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- resonant photoelectron spectroscopy (4)
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This chapter reports about tin oxide (SnO₂), a material which belongs to the transparent conducting oxide family and is best characterized by its high conductivity, high carrier mobility, and the ability to form p-type conductivity. We correlate these properties in terms of localized intrinsic electronic defect states which are resolved by resonant photoelectron spectroscopy measurements. We describe SnO₂ in terms of an inhomogeneous, mixed-ionic-covalent semiconductor in which these intrinsic electronic defects state are stabilized.
Exploring efficient and inexpensive electrocatalysts for the oxidation of water is of great importance for various electrochemical energy
storage and conversion technologies. In the present study, a new water-soluble [Ce
III(DMF) (HSO4)3] complex was synthesized and characterized
by UV−vis, photoluminescence, and high-resolution X-ray photoelectron spectroscopy techniques. Owing to classic 5d →4f transitions, an intense
photoluminescence in the UV region was observed from the water-soluble [CeIII(DMF)(HSO4)3] complex. A stacking electrode was designed where
self-assembled L-cysteine monolayer modified gold was immobilized with the synthesized cerium complex and was characterized by scanning electron microscopy, electrochemical impedance spectroscopy, and cyclic voltam-metry. The resulting electrode, i.e., [CeIII(DMF)(HSO4)3]−L-cysteine-Au
stacks shows high electrocatalytic water oxidation behavior at an
overpotential of η ≈0.34 V under neutral pH conditions. We also demonstrated a way where the overpotential is possible to decrease upon irradiation of UV light.
We report on the X-ray absorption data for Indium–Gallium–Zink–Oxide thin films, amorphous ZnO films, amorphous SnOx films, and single crystalline In2O3, Ga2O3, ZnO, and SnO2 data. These absorption data probe the empty conduction band states explicitly. Also they allow for an elemental assignment using resonant excitation to derive the contributions of each metal ion. We find that the lowest states appear right at the Fermi energy and result from configuration interaction induced charge transfer states which we consider as intrinsic gap states.
The electronic structure of a SnO2 single crystal is determined by employing resonant photoelectron spectroscopy. We determine the core level, valence band, and X-ray absorption (XAS) data and compare these with those of amorphous SnOx thin films. We find similar properties concerning the data of the core levels, the valence band features, and the absorption data at the O1s
edge. We find strong signals arising from intrinsic in-gap states and discuss their origin in terms of polaronic and charge-transfer defects. We deduce from the XAS data recorded at the Sn3d edge
that the Sn4d10 ground state has contributions of 4d9 and 4d8 states due to configuration interaction.
We identify localized electronic states depending on the strength of the 4d-5s5p interaction and of
the O2p-to-Sn4d charge-transfer processes, both appear separated from the extended band-like states of the conduction band. For the amorphous SnOx thin films, significant differences are found only in the absorption data at the Sn3d-edge due to a stronger localization of the in-gap states.
Die Materialklasse der transparenten leitenden Metalloxide (engl. transparent conducting oxides (TCO)) und amorphen oxidischen Dünnschichtsysteme (engl. amorphous oxidic semiconductors (AOS)) sind überaus faszinierend, da sie gegensätzliche physikalische Eigenschaften, wie Transparenz und hohe Leitfähigkeit in sich vereinen. Die zugrunde liegenden physikalischen Mechanismen sind immer noch unklar und werden in dieser Dissertation beleuchtet. Dazu wurde die resonante Photoelektronenspektroskopie (resPES)gewählt, da sie sich in den letzten Jahren als vielseitiges Werkzeug für die detaillierte Untersuchung der elektronischen Struktur und der Identifikation von Defekten ausgezeichnet hat. Im Rahmen dieser Arbeit ergab sie die einmalige Möglichkeit, sowohl hoch qualitative TCO-Einkristalle (ZnO, Ga2O3, In2O3 und SnO2) als auch amorphe oxidische Dünnschichtsysteme (GIZO und SnOx) photeelektronenspektroskopisch zu untersuchen und zu vergleichen. Somit wird gezeigt, dass die elektronische Struktur der Materialklasse der TCO und ihrer korrespondierenden AOS mehr Gemeinsamkeiten aufweisen, als bisher erwartet wurde.
