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

Description: 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 Tl{sub 2}Ba{sub 2}CuO{sub 6+{delta}} (Tl2201) T{sub c,max} {approx} 95 K and (Bi{sub 1.35}Pb{sub 0.85})(Sr{sub 1.47}La{sub 0.38})CuO{sub 6+{delta}} (Bi2201) T{sub c,max} {approx} 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 ({pi},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 T{sub c} Tl2201. The second study looks at the different ways of doping Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8+{delta}} (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 CO{sub 2}/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 with a charge density wave (CDW) origin of the ...
Date: December 15, 2010
Creator: Palczewski, Ari Deibert
Partner: UNT Libraries Government Documents Department

Two-photon Photoemission of Organic Semiconductor Molecules on Ag(111)

Description: 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.
Date: May 15, 2008
Creator: Yang, Aram & Yang, Aram
Partner: UNT Libraries Government Documents Department

A New Spin on Photoemission Spectroscopy

Description: 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.
Date: December 1, 2008
Creator: Jozwiak, Chris
Partner: UNT Libraries Government Documents Department

Watching Electrons Transfer from Metals to Insulators using Two Photon Photoemission

Description: 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 ...
Date: May 1, 2010
Creator: Johns, James E.
Partner: UNT Libraries Government Documents Department

High Pressure Scanning Tunneling Microscopy and High PressureX-ray Photoemission Spectroscopy Studies of Adsorbate Structure,Composition and Mobility during Catalytic Reactions on A Model SingleCrystal

Description: Our research focuses on taking advantage of the ability of scanning tunneling microscopy (STM) to operate at high-temperatures and high-pressures while still providing real-time atomic resolution images. We also utilize high-pressure x-ray photoelectron spectroscopy (HPXPS) to monitor systems under identical conditions thus giving us chemical information to compare and contrast with the structural and dynamic data provided by STM.
Date: May 12, 2006
Creator: Montano, M. O.
Partner: UNT Libraries Government Documents Department

Fourier transform photoelectron diffraction and its application to molecular orbitals and surface structure

Description: Photoemission intensities from the molecular orbitals of c(2x2)CO/Pt(111) over a wide photon energy range were measured and analyzed by the same methods developed for structural studies using core levels. The 4{sigma} orbital center of gravity is found to be concentrated between the C and O atoms, while that of the 5{sigma} orbital lies between the C atom and the Pt surface. The C 1s photoelectron diffraction was used to determine the adsorption geometry. The earlier ambiguity that multiple scattering is needed to correctly model a {chi} curve while single scattering is sufficient for understanding major peaks in the ARPEFS-FTS is clarified by studying the clean Ni(111) surface. In the normal emission case, several different combinations of scattering events have similar path length differences (PLDs), and can either cancel each other or enhance the corresponding FT peak. In the off-normal case the degeneracy is greatly reduced due to the lower degree of symmetry. In normal emission AR PEFS, up to third order multiple scattering is needed to describe fully both the {chi} curve and its FT spectrum. To improve the spectral resolution in the ARPEFS-FT analysis, several new spectral analysis methods are introduced. With both autocorrelation autoregression (ACAR) and autocorrelation eigenvector (ACE), we can produce a reliable power spectrum by following the order-closing procedure. The best spectra are usually obtained when the autocorrelation sequence is computed with lags up to half the data range. A simple way of determining surface adsorption sites is proposed as follows: First use a single scattering cluster for possible adsorption sites to construct the geometrical PLDs from the strong backscattering events; then compare these PLDs with those obtained from the ARPEFS-FT analysis of the experimental data. After the preferred adsorption site is determined, fine tune the interlayer distances according to the positional R-factor.
Date: November 30, 1998
Creator: Zhou, Xin
Partner: UNT Libraries Government Documents Department

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

Description: 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.
Date: May 1, 1997
Creator: Menchero, J.G.
Partner: UNT Libraries Government Documents Department

Multi-atom resonant photoemission and the development of next-generation software and high-speed detectors for electron spectroscopy

Description: 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 matched to ...
Date: September 1, 2000
Creator: Kay, Alexander William
Partner: UNT Libraries Government Documents Department

