976 resultados para SYNCHROTRON RADIATION SOURCES


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The results and discussions in this thesis are based on my studies about selfassembled thiol layers on gold, platinum, silver and copper surfaces. These kinds of layers are two-dimensional, one molecule thick and covalently organized at the surface. They are an easy way to modify surface properties. Self-assembly is today an intensive research field because of the promise it holds for producing new technology at nanoscale, the scale of atoms and molecules. These kinds of films have applications for example, in the fields of physics, biology, engineering, chemistry and computer science. Compared to the extensive literature concerning self-assembled monolayers (SAMs) on gold, little is known about the structure and properties of thiolbased SAMs on other metals. In this thesis I have focused on thiol layers on gold, platinum, silver and copper substrates. These studies can be regarded as a basic study of SAMs. Nevertheless, an understanding of the physical and chemical nature of SAMs allows the correlation between atomic structure and macroscopic properties. The results can be used as a starting point for many practical applications. X-ray photoelectron spectroscopy (XPS) and synchrotron radiation excited high resolution photoelectron spectroscopy (HR-XPS) together with time-offlight secondary ion mass spectrometry (ToF-SIMS) were applied to investigate thin organic films formed by the spontaneous adsorption of molecules on metal surfaces. Photoelectron spectroscopy was the main method used in these studies. In photoelectron spectroscopy, the sample is irradiated with photons and emitted photoelectrons are energy-analyzed. The obtained spectra give information about the atomic composition of the surface and about the chemical state of the detected elements. It is widely used in the study of thin layers and is a very powerful tool for this purpose. Some XPS results were complemented with ToF-SIMS measurements. It provides information on the chemical composition and molecular structure of the samples. Thiol (1-Dodecanethiol, CH3(CH2)11SH) solution was used to create SAMs on metal substrates. Uniform layers were formed on most of the studied metal surfaces. On platinum, surface aligned molecules were also detected in investigations by XPS and ToF-SIMS. The influence of radiation on the layer structure was studied, leading to the conclusion that parts of the hydrocarbon chains break off due to radiation and the rest of the layer is deformed. The results obtained showed differences depending on the substrate material. The influence of oxygen on layer formation was also studied. Thiol molecules were found to replace some of the oxygen from the metal surfaces.

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This thesis presents experimental studies of rare earth (RE) metal induced structures on Si(100) surfaces. Two divalent RE metal adsorbates, Eu and Yb, are investigated on nominally flat Si(100) and on vicinal, stepped Si(100) substrates. Several experimental methods have been applied, including scanning tunneling microscopy/spectroscopy (STM/STS), low energy electron diffraction (LEED), synchrotron radiation photoelectron spectroscopy (SR-PES), Auger electron spectroscopy (AES), thermal desorption spectroscopy (TDS), and work function change measurements (Δφ). Two stages can be distinguished in the initial growth of the RE/Si interface: the formation of a two-dimensional (2D) adsorbed layer at submonolayer coverage and the growth of a three-dimensional (3D) silicide phase at higher coverage. The 2D phase is studied for both adsorbates in order to discover whether they produce common reconstructions or reconstructions common to the other RE metals. For studies of the 3D phase Yb is chosen due to its ability to crystallize in a hexagonal AlB2 type lattice, which is the structure of RE silicide nanowires, therefore allowing for the possibility of the growth of one-dimensional (1D) wires. It is found that despite their similar electronic configuration, Eu and Yb do not form similar 2D reconstructions on Si(100). Instead, a wealth of 2D structures is observed and atomic models are proposed for the 2×3-type reconstructions. In addition, adsorbate induced modifications on surface morphology and orientational symmetry are observed. The formation of the Yb silicide phase follows the Stranski-Krastanov growth mode. Nanowires with the hexagonal lattice are observed on the flat Si(100) substrate, and moreover, an unexpectedly large variety of growth directions are revealed. On the vicinal substrate the growth of the silicide phase as 3D islands and wires depends drastically on the growth conditions. The conditions under which wires with high aspect ratio and single orientation parallel to the step edges can be formed are demonstrated.

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Chlorinated polymers (PVC, PVDC and E-CTFE) were irradiated with white light produced at the Brazilian Synchrotron Light Source (LNLS). The emitted gases were analyzed by mass spectrometry. The spectra were dominated by peaks related to hydrochloric acid, HCl, and chlorine (35Cl). The measured HCl intensity is used to evaluate the sensitivity of the polymers over a broad energy range. PVDC showed the greatest light sensitivity as compared to PVC and E-CTFE.