Es zeigt sich, dass die Bandlücke, im eigentlichen Sinne, in der Materialklasse der TCO und AOS nicht existiert. Lokalisierte Zustände füllen den gesamten Bereich dieser Bandlücke aus und reichen zum Teil in das Valenzband (VB) und Leitungsband (CB) hinein. Dies führt dazu, dass es keine, wie bisher gedacht, scharfen Grenzen zwischen lokalisierten und delokalisierten Zuständen gibt. Um dies zu verdeutlichen wird ein neuartiges Modell eingeführt, das aufzeigt, dass die Wechselwirkung von metallischen d- und s-Niveaus in einer Öffnung der d-Schale resultiert. Durch Charge-Transfer (CT)-Mechanismen und weitere Hybridisierung mit metallischen unbesetzten p-Zuständen folgt eine stärkere Lokalisierung. Die Diskussion wird begonnen mit der Klärung der Elementeverhältnisse der untersuchten Materialsysteme. Darauf folgt die Charakterisierung von intrinsischen Defekten und ihren Beiträgen auf die elektronische Struktur. Abschließend werden die elektronischen Strukturen der AOS mit denen der korrespondierenden TCO verglichen.
A flexible nanogenerator (NG) is fabricated with a poly(vinylidene fluoride) (PVDF)film, where deoxyribonu-cleic acid (DNA) is the agent for the electroactive β-phase
nucleation. Denatured DNA is co-operating to align the
molecular−CH2/−CF2 dipoles of PVDF causing piezo- electricity without electrical poling. The NG is capable of harvesting energy from a variety of easily accessible mechanical
stress such as human touch, machine vibration, football
juggling, and walking. The NG exhibits high piezoelectric
energy conversion efficiency facilitating the instant turn-on of several green or blue light-emitting diodes. The generated energy can be used to charge capacitors providing a wide scope
for the design of self-powered portable devices.
Spin State and Satellite Structures of ε-Fe₂O₃ as determined by Resonant Photoelectron Spectroscopy
(2015)
We use resonant photoelectron spectroscopy at the Fe2p and the O1s absorption edges to report on spectroscopic investigation of Fe-oxides nanoparticles. We discuss the spectroscopic details like multiple Auger decays, satellite emission in the X-ray absorption process and the core level data. We explain these data by a novel mechanism in which the resonant excitation between Fe3d and Fe4s states are involved.
This mechanism is observed when the photo-excited electron becomes polarized by the electron–hole pairs existing in the conduction and valence bands.
We compare the electronic properties of amorphous p-type SnOx thin film grown by rf magnetron sputtering with those of n-type SnO2 single crystals grown by cvt. We use resPES to study the electronic band structure. We measure the core levels, the VB PES data, partial Integrated Yield (pIY) and the XAS absorption data. From the resPES data recorded at the O1s and the Sn3d edges we derive the VB pDOS and the CB pDOS . The differences are most pronounced in the position of the VBM as for the a-SnOx films there appears a band closer to the Fermi energy. In addition for the SnOx we find in the XAS and pIY data a significant peak that appears right at the Fermi energy. This peak is absent in the single crystalline data. We attribute this to a change in the configuration of the Sn4d states to form a 4d8 configuration instead of 4d9 and 4d10 configurations which are identified in the single crystalline data.
Dünne Al2O3-Schichten wurden bei Substrattemperaturen zwischen Raumtemperatur und 200°C mittels PE-ALD auf Si-Substraten abgeschieden und ellipsometrisch, spektroskopisch und elektrisch charakterisiert. Ihr Potenzial für die chemische und Feldeffektpassivierung der Oberflächenrekombination wird bewertet.
We use resonant photoemission spectroscopy (resPES) to study the electronic properties of amorphous ZnO (a-ZnO) layers. We report on the core levels, the valence band (VB) PES data, and the X-ray absorption (XAS) data which we use for the conduction band (CB) density of states. From these results we are able to derive the partial density of states
(pDOS) of O2p and Zn4s4p states in the VB and CB, respectively as well as a band scheme. At the O1s resonance we observe a band of localized defect states which is located between the Fermi energy and the CBM. At the Zn2p edge the XAS data indicate that localized Zn4s4p states are involved in the DOS starting already at the Fermi energy.