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Structure and Dynamics of Core-Excited SpeciesTravnikova, Oksana January 2008 (has links)
In this thesis we have performed core-electron spectroscopy studies of gas phase molecular systems starting with smaller diatomic, continuing with triatomic and extending our research to more complex polyatomic ones. We can subdivide the results presented here into two categories: the first one focusing on electronic fine structure and effect of the chemical bonds on molecular core-levels and the other one dealing with nuclear dynamics induced by creation of a core hole. In our research we have mostly used synchrotron radiation based techniques such as X-ray Photoelectron (XPS), X-ray Absorption (XAS), normal and Resonant Auger (AES and RAS, respectively) and Energy-Selected Auger Electron PhotoIon COincidence (ES-AEPICO) spectroscopies. We have demonstrated that resonant Auger spectroscopy can be used to aid interpretation of the features observed in XAS for Rydberg structures in the case of Cl2 and C1s−1π*1 states of allene molecules. The combined use of high-resolution spectroscopy with ab initio calculations can help the interpretation of strongly overlapped spectral features and disentangle their complex profiles. This approach enabled us to determine the differences in the lifetimes for core-hole 2p sublevels of Cl2 which are caused by the presence of the chemical bond. We have shown that contribution in terms of the Mulliken population of valence molecular orbitals is a determining factor for resonant enhancement of different final states and fragmentation patterns reached after resonant Auger decays in N2O. We have also performed a systematic study of the dependence of the C1s resonant Auger kinetic energies on the presence of different substituents in CH3X compounds. For the first time we have studied possible isomerization reaction induced by core excitation of acetylacetone. We could observe a new spectral feature in the resonant Auger decay spectra which we interpreted as a signature of core-excitation-induced keto-enol tautomerism.
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Theoretical Investigations Of Core-Level Spectroscopies In Strongly Correlated SystemsGupta, Subhra Sen 12 1900 (has links)
Ever since the discovery of exotic phenomena like high temperature (Tc) superconductivity
in the cuprates and colossal magnetoresistance in the manganites, strongly correlated electron systems have become the center of attention in the field of condensed matter physics research. This renewed interest has been further kindled by the rapid development of sophisticated experimental techniques and tremendous computational power. Computation plays
a pivotal role in the theoretical investigation of these systems, because one cannot explain their complicated phase diagrams by simple, exactly solvable models. Among the plethora of experimental techniques, various kinds of high energy electron spectroscopies are fast gaining importance due to the multitude of physical properties and phenomena which they
can access. However the physical processes involved and the interpretation of the spectra obtained from these spectroscopies are extremely complex and require extensive theoretical modelling. This thesis is concerned with the theoretical modelling of a certain class of high energy electron spectroscopies, viz. the core-level electron spectroscopies, for strongly correlated systems of various kinds. The spectroscopies covered are Auger electron spectroscopy
(AES), core-level photoemission spectroscopy (core-level PES) and X-ray absorption spec-
troscopy (XAS), which provide non-magnetic information, and also X-ray magnetic circular
and linear dichroism (XMCD and XMLD), which provide magnetic information.
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Elektronenspektroskopie und Faktoranalyse zur Untersuchung von ionenbeschossenen Metall (Re, Ir, Cr, Fe)-Silizium-SchichtenReiche, Rainer 29 January 2000 (has links) (PDF)
No description available.