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A microcontrolled, portable and inexpensive photometer is described. It uses six light-emitting diodes (LEDs) as radiation sources and a phototransistor as detector, as well as a microcontroller (PIC - Programmable Controller of Interruption). This device provided total autonomy to the proposed photometer, which was successfully applied to determination of Fe2+ in ferrous syrups and of seven clinical biochemical parameters. As the components are cheap (~U$30.00) and easy to find, the proposed photometer is an economical alternative for routine chemical analyses in small laboratories, for research and teaching. Being portable and microcontrolled, it allows doing field chemical analyses.

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A threshold photoelectron spectrometer applied to the study of atomic and molecular threshold photoionization processes is described. The spectrometer has been used in conjunction with a toroidal grating monochromator at the National Synchrotron Radiation Laboratory (LNLS), Brazil. It can be tuned to accept threshold electrons (< 20 meV) and work with a power resolution of 716 (~18 meV at 12 eV) with a high signal/noise ratio. The performance of this apparatus and some characteristics of the TGM (Toroidal Grating Monochromator) beam line of LNLS are described and discussed by means of argon, O2 and N2 threshold photoelectron spectra.

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TiO2 immobilization on concrete was studied using mixtures with cement, varnish and resin. The UV radiation sources were a germicide UV lamp and solar light. Aqueous solutions of chloroform (CHCl3) and of phenol were prepared and recirculated over the TiO2 immobilized surfaces. The immobilized TiO2 surfaces showed better photocatalytic efficiency for phenol degradation compared to the control. For CHCl3, the presence or absence of the catalyst did not cause any significant difference to its degradation efficiency. The micrographic results showed a more homogeneous surface for TiO2 immobilized in resin and varnish.

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The understanding and engineering of bismuth (Bi) containing semiconductor surfaces are signi cant in the development of novel semiconductor materials for electronic and optoelectronic devices such as high-e ciency solar cells, lasers and light emitting diodes. For example, a Bi surface layer can be used as a surfactant which oats on a III-V compound-semiconductor surface during the epitaxial growth of IIIV lms. This Bi surfactant layer improves the lm-growth conditions if compared to the growth without the Bi layer. Therefore, detailed knowledge of the properties of the Bi/III-V surfaces is needed. In this thesis, well-de ned surface layers containing Bi have been produced on various III-V semiconductor substrates. The properties of these Bi-induced surfaces have been measured by low-energy electron di raction (LEED), scanning-tunneling microscopy and spectroscopy (STM), and synchrotron-radiation photoelectron spectroscopy. The experimental results have been compared with theoretically calculated results to resolve the atomic structures of the studied surfaces. The main ndings of this research concern the determination of the properties of an unusual Bi-containing (2×1) surface structure, the discovery and characterization of a uniform pattern of Bi nanolines, and the optimization of the preparation conditions for this Bi-nanoline pattern.

