiferromagnetic transition in delafossite-type PdCrO2 by angle-resolved photoemission spectroscopy (ARPES). This demonstrates how to circumvent the shortcomings of ARPES for investigation of magnetism involved with localized spins in limited size of two-dimensional crystals or multi-layer thin films that neutron scattering can hardly study due to lack of bulk compared to surface. Also, our observations give direct evidence for the spin ordering pattern of Cr3+ ions in PdCrO2 suggested by neutron diffraction and quantum oscillation measurements, and provide a strong constraint that has to be satisfied by a microscopic mechanism for the unconventional anomalous Hall effect recently reported in this system. This work was supported by the National Research Foundation (NRF) of Korea Grant funded by the Korean Government (MEST) (Nos. 2010-0010771 and 2012M2B2A4029607). K.K. and B.I.M. acknowledge the support of NRF (Nos. 2009-0079947 and 2011-0025237) and KISTI.

  11. Angle-resolved photoemission spectroscopy with a femtosecond high harmonic light source using a two-dimensional imaging electron analyzer

    NASA Astrophysics Data System (ADS)

    Mathias, S.; Miaja-Avila, L.; Murnane, M. M.; Kapteyn, H.; Aeschlimann, M.; Bauer, M.

    2007-08-01

    An experimental setup for time- and angle-resolved photoemission spectroscopy using a femtosecond 1kHz high harmonic light source and a two-dimensional electron analyzer for parallel energy and momentum detection is presented. A selection of the 27th harmonic (41.85eV) from the harmonic spectrum of the light source is achieved with a multilayer Mo /Si double mirror monochromator. The extinction efficiency of the monochromator in selecting this harmonic is shown to be better than 7:1, while the transmitted bandwidth of the selected harmonic is capable of supporting temporal pulse widths as short as 3fs. The recorded E(k ) photoelectron spectrum from a Cu(111) surface demonstrates an angular resolution of better than 0.6° (=0.03Å-1 at Ekin ,e=36eV). Used in a pump-probe configuration, the described experimental setup represents a powerful experimental tool for studying the femtosecond dynamics of ultrafast surface processes in real time.

  12. Exploring three-dimensional orbital imaging with energy-dependent photoemission tomography

    PubMed Central

    Weiß, S.; Lüftner, D.; Ules, T.; Reinisch, E. M.; Kaser, H.; Gottwald, A.; Richter, M.; Soubatch, S.; Koller, G.; Ramsey, M. G.; Tautz, F. S.; Puschnig, P.

    2015-01-01

    Recently, it has been shown that experimental data from angle-resolved photoemission spectroscopy on oriented molecular films can be utilized to retrieve real-space images of molecular orbitals in two dimensions. Here, we extend this orbital tomography technique by performing photoemission initial state scans as a function of photon energy on the example of the brickwall monolayer of 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA) on Ag(110). The overall dependence of the photocurrent on the photon energy can be well accounted for by assuming a plane wave for the final state. However, the experimental data, both for the highest occupied and the lowest unoccupied molecular orbital of PTCDA, exhibits an additional modulation attributed to final state scattering effects. Nevertheless, as these effects beyond a plane wave final state are comparably small, we are able, with extrapolations beyond the attainable photon energy range, to reconstruct three-dimensional images for both orbitals in agreement with calculations for the adsorbed molecule. PMID:26437297

  13. Circular Dichroism Observed by Photoemission from Ultrathin Bi2Te3 Films

    NASA Astrophysics Data System (ADS)

    Xu, Cai-Zhi; Liu, Yang; Yukawa, Ryu; Zhang, Long-Xiang; Miller, Tom; Chiang, Tai-Chang

    2015-03-01

    Circular dichroism (CD) observed by photoemission from the surface states of topological insulators has drawn much interest. It was initially attributed to the spin polarization or chiral orbital momentum of the initial states, but later proven to also involve the final states. The detailed mechanism remains controversial. To address this question, we have performed measurements of ultrathin films of the prototypical topological insulator Bi2Te3 over a wide range of film thickness and photon energy. The results show that the CD depends not only on the photon energy, but also on the film thickness in a nontrivial manner. A theoretical model has been developed that involves dipole transition, surface photoemission, and spin-orbit coupling. The computed results are in good agreement with the general trends of the data including sign reversals as a function of photon energy and film thickness. The complex behavior of the measured CD function is partially caused by modifications of both the initial and final states in the thin film geometry.