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Solvent–Solute Interaction : Studied by Synchrotron Radiation Based Photo and Auger Electron SpectroscopiesPokapanich, Wandared January 2011 (has links)
Aqueous solutions were studied using photoelectron and Auger spectroscopy, based on synchrotron radiation and a liquid micro-jet setup. By varying the photon energy in photoelectron spectra, we depth profiled an aqueous tetrabutylammonium iodide (TBAI) solution. Assuming uniform angular emission from the core levels, we found that the TBA+ ions were oriented at the surface with the hydrophobic butyl arms sticking into the liquid. We investigated the association between ions and their neighbors in aqueous solutions by studying the electronic decay after core ionization. The (2p)−1 decay of solvated K+ and Ca2+ ions was studied. The main features in the investigated decay spectra corresponded to two-hole final states localized on the ions. The spectra also showed additional features, related to delocalized two-hole final states with vacancies on a cation and a neighboring water molecule. These two processes compete, and by comparing relative intensities and using the known rate for the localized decay, we determined the time-scale for the delocalized process for the two ions. We compared to delocalized electronic decay processes in Na+, Mg2+, and Al3+, and found that they were slower in K+ and Ca2+, due to different internal decay mechanisms of the ions, as well as external differences in the ion-solute distances and interactions. In the O 1s Auger spectra of aqueous metal halide solutions, we observed features related to delocalized two-hole final states with vacancies on a water molecule and a neighboring solvated anion. The relative intensity of these feature indicated that the strength of the interaction between the halide ions and water correlated with ionic size. The delocalized decay was also used to investigate contact ion pair formation in high concentrated potassium halide solutions, but no concrete evidence of contact ion pairs was observed. / Felaktigt tryckt som Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 726
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Development of a Spin-Polarized Low Energy Electron Diffraction System and Investigation on Spin-Orbit and Exchange Interactions on Ir(100) and Ultrathin Fe(100) Grown on Ir(100)Pradeep, A V January 2016 (has links) (PDF)
Spin-polarized electron beam has not yet been produced from an unpolarized electron beam using Stern-Gerlach type spin filter, because of the Lorentz force and Heisenberg uncertainty principle. At present, electron spin detectors and filters work on the basis of spin-dependent scattering of an electron beam from crystal surfaces. Single channel efficiencies of all the spin detectors for electrons are orders of magnitudes lower than the ideal one. Specular reflection type spin-polarized low energy electron diffraction (SPLEED)-spin detectors are having higher single channel efficiencies compared to the conventional Mott detectors. Moreover, multichannel detection can be realized from specular reflection type SPLEED-spin detectors. They have higher effective efficiency than the ideal spin detector. In order to develop specular reflection type spin filter, it is important to develop a spin-polarized low energy electron diffraction system. In addition, SPLEED system allows us to study the spin-orbit and exchange scattering at crystal surfaces.
The general direction of the thesis has been the development of spin-polarized low energy electron diffraction (SPLEED) system. This system has been used to investigate the spin-orbit interactions on Ir(100) surface and exchange interactions of Fe grown on Ir(100). The thesis is organized into chapters as follows.
Chapter 1 introduce the reader to some of the basic concepts of polarized electrons and the evolution of spin-polarized electron sources and detectors. Sources of polarized electrons are discussed with emphasis on photocathodes such as GaAs and strained GaAs. Widely used spin detector is the Mott detector which works in the higher energy range. The working principle of the Mott detector is discussed. Commonly used spin detector in the lower energy range is the LEED detector. The concept of the LEED detector is also discussed. Working principle and recent developments of specular reflection type SPLEED spin filters are introduced. Evolution of electron spin detector is discussed towards the end of the chapter.
Chapter 2 discusses about the two instruments designed and developed during the course of the thesis. The first one is a spin-polarized low energy electron diffraction system working in the reflected electron pulse counting mode in UHV. This system is capable of measuring spin asymmetries due to spin-orbit interaction and exchange interaction. This instrument is useful in understanding structure and magnetism at surfaces as well as helps to develop new spin polarimeter based on SPLEED by evaluating spin asymmetries from different surfaces. All instruments connected to SPLEED system, measurement protocol and controlling software are discussed with some details. Along with this, standard characterization tools such as X-ray diffraction and magneto-optic Kerr effect measurements are discussed. The second instrument is a novel quadratic magneto-optic Kerr effect measurement system using permanent magnets, which is simple, compact and cost-effective. We have used rotating field method to extract QMOKE component in saturation. So there is no need for precise real-time measurement of magnitude and direction of the magnetic field as in the case of vector magnet. This instrument can easily quantify QMOKE coefficients for ferrimagnetic and ferromagnetic thin films and single crystals.
