In der vorliegenden Dissertation werden die elektronischen Eigenschaften der c(2x2)MnCu/Cu(001) Oberfläche untersucht. Es wird eine Möglichkeit vorgestellt, unter Nutzung verschiedener Symmetrien der Brillouinzonen, Photoemissionsspektren voneinander zu trennen und damit die energetische Position des Mayoritätsspinbandes von Mangan in der c(2x2) Überstruktur zu bestimmen. Es konnte mittels Vergleich zu Rechnungen der Bandstruktur außerdem festgestellt werden, daß Teile des Minoritätsspinbandes besetzt werden. Die Fermioberfläche des c(2x2)MnCu/Cu(001) Systems wurde mittels Photoemission untersucht. Es konnte weiterhin gezeigt werden, daß Kupfer epitaktisch auf dieser Oberfläche aufwächst und weitere c(2x2)MnCu Sequenzen gewachsen werden können, wobei sich auch hier die Manganatome in einem magnetischen Grundzustand befinden. Es wird das Wachstum von Mangan auf Eisen, Kobalt und Nickel analysiert. Dafür werden dünne Eisen-, Kobalt- und Nickelschichten auf einem Kupfer-(001)-Einkristall präpariert und damit eine metastabile flächenzentrierte Oberfläche geschaffen, die wiederum als Substrat für das Mangan dient. Alle diese Zwischenschritte werden von Untersuchungen der elektronischen Eigenschaften mittels Photoemissionsmessungen begleitet, die dazu dienen, Aussagen über die Bandstruktur und die Fermi-Oberfläche zu erhalten. Diese experimentellen Daten werden anschließend mit theoretisch berechneten Daten verglichen und daraus Schlußfolgerungen für den Magnetismus in den einzelnen Systemen getroffen. / This thesis deals about the electronic properties of the c(2x2)MnCu/Cu(001) surface. Under use of different symmetries in the Brillouin zones, a possibility for the separation of photoemission spectra is presented and the energy position of the manganese spin majority band is determined. Furthermore, a comparison with theoretic studies found part of the spin minority band occupied. The Fermi surface of the c(2x2)MnCu/Cu(001) system was analysed. It could be shown, that copper grows epitaxially on top of this surface and a further growth of c(2x2)MnCu sequences is possible with the manganese atoms in a high spin ground state. Further, the growth of manganese on iron, cobalt, and nickel will be investigated. For this purpose thin iron, cobalt, and nickel films are prepared on a copper-(001) crystal and the resulting metastable face centred surface can be used as a substrate for the manganese. All these intermediate steps are accompanied by investigations of the electronic properties using photoemission, that give an insight in the band structure and the Fermi surface. The experimental data will be compared to theory and some conclusions about the magnetism of the systems can be drawn.

In dieser Arbeit wurden Ergebnisse einer Analyse der elektronischen Struktur in Sr2CuO2Cl2 mittels winkelaufgelöster Photoemission dargelegt. Sie betreffen i) Sr2CuO2Cl2 als Untersuchungsgegenstand für die Grundlagenforschung an Hochtemperatursupraleitern (HTSL), ii) winkelaufgelöste Photoemission als Untersuchungsmethode zur Messung der elektronischen Struktur von HTSL und deren Muttersubstanzen, iii) Eigenschaften der elektronische Anregungen in Sr2CuO2Cl2 in unmittelbarer Nähe des chemischen Potenzials, sowie iv) das durch Korrelationen stark beeinflusste Dotierungsverhalten der Kuprate. 