  14. Solar energy conversion via hot electron internal photoemission in metallic nanostructures: Efficiency estimates

    SciTech Connect

    Leenheer, Andrew J.; Narang, Prineha; Atwater, Harry A.; Lewis, Nathan S.

    2014-04-07

    Collection of hot electrons generated by the efficient absorption of light in metallic nanostructures, in contact with semiconductor substrates can provide a basis for the construction of solar energy-conversion devices. Herein, we evaluate theoretically the energy-conversion efficiency of systems that rely on internal photoemission processes at metal-semiconductor Schottky-barrier diodes. In this theory, the current-voltage characteristics are given by the internal photoemission yield as well as by the thermionic dark current over a varied-energy barrier height. The Fowler model, in all cases, predicts solar energy-conversion efficiencies of <1% for such systems. However, relaxation of the assumptions regarding constraints on the escape cone and momentum conservation at the interface yields solar energy-conversion efficiencies as high as 1%–10%, under some assumed (albeit optimistic) operating conditions. Under these conditions, the energy-conversion efficiency is mainly limited by the thermionic dark current, the distribution of hot electron energies, and hot-electron momentum considerations.

  15. Ultrahigh-spatial-resolution chemical and magnetic imaging by laser-based photoemission electron microscopy

    SciTech Connect

    Taniuchi, Toshiyuki Kotani, Yoshinori; Shin, Shik

    2015-02-15

    We report the first experiments carried out on a new chemical and magnetic imaging system, which combines the high spatial resolution of a photoemission electron microscope (PEEM) with a continuous-wave deep-ultraviolet laser. Threshold photoemission is sensitive to the chemical and magnetic structures of the surface of materials. The spatial resolution of PEEM is limited by space charging when using pulsed photon sources as well as aberrations in the electron optics. We show that the use of a continuous-wave laser enabled us to overcome such a limit by suppressing the space-charge effect, allowing us to obtain a resolution of approximately 2.6 nm. With this system, we demonstrated the imaging of surface reconstruction domains on Si(001) by linear dichroism with normal incidence of the laser beam. We also succeeded in magnetic imaging of thin films with the use of magnetic circular dichroism near the Fermi level. The unique features of the ultraviolet laser will give us fast switching of the incident angles and polarizations of the photon source, which will be useful for the characterization of antiferromagnetic materials as well as ferromagnetic materials.

  16. Determination of transport levels of inorganic semiconductors by ultraviolet and inverse photoemission

    NASA Astrophysics Data System (ADS)

    Krause, S.; Schöll, A.; Umbach, E.

    2015-05-01

    A combination of ultraviolet and inverse photoemission is often used to determine the position of the transport levels of semiconductors. Although data from direct methods like photoemission appear advantageous at first glance, large discrepancies between thus-derived band gaps and optically measured band gaps have led to fundamentally different evaluation methods of the data from ultraviolet photoelectron spectroscopy (UPS)/inverse photoelectron spectroscopy (IPS) experiments, the essential alternatives being the maxima or the onsets of the frontier peaks. In this paper, we review published data as well as present new experimental data for a few representative II-VI and III-V compound and element semiconductors. New data from silicon are utilized as examples for evaluating details of such combined UPS and IPS spectra and for answering the question of how surface effects, especially the consequences of surface reconstruction, can adequately be taken into account. The results clearly indicate that, for all three types of semiconductors, only peak onsets represent the correct band positions. Possible reasons for this finding are discussed, and an explanation in the framework of relaxation (i.e., dynamical screening) is suggested.

  17. Watching Electrons Transfer from Metals to Insulators using Two Photon Photoemission

    SciTech Connect

    Johns, James E.