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This thesis is devoted to understanding and improving technologically important III-V compound semiconductor (e.g. GaAs, InAs, and InSb) surfaces and interfaces for devices. The surfaces and interfaces of crystalline III-V materials have a crucial role in the operation of field-effect-transistors (FET) and highefficiency solar-cells, for instance. However, the surfaces are also the most defective part of the semiconductor material and it is essential to decrease the amount of harmful surface or interface defects for the next-generation III-V semiconductor device applications. Any improvement in the crystal ordering at the semiconductor surface reduces the amount of defects and increases the material homogeneity. This is becoming more and more important when the semiconductor device structures decrease to atomic-scale dimensions. Toward that target, the effects of different adsorbates (i.e., Sn, In, and O) on the III-V surface structures and properties have been investigated in this work. Furthermore, novel thin-films have been synthesized, which show beneficial properties regarding the passivation of the reactive III-V surfaces. The work comprises ultra-high-vacuum (UHV) environment for the controlled fabrication of atomically ordered III-V(100) surfaces. The surface sensitive experimental methods [low energy electron diffraction (LEED), scanning tunneling microscopy/spectroscopy (STM/STS), and synchrotron radiation photoelectron spectroscopy (SRPES)] and computational density-functionaltheory (DFT) calculations are utilized for elucidating the atomic and electronic properties of the crucial III-V surfaces. The basic research results are also transferred to actual device tests by fabricating metal-oxide-semiconductor capacitors and utilizing the interface sensitive measurement techniques [capacitance voltage (CV) profiling, and photoluminescence (PL) spectroscopy] for the characterization. This part of the thesis includes the instrumentation of home-made UHV-compatible atomic-layer-deposition (ALD) reactor for growing good quality insulator layers. The results of this thesis elucidate the atomic structures of technologically promising Sn- and In-stabilized III-V compound semiconductor surfaces. It is shown that the Sn adsorbate induces an atomic structure with (1×2)/(1×4) surface symmetry which is characterized by Sn-group III dimers. Furthermore, the stability of peculiar ζa structure is demonstrated for the GaAs(100)-In surface. The beneficial effects of these surface structures regarding the crucial III-V oxide interface are demonstrated. Namely, it is found that it is possible to passivate the III-V surface by a careful atomic-scale engineering of the III-V surface prior to the gate-dielectric deposition. The thin (1×2)/(1×4)-Sn layer is found to catalyze the removal of harmful amorphous III-V oxides. Also, novel crystalline III-V-oxide structures are synthesized and it is shown that these structures improve the device characteristics. The finding of crystalline oxide structures is exploited by solving the atomic structure of InSb(100)(1×2) and elucidating the electronic structure of oxidized InSb(100) for the first time.

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Suomen ydinenergialaki vaatii ydinenergian käytössä syntyvän ydinjätteen käsittelyn ja varastoinnin sekä loppusijoittamisen Suomeen. Fortumin ja TVO:n ydinvoimalaitoksissa syntyvä käytetty ydinpolttoaine tullaan kapseloimaan ja loppusijoittamaan Olkiluotoon rakennettavassa kapselointi- ja loppusijoituslaitoksessa. Tämän työn tavoitteena on muodostaa kokonaiskuva kapselointi- ja loppusijoituslaitoksen säteilysuojelusta aikaisemmin tehtyjen selvitysten ja suunnitelmien perusteella. Kapselointilaitoksella käytetty ydinpolttoaine suljetaan kuparikapseleihin, jotka loppusijoitetaan maan alle loppusijoituslaitoksella. Työn aluksi kuvataan loppusijoitusmenetelmä ja kapselointi- ja loppusijoituslaitoksen käyttötoiminta. Tämän jälkeen käsitellään lainsäädäntöä ja viranomaisohjeita, jotka ohjaavat ydinlaitosten säteilysuojelua. Seuraavaksi käsitellään kapselointi- ja loppusijoituslaitoksella olevia säteilylähteitä. Lisäksi työssä käsitellään kapselointi- ja loppusijoituslaitokselle suunniteltua valvonta-aluetta ja sen säteilyolosuhteiden mukaista vyöhykejakoa. Työssä saatiin tulokseksi kokonaiskuva kapselointi- ja loppusijoituslaitoksen säteilysuojelusta. Kokonaiskuvan muodostamisen lisäksi laadittiin alustavia suunnitelmia käyttötoiminnan säteilysuojelun järjestämisestä. Lisäksi laadittiin ehdotuksia valvonta-alueen tarkemmista rajoista loppusijoituslaitoksella sekä havaittiin laitosten säteilysuojeluun liittyviä ongelmia ja esitettiin ratkaisuja niihin. Ongelmaksi osoittautui muun muassa, että kapselointi- ja loppusijoituslaitoksen valvonta-alueiden luonteiden eroa ei ollut huomioitu suunnitelmissa. Lisäksi todettiin, että nykyisin ydinlaitoksilla käytössä oleva valvonta-alueen vyöhykejako ei vastaa kapselointi- ja loppusijoituslaitosten tarpeita. Näihin esitettiin ratkaisuiksi laitosten välille perustettavaa kenkärajaa ja uuden korkeamman säteilyvyöhykkeen käyttöönottoa.