1. Sr2CuO2Cl2 eignet sich Dank seiner exakten Stöchiometrie und der strukturell perfekten Kupfer-Sauerstoff Ebenen hervorragend als Untersuchungssubstanz für die isolierende Phase der HTSL. 2. Mittels winkelaufgelöster Photoemission ist es möglich, die k-Raum- und Energieverteilung (Dispersion) von Anregungen nahe des chemischen Potenzials in Sr2CuO2Cl2 auszumessen. Dabei wurde eine starke Abhängigkeit der Intensität des Photoemissionssignales in Abhängigkeit von der Photonenenergie beobachtet. Es konnte nachgewiesen werden, dass sich diese Intensitätsoszillationen mit hoher Wahrscheinlichkeit durch eine Bragg-Interferenz der Photoelektronenewelle an der Schichtstruktur von Sr2CuO2Cl2 erklären und weiterhin, dass die gemessenen Dispersionskurven, von einer willkürlichen Normierung der Intensität abgesehen, unabhängig von der verwendeten Photoenenenergie sind. 3. Die Photoemissionsspektren von Sr2CuO2Cl2 zeigen die für Ladungstransfer-Isolatoren charakteristische Aufteilung des spektralen Gewichts (der besetzten Elektronenstruktur) in ein unteres Hubbardband, bindende und nichtbindende Sauerstoffbänder und der ZR-Singlet Struktur. Dabei konnte das untere Hubbardband identifiziert werden durch seine durch Resonanz hervorgerufene Intensitätsverstärkung (und dem daraus resultierenden d8-Charakter dieser Struktur), die Sauerstoffbänder und die ZR-Singlet Struktur durch eine Analyse ihres Symmetrieverhaltens unter Berücksichtigung der Polarisationsabhängigkeit des Photoemissionssignales. Das ZR-Singlet besitzt eine a1g-Symmetrie was sowohl die Konstruktion des ZR-Singlets nach Zhang und Rice als auch die Ergebnisse der Diagonalisierung der isolierten, mit zwei Löchern besetzten Plakette bestätigt. 4. Die Dispersion des ZR-Singlets ist parabolisch entlang Gamma-(Pi,Pi) mit einem absoluten Bindungsenergieminimum bei (0.5Pi,0.5Pi) und parabolisch entlang Gamma-(Pi,0) mit einem lokalen Bindungsenergieminimum bei (0.7Pi,0). Die Bandbreite entlang dieser beiden Richtungen beträgt etwa 300 meV beziehungsweise 200 meV, der Abstand der beiden minimalen Bindungsenergien entlang dieser Richtungen ist 72 meV. Das Spektralgewicht des ZR-Singlets ist keilförmig verteilt mit einem Maximum bei (0.5Pi,0.5Pi) und (0.7Pi,0), also jeweils in unmittelbarer Nähe der minimalen Bindungsenergien dieser Struktur. Es verschwindet bei Gamma und (Pi,Pi), hat jedoch einen endlichen Wert bei (Pi,0). Der Vergleich dieser Resultate favorisiert das erweiterte t-J-Modell zur Beschreibung der Dynamik des ZR-Singlets. Insbesondere i) die parabolische Dispersion des ZR-Singlets entlang Gamma-(Pi,Pi), ii) der geringe aber endliche energetische Abstand der Bindungsenergie-Minima entlang Gamma-(Pi,Pi) und Gamma-(Pi,0) und iii) die keilförmige Verteilung des Spektralen Gewichts entlang Gamma-(Pi,0) sind die experimentellen Indizien dafür. / A detailed ARPES study of the low binding-energy occupied electronic structure of Sr2CuO2Cl2 has been done. It corresponds to an investigation of the first electron-removal states of an undoped CuO2-plane: 1. The photoemission signal of the first electron-removal states at both (0.5Pi,0.5Pi) and (0.7Pi,0) exhibits a marked photon-energy dependence. The intensity profile shows strong oscillations with maxima near 16, 25, 35 and 49 eV, corresponding to final state crystal momenta kperp=0.82, 1.63, 2.40 and 3.12 A-1. 2. Along the high-symmetry directions Gamma-(Pi,Pi) and Gamma-(Pi,0) the first electron-removal states shows a strong polarization dependence. This can be linked to the strongly polarization-dependent matrix element, which in turn allows the determination of the symmetry of the first electron-removal state itself. For both high-symmetry directions we observe a polarization dependence in keeping with that expected for a Zhang-Rice singlet state in the framework of either a three-band or one-band model Hamiltonian. 