    2010-05-01

    Ultrafast angle-resolved two photon photoemission was used to study the dynamics and interfacial band structure of ultrathin films adsorbed onto Ag(111). Studies focused on the image potential state (IPS) in each system as a probe for measuring changes in electronic behavior in differing environments. The energetics and dynamics of the IPS at the toluene/Ag(111) interface are strongly dependent upon coverage. For a single monolayer, the first IPS is bound by 0.81 eV below the vacuum level and has a lifetime of 50 femtoseconds (fs). Further adsorption of toluene creates islands of toluene with an exposed wetting layer underneath. The IPS is then split into two peaks, one corresponding to the islands and one corresponding to the monolayer. The wetting layer IPS shows the same dynamics as the monolayer, while the lifetime of the islands increases exponentially with increasing thickness. Furthermore, the island IPS transitions from delocalized to localized within 500 fs, and electrons with larger parallel momenta decay much faster. Attempts were made using a stochastic model to extract the rates of localization and intraband cooling at differing momenta. In sexithiophene (6T) and dihexyl-sexithiophene (DH6T), the IPS was used as a probe to see if the nuclear motion of spectating side chains can interfere with molecular conduction. The energy and band mass of the IPS was measured for 6T and two geometries of DH6T on Ag(111). Electrons injected into the thicker coverages of DH6T grew exponentially heavier until they were completely localized by 230 fs, while those injected into 6T remained nearly free electron like. Based off of lifetime arguments and the density of defects, the most likely cause for the mass enhancement of the IPS in this system is small polaron formation caused by coupling of the electron to vibrations of the alkyl substituents. The energetic relaxation of the molecular adsorbate was also measured to be 20 meV/100 fs for the DH6T, and 0 meV/100 fs for

  18. Watching adsorption and electron beam induced decomposition on the model system Mo(CO)6/Cu(1 1 1) by X-ray absorption and photoemission spectroscopies

    NASA Astrophysics Data System (ADS)

    Paufert, Pierre; Fonda, Emiliano; Li, Zheshen; Domenichini, Bruno; Bourgeois, Sylvie

    2013-11-01

    An in-depth study of the first steps of electron beam assisted growth of Mo from molybdenum hexacarbonyl on Cu(1 1 1) has been carried out exploiting the complementarity of X-ray photoemission and X-ray absorption spectroscopies. Frank van der Merwe (2D) growth mode has been observed for the completion of the two first monolayers of adsorbed molecules through a simple physisorption process. Irradiation of the Mo(CO)6 deposit by 1 keV electron beam induces a modification of molybdenum coordination, the average number of C-neighbors decreasing from 6 to 3. Decomposed molecules remain on the surface after annealing at 520 K and organize themselves, the molybdenum atoms moving in Cu(1 1 1) surface fcc hollow sites. After annealing at 670 K, metallic molybdenum growth begins, if the total amount of adsorbed Mo atoms exceeds 1.2 monolayers.

  19. X-ray absorption and photoemission spectroscopy of zinc protoporphyrin adsorbed on rutile TiO{sub 2}(110) prepared by in situ electrospray deposition

    SciTech Connect

    Rienzo, Anna; Mayor, Louise C.; Magnano, Graziano; Satterley, Christopher J.; O'Shea, James N.; Ataman, Evren; Schnadt, Joachim; Schulte, Karina

    2010-02-28

    Zinc-protoporphyrin, adsorbed on the rutile TiO{sub 2}(110) surface, has been studied using photoemission spectroscopy and near-edge absorption fine structure spectroscopy to deduce the nature of the molecule-surface bonding and the chemical environment of the central metal atom. To overcome the difficulties associated with sublimation of the porphyrin molecules, samples were prepared in situ using ultrahigh vacuum electrospray deposition, a technique which facilitates the deposition of nonvolatile and fragile molecules. Monolayers of Zn protoporphyrin are found to bond to the surface via the oxygen atoms of the deprotonated carboxyl groups. The molecules initially lie largely parallel to the surface, reorienting to an upright geometry as the coverage is increased up to a monolayer. For those molecules directly chemisorbed to the surface, the interaction is sufficiently strong to pull the central metal atom out of the molecule.

  20. Emergent photovoltage on SmB6 surface upon bulk-gap evolution revealed by pump-and-probe photoemission spectroscopy

    PubMed Central

    Ishida, Y.; Otsu, T.; Shimada, T.; Okawa, M.; Kobayashi, Y.; Iga, F.; Takabatake, Y.; Shin, S.