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Semiconductor laser devices are readily available and practical radiation sources providing wavelength tenability and high monochromaticity. Low-intensity red and near-infrared lasers are considered safe for use in clinical applications. However, adverse effects can occur via free radical generation, and the biological effects of these lasers from unusually high fluences or high doses have not yet been evaluated. Here, we evaluated the survival, filamentation induction and morphology of Escherichia coli cells deficient in repair of oxidative DNA lesions when exposed to low-intensity red and infrared lasers at unusually high fluences. Cultures of wild-type (AB1157), endonuclease III-deficient (JW1625-1), and endonuclease IV-deficient (JW2146-1) E. coli, in exponential and stationary growth phases, were exposed to red and infrared lasers (0, 250, 500, and 1000 J/cm2) to evaluate their survival rates, filamentation phenotype induction and cell morphologies. The results showed that low-intensity red and infrared lasers at high fluences are lethal, induce a filamentation phenotype, and alter the morphology of the E. coli cells. Low-intensity red and infrared lasers have potential to induce adverse effects on cells, whether used at unusually high fluences, or at high doses. Hence, there is a need to reinforce the importance of accurate dosimetry in therapeutic protocols.

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The research on the interaction between radiation and biomolecules pro-vides valuable information for both radiobiology and molecular physics. While radiobiology is interested in the damage inflicted on the molecule upon irradiation, molecular physics exploits these studies to obtain infor-mation about the physical properties of the molecule and the quantum me-chanical processes involved in the interaction. This thesis work investigated how a small change in the structure or composition of a biomolecule changes the response of the molecule to ioniz-ing radiation. Altogether eight different biomolecules were studied: nucleo-sides uridine, 5-methyluridine and thymidine; amino acids alanine, cysteine and serine; and halogenated acetic acids chloro- and bromoacetic acids. The effect of ionizing radiation on these molecules was studied on molecular level, investigating the samples in gas phase. Synchrotron radiation of VUV or soft x-ray range was used to ionize sample molecules, and the subsequent fragmentation processes were investigated with ion mass spectroscopy and ion-ion-electron coincidence spectroscopy. The comparison between the three nucleosides revealed that adding or removing a single functional group can affect not only the bonds from which the molecule ruptures upon ionization but also the charge localiza-tion in the formed fragments. Studies on amino acids and halogenated acetic acids indicated that one simple substitution in the molecule can dramatical-ly change the extent of fragmentation. This thesis work also demonstrates that in order to steer the radiation-induced fragmentation of the molecules, it is not always necessary to alter the amount of energy deposited on the molecules but selecting a suitable substitution may suffice.

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Die photoneninduzierte Fluoreszenzspektroskopie (PIFS) wurde als Methode zur Untersuchung von Fluoreszenzspektren der Edelgasatome Krypton und Xenon nach Anregung mit Synchrotronstrahlung des Elektronenspeicherrings BESSY II, Berlin, benutzt. Die Anregung der Edelgase erfolgte bei Zimmertemperatur und einem Druck von 40mTorr mit extrem schmalbandiger Strahlung mit DeltaE=3meV bei 21,55eV. Die untersuchten Anregungsenergiebereiche waren bei Krypton zwischen 29,4eV und 29,8eV und bei Xenon zwischen 23,74eV und 23,80eV, zwischen 24,4eV und 24,7eV und zwischen 25,25eV und 25,5eV. Die Anregungsenergiebereiche waren so gewählt, um Autoionisationsresonanzen untersuchen zu können, die erstmalig von Codling und Madden [J. Res. Nat. B. Stan. 1972, 76A, 1-12] veröffentlicht worden sind. Besonders die Besetzung in Abhängigkeit der Anregungsenergie von Satellitenzuständen in den jeweiligen einfach geladenen Ionen durch vorherige Anregung der genannten Autoionisationsresonanzen war der Fokus der vorliegenden Arbeit.