Photoelectron holography applied to surface structural determination

Description: Photoemitted electron waves are used as coherent source waves for angstrom-scale holographic imaging of local atomic geometry at surfaces. Electron angular distribution patterns are collected above a sample surface and serve as a record of the interference between source wave and waves scattered from surrounding ion cores. Using a mathematical imaging integral transformation, the three-dimensional structural information is obtained directly from these collected patterns. Patterns measured with different electron kinetic energies are phase-summed for image improvement. Pt (111) surface is used as a model system. A pattern 9.6{angstrom}{sup {minus}1} (351 eV) is used to generate a full 3-D image of atom locations around an emitter with nearest neighbors within 0.l{angstrom} of the expected bulk positions. Atoms several layers beyond the nearest neighbors are also apparent. Twin-image reduction and artifact suppression is obtained by phase-summing eight patterns measured from 8.8 to 10.2{angstrom}{sup {minus}1} (295 to 396 eV). 32 were measured in 0.2{angstrom}{sup {minus}1} steps from 6.0 to 12.2{angstrom}{sup {minus}1} (137 to 567 eV) are presented here. Simple models of two-slit interference are compared with electron scattering to illuminate understanding of holographic recording of the structural information. This also shows why it sometimes fails due to destructive interferences. Simple theoretical models of electron scattering are compared to experiment to show the origin of the structural information and the differences that result from atomic scattering and from the source wave. Experimental parameters and their relation to imaging is discussed. Comparison is made to the Pt pattern measured at 351 eV using the simple theoretical model. The remaining data set is also modeled, and the eight appropriate theoretical patterns are used to regenerate the multiple-wavenumber experimental result. A clean Cu (001) surface is also measured and imaged.
Date: May 1, 1995
Creator: Petersen, B.L.
Partner: UNT Libraries Government Documents Department

Structural and Photoelectron Emission Properties of Chemical Vapor Deposition Grown Diamond Films

Description: The effects of methane (CH4), diborone (B2H6) and nitrogen (N2) concentrations on the structure and photoelectron emission properties of chemical vapor deposition (CVD) polycrystalline diamond films were studied. The diamond films were grown on single-crystal Si substrates using the hot-tungsten filament CVD technique. Raman spectroscopy and x-ray photoelectron spectroscopy (XPS) were used to characterize the different forms of carbon in the films, and the fraction of sp3 carbon to sp3 plus sp2 carbon at the surface of the films, respectively. Scanning electron microscopy (SEM) was used to characterize the surface morphology of the films. The photoelectron emission properties were determined by measuring the energy distributions of photoemitted electrons using ultraviolet photoelectron spectroscopy (UPS), and by measuring the photoelectric current as a function of incident photon energy.
Date: August 1998
Creator: Akwani, Ikerionwu Asiegbu
Partner: UNT Libraries

The Electron Emission Characteristics of Aluminum, Molybdenum and Carbon Nanotubes Studied by Field Emission and Photoemission.

Description: The electron emission characteristics of aluminum, molybdenum and carbon nanotubes were studied. The experiments were setup to study the emission behavior as a function of temperature and exposure to oxygen. Changes in the surface work function as a result of thermal annealing were monitored with low energy ultra-violet photoelectron spectroscopy for flat samples while field emission energy distributions were used on tip samples. The change in the field emission from fabricated single tips exposed to oxygen while in operation was measured using simultaneous Fowler-Nordheim plots and electron energy distributions. From the results a mechanism for the degradation in the emission was concluded. Thermal experiments on molybdenum and aluminum showed that these two materials can be reduced at elevated temperatures, while carbon nanotubes on the other hand show effects of oxidation. To purely reduce molybdenum a temperature in excess of 750 ºC is required. This temperature exceeds that allowed by current display device technology. Aluminum on the other hand shows reduction at a much lower temperature of at least 125 ºC; however, its extreme reactivity towards oxygen containing species produces re-oxidation. It is believed that this reduction is due to the outward diffusion of aluminum atoms through the oxide. Carbon nanotubes on the other hand show signs of oxidation as they are heated above 700 ºC. In this case the elevated temperatures cause the opening of the end caps allowing the uptake of water. Oxygen exposure experiments indicate that degradation in field emission is two-fold and is ultimately dependent on the emission current at which the tip is operated. At low emission currents the degradation is exclusively due to oxidation. At high emission currents ion bombardment results in the degradation of the emitter. In between the two extremes, molybdenum tips are capable of stable emission.
Date: December 2002
Creator: Sosa, Edward Delarosa
Partner: UNT Libraries

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

Description: 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.
Date: December 19, 2004
Creator: Park, Jongik
Partner: UNT Libraries Government Documents Department

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

Description: 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.
Date: October 1, 1992
Creator: Huang, Z.
Partner: UNT Libraries Government Documents Department