    2015-01-01

    Recent studies suggest that an exemplary Kondo insulator SmB6 belongs to a new class of topological insulators (TIs), in which non-trivial spin-polarized metallic states emerge on surface upon the formation of Kondo hybridization gap in the bulk. Remarkably, the bulk resistivity reaches more than 20 Ω cm at 4 K, making SmB6 a candidate for a so-called bulk-insulating TI. We here investigate optical-pulse responses of SmB6 by pump-and-probe photoemission spectroscopy. Surface photovoltage effect is observed below ~90 K. This indicates that an optically-active band bending region develops beneath the novel metallic surface upon the bulk-gap evolution. The photovoltaic effect persists for >200 µs, which is long enough to be detected by electronics devices, and could be utilized for optical gating of the novel metallic surface. PMID:25640966

  1. Measurement of an exceptionally weak electron-phonon coupling on the surface of the topological insulator Bi2Se3 using angle-resolved photoemission spectroscopy.

    PubMed

    Pan, Z-H; Fedorov, A V; Gardner, D; Lee, Y S; Chu, S; Valla, T

    2012-05-01

    Gapless surface states on topological insulators are protected from elastic scattering on nonmagnetic impurities which makes them promising candidates for low-power electronic applications. However, for widespread applications, these states should have to remain coherent at ambient temperatures. Here, we studied temperature dependence of the electronic structure and the scattering rates on the surface of a model topological insulator, Bi2Se3, by high-resolution angle-resolved photoemission spectroscopy. We found an extremely weak broadening of the topological surface state with temperature and no anomalies in the state's dispersion, indicating exceptionally weak electron-phonon coupling. Our results demonstrate that the topological surface state is protected not only from elastic scattering on impurities, but also from scattering on low-energy phonons, suggesting that topological insulators could serve as a basis for room-temperature electronic devices.

  2. Modeling angle-resolved photoemission of graphene and black phosphorus nano structures

    PubMed Central

    Park, Sang Han; Kwon, Soonnam

    2016-01-01

    Angle-resolved photoemission spectroscopy (ARPES) data on electronic structure are difficult to interpret, because various factors such as atomic structure and experimental setup influence the quantum mechanical effects during the measurement. Therefore, we simulated ARPES of nano-sized molecules to corroborate the interpretation of experimental results. Applying the independent atomic-center approximation, we used density functional theory calculations and custom-made simulation code to compute photoelectron intensity in given experimental setups for every atomic orbital in poly-aromatic hydrocarbons of various size, and in a molecule of black phosphorus. The simulation results were validated by comparing them to experimental ARPES for highly-oriented pyrolytic graphite. This database provides the calculation method and every file used during the work flow. PMID:27164313

  3. Design of a high-bunch-charge 112-MHz superconducting RF photoemission electron source

    NASA Astrophysics Data System (ADS)

    Xin, T.; Brutus, J. C.; Belomestnykh, Sergey A.; Ben-Zvi, I.; Boulware, C. H.; Grimm, T. L.; Hayes, T.; Litvinenko, Vladimir N.; Mernick, K.; Narayan, G.; Orfin, P.; Pinayev, I.; Rao, T.; Severino, F.; Skaritka, J.; Smith, K.; Than, R.; Tuozzolo, J.; Wang, E.; Xiao, B.; Xie, H.; Zaltsman, A.

    2016-09-01

    High-bunch-charge photoemission electron-sources operating in a continuous wave (CW) mode are required for many advanced applications of particle accelerators, such as electron coolers for hadron beams, electron-ion colliders, and free-electron lasers. Superconducting RF (SRF) has several advantages over other electron-gun technologies in CW mode as it offers higher acceleration rate and potentially can generate higher bunch charges and average beam currents. A 112 MHz SRF electron photoinjector (gun) was developed at Brookhaven National Laboratory to produce high-brightness and high-bunch-charge bunches for the coherent electron cooling proof-of-principle experiment. The gun utilizes a quarter-wave resonator geometry for assuring beam dynamics and uses high quantum efficiency multi-alkali photocathodes for generating electrons.