Chapter 3 discusses SPLEED experiments carried out on Ir(100)-(1×5)-Hex and Ir(100)-(1×2+2×1)-O surfaces. The surface structure and surface preparation techniques are discussed. The stability of the Ir(100)-(1×5)-Hex surface is evaluated by monitoring the spin asymmetry as the function of time. Within 25 hours after the surface preparation, the profile of the spin asymmetry and the reflected electron count for Ir(100)-(1×5)-Hex surface resembles that of hydrogen adsorbed Ir(100)-(1×5)-H surface. The electron energy-angle of incidence landscape of reflectivity, spin asymmetry and figure of merit are recorded for Ir(100)-(1×2+2×1)-O surface. Many wide regions with a large figure of merit are identified in the E- landscape.
Chapter 4 reports SPLEED experiments carried out on Ir(100)-(1×5)-H surface. The comparison between asymmetries evaluated for the Ir(100)-(1×5)-Hex surface after 25 hours and Ir(100)-(1×5)-H surface suggests that Ir(100)-(1×5)-Hex surface is transforming to Ir(100)-(1×5)-H surface, in 25 hours. This can be due to the adsorption of more than four Langmuir of residual hydrogen during this time. The energy-angle landscape of reflectivity, asymmetry and figure of merit are recorded for Ir(100)-(1×5)-H surface in an energy range 20 eV to 100 eV and angle range 10 to 60 . Many regions are identified as the working point for specular reflection type spin filter based on SPLEED. The surface structure and surface preparation techniques are discussed. The stability of the surface is also evaluated.
Chapter 5 investigates the growth and magnetic properties of Fe(100) film on Ir(100)-(1×1), Ir(100)-(1×5)-Hex and Ir(100)-(1×2+2×1)-O surfaces. LEED, MEED, LMOKE and QMOKE studies were presented. The growth is found to be layer-by-layer at least up to 20 monolayers (ML) at room temperature. At higher deposition temperature, the MEED oscillations disappear around 3-5 ML. Magnetic anisotropy of the Fe(100) film grown on Ir(100)-(1×2+2×1)-O surfaces is evaluated using LMOKE measurement using Kerr microscope. Simultaneous in-situ LMOKE and MEED measurements were carried out during the deposition. Ferromagnetic ordering with an in-plane easy axis starts above 4.5 ML at room temperature. The Kerr rotation normalized by thickness is evaluated in the pseudomorphic regime and strain relaxed regime. The probing depth of the MOKE is found to be around 14 nm in Fe(100)/Ir(100). An antisymmetric component is observed in the re-magnetization loop measured using MOKE. This antisymmetric loop arises due to the quadratic magneto-optic coupling which is separated by symmetrization and antisymmetrization procedure. The observed quadratic magneto-optic coupling suggests that the analysis based on the assumption that the magneto-optic coupling is linear in magnetization has to be modified. In order to quantify the quadratic magneto-optic coupling parameters, a QMOKE measurement system is developed and measurements were carried out.
Chapter 6 discusses SPLEED experiments carried out on various thicknesses of Fe(100) film. Fe(100) films grown on Ir(100) substrate with the thickness less than or equal to 4 ML is not ferromagnetic with in-plane easy axis at room temperature. The non-zero exchange asymmetry observed for 5 ML and above indicates the presence of ferromagnetic ordering. A difference in the profile of exchange asymmetry is observed between pseudomorphic and strain relaxed regime. Large spin-orbit asymmetry is observed for 1 ML and 2 ML Fe(100) which is unexpected from a low atomic number (Z) material. The reason for large spin-orbit asymmetry is still unknown. The energy-angle landscape of reflectivity, exchange asymmetry, spin-orbit asymmetry and figure of merit were evaluated for 21 ML of Fe(100). Many working points were identified for different types multichannel spin filter based on exchange interaction
Finally, the various results are summarized and a broad outlook is given.
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Elektronenspektroskopie und Faktoranalyse zur Untersuchung von ionenbeschossenen Metall (Re, Ir, Cr, Fe)-Silizium-SchichtenReiche, Rainer 07 February 2000 (has links)
No description available.
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