3. Our data show that the dispersion of the first electron-removal states along both high symmetry directions (Gamma-(Pi,Pi) and Gamma-(Pi,0)) is parabolic-like and independent of the excitation energy. This, and the rather large difference in lowest binding energy of the first electron-removal state along these directions, shows the validity of the extended t-J model for describing the disperion relation of a single hole in an antiferromagnetic CuO2 plane. Thus, the inclusion of second (t2) and third (t3) neighbor hopping terms with realistic values of t2=-0.08 and t3=0.15 in units of the next neighbor hopping t=t1 are required. 4. Upon application of a simple fit procedure, we infer the momentum distribution of the spectral weight of the coherent and incoherent part of the first electron-removal state to have its maximum along Gamma-(Pi,Pi) at (0.5Pi,0.5Pi), being symmetrically suppressed away from this point. Along Gamma-(Pi,0) the spectral weights of both parts reach their maximum at (0.7Pi,0) and then drop fast. The ratio between the coherent and incoherent spectral weight is strongly photon-energy dependent, which, at first sight would appear to violate the physics of the spectral function: (i) the necessity for a more sophisticated framework in which to analyse the weight of the coherent and incoherent contributions to the spectral weight (ii) significant (hn-dependent) intensity due to extrinsic processes (iii) intensity in this energy region due to intrinsic electronic states other than the Zhang-Rice singlet.

XX

The studies presented in this work are aimed towards a better understanding of the fundamental physics of the electrode/organic molecule interface in both the ground and excited state manifolds. Systematic investigations of single systems using two-photon photoemission (TPPE) and ultraviolet photoelectron spectroscopy (UPS) were undertaken in order to assess the evolution of the electronic structure and molecular organization at the interface. The adsorbate molecule vanadyl naphthalocyanine (VONc) was used whose properties are well-suited to this purpose. Interfacial electronic states of thin films of VONc were studied with two different substrates: highly ordered pyrolytic graphite (HOPG) and Au(111).The substrate of HOPG is a surface which does not possess reactive dangling bonds and the electron density close to the Fermi edge is very low, permitting high resolution spectroscopic band analysis of VONc and revealing subtle changes to the electronic structure. From interfacial studies of this weakly interacting substrate/ adsorbate system, it is shown in this work that molecular electronic levels in both the ground and excited state manifolds can shift independently of the vacuum level. Further, electron transfer between close lying electron donor and acceptor energy levels may be influenced by energy level shifts caused by depolarization effects as a function of dipole density.The VONc/Au(111) interface is investigated in order to examine energy level alignment in a system with the additional complexity of molecule/substrate interactions. The electron rich Au(111) surface leads to a strong interface dipole upon addition of VONc. Joint experimental and computational data is presented showing that the underlying cause of this interface dipole is Pauli repulsion. Additionally, investigations of energy level alignment in the excited state manifold are presented and the possibility of quantum interference is discussed.The interfacial electronic structure is quite different among these two model systems. The interfacial alignment observed in the HOPG/VONc system was largely due to depolarization of the intrinsic molecular dipole as a function of density, whereas the Au(111)/VONc interface is dominated by interfacial Pauli repulsion interactions.

No description available.