  4. Electron-vibration coupling induced renormalization in the photoemission spectrum of diamondoids

    NASA Astrophysics Data System (ADS)

    Gali, Adam; Demján, Tamás; Vörös, Márton; Thiering, Gergő; Cannuccia, Elena; Marini, Andrea

    2016-04-01

    The development of theories and methods devoted to the accurate calculation of the electronic quasi-particle states and levels of molecules, clusters and solids is of prime importance to interpret the experimental data. These quantum systems are often modelled by using the Born-Oppenheimer approximation where the coupling between the electrons and vibrational modes is not fully taken into account, and the electrons are treated as pure quasi-particles. Here, we show that in small diamond cages, called diamondoids, the electron-vibration coupling leads to the breakdown of the electron quasi-particle picture. More importantly, we demonstrate that the strong electron-vibration coupling is essential to properly describe the overall lineshape of the experimental photoemission spectrum. This cannot be obtained by methods within Born-Oppenheimer approximation. Moreover, we deduce a link between the vibronic states found by our many-body perturbation theory approach and the well-known Jahn-Teller effect.

  5. Photoemission from cesium-oxide-activated InGaAsP.

    NASA Technical Reports Server (NTRS)

    James, L. W.; Antypas, G. A.; Moon, R. L.; Edgecumbe, J.; Bell, R. L.

    1973-01-01

    Zinc-doped InGaAsP quaternary III-V material of the proper composition range shows superior photoemission properties to either InGaAs or InAsP ternary material. The minority-carrier diffusion length in the quaternary material is at least as long as that in InAsP and much longer than observed in InGaAs. The barrier height at the InGaAsP-Cs2O interface is lowered by cooling, giving increased electron escape probability and new highs in quantum efficiency over a wide wavelength range. For example, a 1.06-micron quantum efficiency of 7.5%/incident photon was observed at -90 C.

  6. Time-resolved photoemission of correlated electrons driven out of equilibrium

    SciTech Connect

    Moritz, B.; Devereaux, T. P.; Freericks, J. K.

    2010-04-15

    We describe the temporal evolution of the time-resolved photoemission response of the spinless Falicov-Kimball model driven out of equilibrium by strong applied fields. The model is one of the few possessing a metal-insulator transition and admitting an exact solution in the time domain. The nonequilibrium dynamics, evaluated using an extension of dynamical mean-field theory, show how the driven system differs from two common viewpoints--a quasiequilibrium system at an elevated effective temperature (the 'hot' electron model) or a rapid interaction quench ('melting' of the Mott gap) - due to the rearrangement of electronic states and redistribution of spectral weight. The results demonstrate the inherent trade-off between energy and time resolution accompanying the finite width probe pulses, characteristic of those employed in pump-probe time-domain experiments, which can be used to focus attention on different aspects of the dynamics near the transition.

  7. Tunable vacuum ultraviolet laser based spectrometer for angle resolved photoemission spectroscopy

    SciTech Connect

    Jiang, Rui; Mou, Daixiang; Wu, Yun; Huang, Lunan; Kaminski, Adam; McMillen, Colin D.; Kolis, Joseph; Giesber, Henry G.; Egan, John J.

    2014-03-15

    We have developed an angle-resolved photoemission spectrometer with tunable vacuum ultraviolet laser as a photon source. The photon source is based on the fourth harmonic generation of a near IR beam from a Ti:sapphire laser pumped by a CW green laser and tunable between 5.3 eV and 7 eV. The most important part of the set-up is a compact, vacuum enclosed fourth harmonic generator based on potassium beryllium fluoroborate crystals, grown hydrothermally in the US. This source can deliver a photon flux of over 10{sup 14} photon/s. We demonstrate that this energy range is sufficient to measure the k{sub z} dispersion in an iron arsenic high temperature superconductor, which was previously only possible at synchrotron facilities.

  8. Substrate interactions with suspended and supported monolayer MoS2: Angle-resolved photoemission spectroscopy

    DOE PAGES

    Jin, Wencan; Yeh, Po -Chun; Zaki, Nader; Zhang, Datong; Liou, Jonathan T.; Dadap, Jerry I.; Barinov, Alexey; Yablonskikh, Mikhail; Sadowski, Jerzy T.; Sutter, Peter; et al

    2015-03-17

    We report the directly measured electronic structure of exfoliated monolayer molybdenum disulfide (MoS₂) using micrometer-scale angle-resolved photoemission spectroscopy. Measurements of both suspended and supported monolayer MoS₂ elucidate the effects of interaction with a substrate. Thus, a suggested relaxation of the in-plane lattice constant is found for both suspended and supported monolayer MoS₂ crystals. For suspended MoS₂, a careful investigation of the measured uppermost valence band gives an effective mass at Γ¯ and Κ¯ of 2.00m₀ and 0.43m₀, respectively. We also measure an increase in the band linewidth from the midpoint of Γ¯Κ¯ to the vicinity of Κ¯ and briefly discussmore » its possible origin.« less

  9. Rashba splitting in an image potential state investigated by circular dichroism two-photon photoemission spectroscopy

    NASA Astrophysics Data System (ADS)

    Nakazawa, T.; Takagi, N.; Kawai, Maki; Ishida, H.; Arafune, R.