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Die lokale Anlagerung molekularer Substanzen auf Oberflächen ist technologisch von großem Interesse. Die Beeinflussung selbstassemblierender Materialien bietet dabei große Vorteile, da sie kostengünstig und großflächig angewendet werden kann. Untersuchungen einer solchen Beeinflussung mithilfe von magnetischen Feldern wurden bisher jedoch noch nicht durchgeführt. Ursache hierfür ist das, insbesondere bei der Verwendung von diamagnetischen Substanzen, geringe induzierte magnetische Moment und die daraus resultierenden geringen magnetischen Kräfte. In der vorliegenden Arbeit wurde untersucht, ob es möglich ist, die lokale Anlagerung von selbstassemblierenden, diamagnetischen Substanzen durch die Verwendung von magnetischen Streufeldern zu beeinflussen und somit ein Schichtwachstum bevorzugt in gewünschten Bereichen eines Substrats zu erreichen. Es wurde ein austauschverschobenes Dünnschichtsystem über das Verfahren der ionenbeschuss-induzierten magnetischen Strukturierung mit einem künstlichen Domänenmuster in streifenförmiger Anordnung im Mikrometermaßstab erzeugt. Über experimentelle Untersuchungen wurden die aus diesem Schichtsystem austretenden magnetischen Streufelder erstmals quantifiziert. Die experimentell unvermeidbaren Mittelungen und technischen Limitierungen wurden mithilfe eines theoretischen Modells herausgerechnet, sodass letztlich die resultierende Magnetfeldlandschaft in allen drei Dimensionen über der Probenoberfläche erhalten wurde. Durch die Bestimmung der magnetischen Suszeptibilitäten der hier verwendeten thioethersubstituierten Subphthalocyanin-Derivate konnte somit die Berechnung der induzierten magnetischen Kräfte erfolgen, deren Vergleich mit Literaturwerten eine erfolgreiche Beeinflussung der Anlagerung dieser Substanzen erhoffen ließ. Aufgrund der Kombination diverser, anspruchsvoller Nachweisverfahren konnte der experimentelle Beweis für die erfolgreiche Positionierung der molekularen Substanzen durch die magnetischen Streufelder des Dünnschichtsystems erbracht werden. Zunächst wurde nachgewiesen, dass sich die Subphthalocyanin-Derivate auf der Probenoberfläche befinden und in einer mit der Periode der magnetischen Domänenstruktur korrelierenden Geometrie anlagern. Über Untersuchungen an Synchrotronstrahlungsquellen konnte die magnetische Streifenstruktur mit der Struktur der angelagerten Moleküle überlagert werden, sodass bekannt wurde, dass sich die Moleküle bevorzugt in den magnetisch begünstigten Bereichen anlagern. Um mögliche Einflüsse einer eventuell durch den magnetischen Strukturierungsprozess lokal modifizierten Substratoberfläche als Ursache für die lokale Molekülanlagerung ausschließen zu können, wurden zusätzliche Referenzmessungen durchgeführt. Alle Untersuchungen zeigen, dass die Molekülpositionierung auf der Wechselwirkung der diamagnetischen Substanzen mit den Streufeldern des Substrats zurückzuführen ist. Der im Rahmen dieser Arbeit entwickelte Mechanismus der magnetischen Beeinflussung der lokalen Molekülanlagerung besagt dabei, dass insbesondere die Oberflächendiffusion der selbstassemblierenden Substanz durch die in-plane-Magnetfeldkomponente beeinflusst wird und vermutlich die Nukleationsphase der Selbstassemblierung entscheidend für die lokale Materialabscheidung ist. Es konnte in dieser Arbeit somit gezeigt werden, dass eine Beeinflussung der Selbstassemblierung von diamagnetischen Subphthalocyanin-Derivaten und somit eine lokal bevorzugte Anlagerung dieser Substanzen durch magnetische Streufelder von magnetisch strukturierten austauschverschobenen Dünnschichtsystemen erreicht werden kann. Es resultiert somit eine neue Möglichkeit die technologisch wichtigen Selbstassemblierungsprozesse nun auch über magnetische Streufelder beeinflussen und kontrollieren zu können. Durch die hohe Flexibilität bei den Strukturierungsmöglichkeiten der magnetischen Domänengeometrien der hier verwendeten austauschverschobenen Dünnschichtsysteme resultieren aus den hier gezeigten Ergebnissen vielfältige Anwendungsmöglichkeiten im Bereich der Beschichtungstechnik.

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The adsorption of L-CySteine and L-methionine amino acids on a chiral Cu{5 3 1} surface was investigated with high resolution X-ray photoelectron spectroscopy (XPS) and carbon K-edge near edge X-ray absorption fine structure (NEXAFS) Spectroscopy using synchrotron radiation. XPS shows that at 300 K L-cysteine adsorbs through two oxygen, a nitrogen and a sulfur atom, in a four point 'quadrangular footprint', whereas L-methionine adsorbs through only two oxygen and a nitrogen atom in a 'triangular footprint'. NEWS was used to clarify the adsorption geometry of both molecules, which suggests a binding orientation to the top layer and second layer atoms in two different orientations associated with adsorption sites on {1 1 0} and {3 1 1} microfacets; of the Cu{5 3 1} surface. (C) 2009 Elsevier B.V. All rights reserved.