La thèse présente l'élaboration et l'étude des films minces (35 nm) cristallins et stœchiométriques de la magnétite Fe304(001)/MgO. La qualité de ces films est étudiée par différentes techniques (DEL, XPS, XMCD, Effet Kerr, Auger). Nous supposons que les films se recouvrent partiellement, même sous ultra vide, par de Fe2O3. Pour la première fois, l'étude de la structure électronique de la bande t2g de ces films est réalisée par photoémission résolue en angle (ARPES)à température ambiante et à 75 K, en utilisant des photons à basses énergies (6eV - 21 eV). Nous avons constaté que le signal de la photoémission est composé des états électroniques de deux périodicités liées à la zone de Brillouin primitive de la surface (a=4.2 Å) et à la zone de Brillouin de la reconstruction de la surface (a=8.4 Å). Nous pensons que la présence des états liés à la reconstruction sont probablement responsables de la chute de la densité d'état à EF. Une signature de Verwey est observée par ARPES à basse température. Nous estimons que la réalisation des films ultra minces de magnétite est difficilement aboutie. / With its half-metallic behavior predicted theoretically, the magnetic oxideFe3O4 (TC = 863 K) is promising for applications in spintronics as thin films.High quality films and the electronic band structure are still a challenge to faceexperimentally. We managed to develop single crystalline Fe3O4(0 0 1) films(35 nm) on MgO. Analysis by XPS, XAS and XMCD allowed to characterizethe quality of the films prepared. The magnetic study shows a perfect XMCDsignal and a form magnetic anisotropy which lays down the axis of easy magnetizationin the film plane. Our samples are stable during the photoemissionmeasurements. The photoemission measurements of the t2g band show thatthe electronic bands cannot be described by a DFT calculation. Indeed, spinpolarons due to strong electron-phonon coupling mechanism are involved inthe electronic transport. Angle-resolved photoemission shows a dispersion ofthe t2g band in the ����M direction corresponding to two periodicities [the unitcell of the surface reconstruction a = 8,4 Å (30% of the signal) and the simpleunit cell of the surface a = 4;2 Å]. At a temperature T < TV (TV = 120 K,Verwey temperature), the angle-resolved photoemission shows the opening ofa 100 meV band gap, with a rigid shift of the spectral weight of the t2g bandto the high binding energy side.

La magnétite (Fe3O4) est un candidat prometteur pour des applications dans des dispositifs en spintronique. Ce ferrimagnétique avec une température de Curie élevée a été théoriquement prévu pour être un demi-métal avec un canal conducteur pour les spins minoritaire et un semi-conducteur pour les spins majoritaires, résultant en 100% de polarisation en spin au niveau de Fermi. Cependant, jusqu'à présent, aucune preuve expérimentale claire sur ce sujet n'a été faite. Cette thèse présente des études en photoémission résolue en angle et en spin sur la structure électronique et magnétique de couches minces de Fe3O4 (001) épitaxiées sur MgO(001) . Un calcul de la structure de bande utilisant l'approximation du gradient généralisé (GGA + U) est proposé pour expliquer les résultats expérimentaux. Bien que l'intensité de photémission au niveau de Fermi soit très faible en raison du rôle joué par les polarons, une dispersion de la bande Fe 3d-t2g est observée. Le comportement global de cette bande est en bon accord avec le calcul de la structure état électronique représentant état fondamental. Pour simuler les spectres de photoémission, nous avons utilisé l'approximation de l'électron libre à l'état final, tout en ignorant les éléments de matrice de la transition électronique. Dans la simulation, les bandes calculées sont convoluées respectivement par la lorentzienne et la gaussien pour tenir compte de la durée de vie et des effets de couplage électron-phonon. En intégrant l'intensité spectrale sur un intervalle d'énergie de 100 MeV au niveau de Fermi, nous avons obtenu la première preuve expérimentale de la surface de Fermi. Détermination de la polarisation de spin des électrons est un test ultime des calculs de bandes et des spectres de photoémission modélisés. Dans nos expériences de photoémission résolue en spin, nous avons utilisé des photons de 4.65 et 6.20 eV. Le même échantillon comme pour la photoémission intégré en spin a été mesuré, nécessitant son transfert par l'air dans une autre chambre. L'échantillons n'a pas été soumis à un nettoyage avant les mesures résolues en spin ce a conduit à une réduction de la polarisation en spin à cause de la présence d'une couche polluée sur la surface. Néanmoins, une polarisation de spin de - 50% et -72 % a été mesurée au voisinage de EF respectivement pour les photons de 6.20 et de 4.65 eV. Nous en concluons que Fe3O4 peuvent être décrits par un modèle de bande et en particulier qu'il est demi-métallique. Nous