    2016-09-01

    We have explored the band splitting and spin texture of the image potential state (IPS) on Au(001) derived from the Rashba-type spin-orbit interaction (SOI) by using angle-resolved bichromatic two-photon photoemission (2PPE) spectroscopy in combination with circular dichroism (CD). The Rashba parameter for the first (n =1 ) IPS is determined to be 48-20+8meV Å , which is consistent with the spin-polarized band structure calculated from the embedded Green's function technique for semi-infinite crystals. The present results demonstrate that bichromatic CD-2PPE spectroscopy is powerful for mapping the spin-polarized unoccupied band structures originating from SOIs in various classes of condensed matter.

  10. Nesting-driven multipolar order in CeB6 from photoemission tomography.

    PubMed

    Koitzsch, A; Heming, N; Knupfer, M; Büchner, B; Portnichenko, P Y; Dukhnenko, A V; Shitsevalova, N Y; Filipov, V B; Lev, L L; Strocov, V N; Ollivier, J; Inosov, D S

    2016-01-01

    Some heavy fermion materials show so-called hidden-order phases which are invisible to many characterization techniques and whose microscopic origin remained controversial for decades. Among such hidden-order compounds, CeB6 is of model character due to its simple electronic configuration and crystal structure. Apart from more conventional antiferromagnetism, it shows an elusive phase at low temperatures, which is commonly associated with multipolar order. Here we show that this phase roots in a Fermi surface instability. This conclusion is based on a full 3D tomographic sampling of the electronic structure by angle-resolved photoemission and comparison with inelastic neutron scattering data. The hidden order is mediated by itinerant electrons. Our measurements will serve as a paradigm for the investigation of hidden-order phases in f-electron systems, but also generally for situations where the itinerant electrons drive orbital or spin order. PMID:26976632

  11. Preparation of layered thin film samples for angle-resolved photoemission spectroscopy

    SciTech Connect

    Harrison, S. E.; Zhou, B.; Huo, Y.; Harris, J. S.; Pushp, A.; Kellock, A. J.; Parkin, S. S. P.; Chen, Y.; Hesjedal, T.

    2014-09-22

    Materials with layered van der Waals crystal structures are exciting research topics in condensed matter physics and materials science due to outstanding physical properties associated with their strong two dimensional nature. Prominent examples include bismuth tritelluride and triselenide topological insulators (TIs), which are characterized by a bulk bandgap and pairwise counter-propagating spin-polarized electronic surface states. Angle-resolved photoemission spectroscopy (ARPES) of ex-situ grown thin film samples has been limited by the lack of suitable surface preparation techniques. We demonstrate the shortcomings of previously successful conventional surface preparation techniques when applied to ternary TI systems which are susceptible to severe oxidation. We show that in-situ cleaving is a simple and effective technique for preparation of clean surfaces on ex-situ grown thin films for high quality ARPES measurements. The method presented here is universally applicable to other layered van der Waals systems as well.

  12. Electronic structure of MgB2 from angle-resolved photoemission spectroscopy.

    PubMed

    Uchiyama, H; Shen, K M; Lee, S; Damascelli, A; Lu, D H; Feng, D L; Shen, Z-X; Tajima, S

    2002-04-15

    The first angle-resolved photoemission spectroscopy results from MgB2 single crystals are reported. Along the GammaK and GammaM directions, we observed three distinct dispersive features approaching the Fermi energy. These can be assigned to the theoretically predicted sigma (B 2p(x,y)) and pi (B 2p(z)) bands. In addition, a small parabolic-like band is detected around the Gamma point, which can be attributed to a surface-derived state. The overall agreement between our results and the band calculations suggests that the electronic structure of MgB2 is of a conventional nature, thus implying that electron correlations are weak and may be of little importance to superconductivity in this system.

  13. Theory of Floquet band formation and local pseudospin textures in pump-probe photoemission of graphene.

    PubMed

    Sentef, M A; Claassen, M; Kemper, A F; Moritz, B; Oka, T; Freericks, J K; Devereaux, T P

    2015-01-01

    Ultrafast materials science promises optical control of physical properties of solids. Continuous-wave circularly polarized laser driving was predicted to induce a light-matter coupled state with an energy gap and a quantum Hall effect, coined Floquet topological insulator. Whereas the envisioned Floquet topological insulator requires high-frequency pumping to obtain well-separated Floquet bands, a follow-up question regards the creation of Floquet-like states in graphene with realistic low-frequency laser pulses. Here we predict that short optical pulses attainable in experiments can lead to local spectral gaps and novel pseudospin textures in graphene. Pump-probe photoemission spectroscopy can track these states by measuring sizeable energy gaps and Floquet band formation on femtosecond time scales. Analysing band crossings and pseudospin textures near the Dirac points, we identify new states with optically induced nontrivial changes of sublattice mixing that leads to Berry curvature corrections of electrical transport and magnetization.

  14. Modeling angle-resolved photoemission of graphene and black phosphorus nano structures.

    PubMed

    Park, Sang Han; Kwon, Soonnam

    2016-01-01

    Angle-resolved photoemission spectroscopy (ARPES) data on electronic structure are difficult to interpret, because various factors such as atomic structure and experimental setup influence the quantum mechanical effects during the measurement. Therefore, we simulated ARPES of nano-sized molecules to corroborate the interpretation of experimental results. Applying the independent atomic-center approximation, we used density functional theory calculations and custom-made simulation code to compute photoelectron intensity in given experimental setups for every atomic orbital in poly-aromatic hydrocarbons of various size, and in a molecule of black phosphorus. The simulation results were validated by comparing them to experimental ARPES for highly-oriented pyrolytic graphite. This database provides the calculation method and every file used during the work flow. PMID:27164313

  15. Nesting-driven multipolar order in CeB6 from photoemission tomography

    PubMed Central

    Koitzsch, A.; Heming, N.; Knupfer, M.; Büchner, B.; Portnichenko, P. Y.; Dukhnenko, A. V; Shitsevalova, N. Y.; Filipov, V. B.; Lev, L. L.; Strocov, V. N.; Ollivier, J.; Inosov, D. S.

    2016-01-01

    Some heavy fermion materials show so-called hidden-order phases which are invisible to many characterization techniques and whose microscopic origin remained controversial for decades. Among such hidden-order compounds, CeB6 is of model character due to its simple electronic configuration and crystal structure. Apart from more conventional antiferromagnetism, it shows an elusive phase at low temperatures, which is commonly associated with multipolar order. Here we show that this phase roots in a Fermi surface instability. This conclusion is based on a full 3D tomographic sampling of the electronic structure by angle-resolved photoemission and comparison with inelastic neutron scattering data. The hidden order is mediated by itinerant electrons. Our measurements will serve as a paradigm for the investigation of hidden-order phases in f-electron systems, but also generally for situations where the itinerant electrons drive orbital or spin order. PMID:26976632

  16. Electron–vibration coupling induced renormalization in the photoemission spectrum of diamondoids

    PubMed Central

    Gali, Adam; Demján, Tamás; Vörös, Márton; Thiering, Gergő; Cannuccia, Elena; Marini, Andrea

    2016-01-01

    The development of theories and methods devoted to the accurate calculation of the electronic quasi-particle states and levels of molecules, clusters and solids is of prime importance to interpret the experimental data. These quantum systems are often modelled by using the Born–Oppenheimer approximation where the coupling between the electrons and vibrational modes is not fully taken into account, and the electrons are treated as pure quasi-particles. Here, we show that in small diamond cages, called diamondoids, the electron–vibration coupling leads to the breakdown of the electron quasi-particle picture. More importantly, we demonstrate that the strong electron–vibration coupling is essential to properly describe the overall lineshape of the experimental photoemission spectrum. This cannot be obtained by methods within Born–Oppenheimer approximation. Moreover, we deduce a link between the vibronic states found by our many-body perturbation theory approach and the well-known Jahn–Teller effect. PMID:27103340

  17. High resolution scanning near field mapping of enhancement on SERS substrates: comparison with photoemission electron microscopy.