avons également utilisé des impulsions femtoseconde laser dans une expérience pompe-sonde pour étudier la dynamique ultra-rapide à l'échelle atomique. Nos résultats montrent que la durée de vie des électrons excités dans Fe3O4 est beaucoup plus longue que dans un métal «ordinaire». L'analyse de la polarisation en spin des électrons excités montre que la désaimantation ne se produit pas dans le domaine de la femtoseconde, ce qui est compatible avec des propriétés demi-métalliques de la magnétite . / Magnetite (Fe3O4) is a promising candidate for application in spintronic devices. This ferrimagnet with a high Curie temperature has been theoretically predicted to be a half-metal with a conductive minority-spin (↓) channel and a semiconductive majority-spin (↑) channel, resulting in 100 % spin polarization at the Fermi level. But up to now, any clear experimental evidence is lacking. This thesis presents spin- and angle-resolved photoemission studies on the magnetic and electronic structure of Fe3O4 (001) epitaxially grown on MgO (001). A band structure calculation using generalized gradient approximation plus U (GGA+U) to the density functional theory (DFT) is proposed to explain the experimental results. Although the PES intensity at Fermi level is very low because of the role played by polarons, a dispersion of the Fe 3d-t2g states is observed. The overall behaviour of these bands is in good agreement with the calculation of ground state electronic structure. In order to simulate the spectra, we used the free electron approximation for the final states, ignoring the matrix elements. Calculated ground state data are convoluted by Lorentzian and Gaussian functions to account for the lifetime and electron-phonon coupling effects, respectively. By integrating the spectral intensity over an energy interval of 100meV at Fermi level, we obtained the first experimental evidence of the Fermi surface plot. Determination of electron spin polarization is an ultimate test of both the band calculations and our model of Fe3O4 photoemission spectra. In our spin-resolved photoemission experiments 4.65 and 6.20 eV photons were used. The same sample was used as for spin-integrated ARPES, requiring its transfer through air to another chamber. It was not subject to any cleaning prior to the SRPES measurements that lead to a reduction of the spin polarization as a consequence of the presence of a dead layer on the surface. Nevertheless the spin polarization close to EF reaches - 50% and -72% for 6.20 and 4.65 eV photons respectively. We conclude that Fe3O4 can be described within a band model and in particular that it is half-metallic. We also used femtosecond laser pulses in pump-probe experiments to investigate ultrafast dynamics on atomic scale. Our results show that the lifetime of excited electrons in Fe3O4 is much longer than in an “ordinary” metal. From the spin analysis of excited electrons, we deduce that the demagnetization does not occur in the femtosecond range, which is compatible with half-metallic properties of magnetite.</dcterms:abstract> <dc:type xsi:type="dcterms:DCMIType"

Espectros de foto-emissão são calculados com um modelo simples para a adsorção química em superfícies metálicas. Neste modelo já discutido por outros autores, o metal é representado por uma banda de condução semipreenchida e o íon adsorvido por dois níveis: um nível profundo, inicialmente ocupado pelo fotoelétron e o segundo, um nível ressonante, um orbital do átomo adsorvido o qual, atraído pelo potencial do buraco profundo, é deslocado para abaixo da energia de Fermi. O cálculo, baseado nas técnicas de grupo de renormalização desenvolvidas por Wilson para resolver o problema Kondo, considera pela primeira vez a interação eletrostática entre o buraco profundo e os estados de condução. Os resultados mostram que esta interação reduz efetivamente o acoplamento entre o nível ressonante e a banda de condução, e, portanto, modifica qualitativamente os espectros de foto-emissão. / X-Ray Photoemission spectra (XPS) are calculated for a simple model for chemisorptions on metallic surfaces. In the spineless model, already discussed by other authors, the metal is represented by a half-filled conduction band and the adsorbed ion by two levels, one representative of a deep core state initially occupied by the photoelectron and the second, a resonant level, of an initially empty adsorbate orbital which, attracted by the core hole potential, is dragged below the Fermi energy. The calculation based on the renormalization group techniques devised by Wilson to analyze the Rondo problem, accounts for the first time for the electrostatic interaction between the core hole and the conduction states. The results show that this interaction effectively narrows the coupling between the resonant level and the conduction band and hence changes qualitatively the photoemission spectra.

Thesis advisor: Hong Ding / Thesis advisor: Ziqiang Wang / The discovery of the high-T_c superconductivity in iron-arsenic materials in 2008 immediately became one of the hottest topics in the condensed matter physics. This dissertation presents a systematic study on the pairing symmetry and electronic structure on the hole doped materials of BaFe₂As₂ (so called &ldquo;122&rdquo;-system), by angle-resolved photoemission spectroscopy (ARPES). In the early ARPES studies on &ldquo;122&rdquo;-pnictides, we observed two hole-like Fermi surfaces (FSs) centered at the Brillouin zone (BZ) center, (&Gamma;), and two electron-like FSs centered at the zone corner (M), which is (&pi;, &pi;) in the BZ or (&pi;, 0) in the unfolded BZ. The size of these FS sheets can be changed by carrier doping, which causes change of the chemical potential. In the superconducting state, temperature (<italic>T</italic>) and momentum (<italic>k</italic>) dependence of ARPES measurements reveals the Fermi-surface-dependent nodeless superconducting gaps in this system and shows that an <italic>s</italic>-wave symmetry is the most natural interpretation for our findings in terms of the pairing order parameter. The ratio 2&Delta;/k_BT_c switches from weak to strong coupling on different FS sheets. Large superconducting gaps are observed with a strong coupling coefficient (2&Delta;/k_BT_c) on the near-nested FSs connected by the antiferromagnetic (AF) wave vector ((&pi;, &pi;) in the BZ or (&pi;, 0) in the unfolded BZ). When T_c is suppressed in the heavily overdoped materials, the near-nesting condition vanishes, or more precisely, the (&pi;, &pi;) inter-FS scattering disappears due to the absence of either the hole-like or the electron-like FS at the Fermi energy (E_F). We have also performed ARPES measurements on k_z-dependence of the superconducting gap and band structure of the optimally hole doped sample Ba_0.6K_0.4Fe₂As₂. By varying the photon energy, we can tune k_z continuously. While significant k_z dispersion of the superconducting gaps is observed on the hole-like bands, much weaker k_z dispersion of the superconducting gaps is observed on the electron-like bands. Remarkably, we find that a 3D gap function based on short-range pairing can fit the superconducting gaps on all the FS sheets. Moreover, an additional hole-like FS (referred as the &alpha;<super>&lsquo;</super> FS) predicted by local density approximation (LDA) calculations is observed around the Z point. The disappearance of intensity of the &alpha;<super>&lsquo;</super> band near E_F at k_z = &pi;/2 suggests that the &alpha;<super>&lsquo;</super> band could either sink below E_F or be degenerate with the inner hole (&alpha;) band. The studies on the &alpha;<super>&lsquo;</super> band in the superconducting state reveal a nearly isotropic superconducting gap on this FS sheet. Underdoped samples Ba_0.75K_0.25Fe₂As₂ are used to study how the AF fluctuations and superconductivity interplay in the underdoped regime that is closer to the AF phase. we observe that the superconducting gap of the underdoped pnictides scales linearly with T_c. A distinct pseudogap develops upon underdoping and coexists with the superconducting gap. Remarkably, this pseudogap occurs mainly on the FS sheets that are connected by the AF wave vector, where the superconducting pairing is stronger as well. This suggests that both the pseudogap and the superconducting gap are driven by the AF fluctuations, and the long-range AF ordering competes with the superconductivity. The observed dichotomic behaviour of the pseudogap and the SC gap on different FS sheets in the underdoped pnictides shares similarities with those observed in the underdoped copper oxide superconductors, providing a possible unifying picture for both families of high-temperature superconductors. / Thesis (PhD) — Boston College, 2010. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.