    PubMed

    Awada, C; Plathier, J; Dab, C; Charra, F; Douillard, L; Ruediger, A

    2016-04-14

    The need for a dedicated spectroscopic technique with nanoscale resolution to characterize SERS substrates pushed us to develop a proof of concept of a functionalized tip-surface enhanced Raman scattering (FTERS) technique. We have been able to map hot spots on semi-continuous gold films; in order to validate our approach we compare our results with photoemission electron microscopy (PEEM) data, the complementary electron microscopy tool to map hot spots on random metallic surfaces. Enhanced Raman intensity maps at high spatial resolution reveal the localisation of hotspots at gaps for many neighboring nanostructures. Finally, we compare our findings with theoretical simulations of the enhancement factor distribution, which confirms a dimer effect as the dominant origin of hot spots. PMID:26979589

  18. Evidencing the need for high spatial resolution in angle-resolved photoemission experiments

    NASA Astrophysics Data System (ADS)

    Joucken, Frédéric; Reckinger, Nicolas; Lorcy, Stéphane; Avila, José; Chen, Chaoyu; Lagoute, Jérôme; Colomer, Jean-François; Ghijsen, Jacques; Asensio, Maria Carmen; Sporken, Robert

    2016-06-01

    Angle-resolved photoemission spectroscopy (ARPES) is the most direct tool to measure the electronic structure of materials. In particular, fine features of the spectra can be analyzed for evaluating the electron self-energy. Owing to a setup allowing ARPES investigation with submicron resolution and state-of-the-art energy and momentum resolution, we show here first that ARPES spectra of pristine and virtually undoped monolayer graphene acquired on a small spot do not display manifestations of self-energy. We next demonstrate that, although the region of the sample investigated is a unique graphene domain, it displays faint spatial inhomogeneity, both in its crystallographic orientation and its thickness, which is undetectable with conventional ARPES but renders the spectra improper for self-energy extraction. These results indicate that care should be taken when analyzing ARPES spectra obtained with poor spatial resolution.

  19. Modeling angle-resolved photoemission of graphene and black phosphorus nano structures.

    PubMed

    Park, Sang Han; Kwon, Soonnam

    2016-05-10

    Angle-resolved photoemission spectroscopy (ARPES) data on electronic structure are difficult to interpret, because various factors such as atomic structure and experimental setup influence the quantum mechanical effects during the measurement. Therefore, we simulated ARPES of nano-sized molecules to corroborate the interpretation of experimental results. Applying the independent atomic-center approximation, we used density functional theory calculations and custom-made simulation code to compute photoelectron intensity in given experimental setups for every atomic orbital in poly-aromatic hydrocarbons of various size, and in a molecule of black phosphorus. The simulation results were validated by comparing them to experimental ARPES for highly-oriented pyrolytic graphite. This database provides the calculation method and every file used during the work flow.

  20. Emergence of anisotropic heavy fermions in antiferromagnetic Kondo lattice CeIn3 revealed by photoemission

    NASA Astrophysics Data System (ADS)

    Zhang, Yun; Lu, Haiyan; Zhu, Xiegang; Tan, Shiyong; Chen, Qiuyun; Feng, Wei; Xie, Donghua; Luo, Lizhu; Zhang, Wen; Lai, Xinchun; Donglai Feng Team; Huiqiu Yuan Team

    One basic concept in heavy fermions systems is the entanglement of localized spin state and itinerant electron state. It can be tuned by two competitive intrinsic mechanisms, Kondo effect and Ruderman-Kittel-Kasuya-Yosida interaction, with external disturbances. The key issue regarding heavy fermions properties is how the two mechanisms work in the same phase region. To investigate the relation of the two mechanisms, the cubic antiferromagnetic heavy fermions compound CeIn3 was investigated by soft x-ray angle resolved photoemission spectroscopy. The hybridization between f electrons and conduction bands in the paramagnetic state was observed directly, providing compelling evidence for Kondo screening scenario and coexistence of two mechanisms. The hybridization strength shows slight and regular anisotropy in K space, implying that the two mechanisms are competitive and anisotropic. This work illuminates the concomitant and competitive relation between the two mechanisms and supplies some evidences for the anisotropic superconductivity of CeIn3