In this dissertation, the studies aim to characterize the electronic structure at the internal interface of hybrid materials. The characterization challenge is originating from the spectral superposition of hybrid constituents. A characterization protocol based on photoemission spectroscopy (PES) was developed and applied to investigate the orbital alignment at the internal interface of the oligothiophene-TiO2 and ArS-CdSe hybrid materials by characterizing the individual constituents and the assembly hybrids respectively. Electrospray deposition technique was used to deposit targeting materials which enabled preparation of thin films in vacuum minimizing ambient contaminations while transmission electron microscopy (TEM) was used to investigate the morphology and the particle size of the pure nanoparticles and the hybrids. Ultraviolet-visible (UV-vis) spectroscopy was also used in the estimation of the optical band gap of the pure nanoparticles and the HOMO-LUMO gap of the organic ligands. One of the hybrid materials studied in this dissertation is oligothiophene-TiO2 nanoparticle hybrids in which the oligothiophene ligands are bonded to the surface of TiO2 nanoparticles covalently. This hybrid system was used to develop and demonstrate a measurement protocol to characterize the orbital alignment at the internal interface. Low intensity X-ray photoemission spectroscopy (LIXPS) was used to determine the work function of the oligothiophene ligands and the TiO2 nanoparticles. In combination with the highest occupied molecular orbital (HOMO) cutoff and the valence band maximum (VBM) measured by ultraviolet photoemission spectroscopy (UPS), the ionization energies (IE) of these two constituents were determined. X-ray photoemission spectroscopy (XPS) was used to characterize the core level emissions of the constituents and the hybrid assembly, which were used to determine the charge injection barriers at the internal interface. The results showed that there was an interface dipole at the internal interface between organic and inorganic constituents of the hybrid. The dipole was determined to be 0.61 eV and the hole injection barrier at the internal interface amounted to 0.73 eV. The electron injection barrier was estimated by taking into account the gap between highest occupied and lowest unoccupied molecular orbitals (HOMO, LUMO). The procedure followed only suggested the presence of an insignificant barrier in the oligothiophene-TiO2 nanoparticle hybrids. Arylthiol functionalized Cadmium Selenide (ArS-CdSe) is a novel hybrid material which can be used in hetero-junction solar cells. The ArSH ligands are bonded on the surface of the CdSe nanoparticles covalently through sulfur atoms serving as anchors. The internal interface in the ArS-CdSe hybrids between the organic constituent and the inorganic constituent was studied by the same characterization protocol developed in this dissertation. Furthermore, a physisorbed interface between the ArSH ligands and the CdSe nanoparticles was created through multi-step in-vacuum deposition procedure. The electrospray deposition technique enabled the formation of a well-defined physisorbed interface which was characterized by LIXPS, UPS and XPS for each deposition step. Accordingly, the orbital alignment at the physisorbed interface was determined. Based on the results obtained, detailed orbital alignments at the ArSH/CdSe physisorbed interface and the internal interface in the ArS-CdSe hybrid materials were delineated and discussed. The hole injection and electron injection barrier at the physisorbed ArSH/CdSe interface are 0.7 eV and 1.0 eV respectively. An interface dipole of 0.4 eV was observed at the interface. In the ArS-CdSe hybrid materials, the electronic system of the ArSH component shifts down due to the charge transfer induced by the covalent hybridization. The hybridization also shifts the electronic system of the CdSe constituent to a lower energy level due to saturation of the unoccupied bonds of the Cd atoms on the surface. The hole injection barrier and electron injection barrier were determined to be 0.5 eV and 1.2 eV respectively. A small interface dipole (0.2 eV) was observed at the internal interface as a result of the presence of covalent bonds.