Diese Dissertation unter dem Titel Experimentelle Bestimmung der elektronischen Eigenschaften anwendungsrelevanter Grenzflächen organischer Halbleiter mittels Photoelektronenspektroskopie wurde am Leibniz Institut für Festkürper- und Werkstoffforschung (IFW) Dresden am Institut für Festkörperforschung (IFF) unter der Betreuung von Prof. Dr. B. Büchner angefertigt. Zur wissenschaftlichen Untersuchung kamen hierbei zwei Typen anwendungsrelevanter Grenzflächen. Zum einem wurde der Einfluss einer Elektrodenpräparation unter Normalbedingungen mittels ex-situ Reinigungsverfahren im Vergleich zu insitu präparierten Kontakten auf das elektronische Verhalten des organischen Halbleiters Sexithiophen an Grenzflächen zu metallischen Substraten studiert. Als Substratmaterialien kamen hierbei die Metalle Silber, Palladium, Gold und Platin zum Einsatz. In einer zweiten Studie wurden die Grenzflächen der organischen Halbleiter Sexithiophen und Kupfer(II)- Phthalocyanin in Kontakt zu dünnen Filmen des Übergangsmetalloxides La0.7Sr0.3MnO3 untersucht. Auch hier wurde eine vergleichende Untersuchung für ex-situ und in-situ gereinigte La0.7Sr0.3MnO3-Kontakte durchgeführt. Die hierzu verwendeten Filme wurden im IFW Dresden am Institut für Metallische Werkstoffe (IMW) hergestellt. Auch im Rahmen dieser Untersuchungen stand der Einfluss von Sauerstoff auf das elektronische und chemische Verhalten an den Grenzflächen im Vordergrund.

The present research work focuses on the fabrication and characterization of epitaxial heterostructures of 0.7 Pb(Mg1/3N2/3)O3 – 0.3 PbTiO3 (PMN-PT) and La0.6Sr0.4MnO3 (LSMO) using multi target pulsed laser ablation technique. Different heterostructures such as bilayered thin films with different individual layer thickness; symmetric and asymmetric superlattices of different periodicities were fabricated. Roles of individual layer thickness, elastic strain and interfaces between PMN-PT and LSMO layers on different physical properties were studied. An attempt has been made to understand the influence of the charge depleted interface states in addition to the probable strain mediated elastic coupling effect on the observed magneto-dielectric response in these engineered heterostructures. Chapter 1 provides a brief introduction to the multiferroic materials, occurrence of magnetoelectric (ME) coupling in them, their possible technological applications and the challenges involved. A short historical account of the multiferroic research is discussed to emphasize the importance of artificial multiferroics, particularly the engineered thin film heterostructures. Finally the specific objectives of the current research are outlined. Chapter 2 deals with the various experimental studies carried out in this research work. It gives the details of the experimental set up and the basic operation principles of various structural and physical characterizations of the materials prepared. A brief explanation of material fabrication, structural, micro structural and physical property measurements is discussed. Chapter 3 addresses the phase formation, structural and microstructural features of the engineered heterostructures fabricated epitaxially on single crystalline LaAlO3 (100) substrates. A thin layer of LaNiO3 used as the bottom electrode material for electrical characterizations was grown on the bare substrate prior to the fabrication of the PMN-PT/LSMO heterostructures. The structural and microstructural features of different individual layers were also studied by fabricating single layer thin films of the materials. The effects of individual layer thicknesses on the surface roughness, grain size and lattice strain of the heterostructures are discussed. Chapter 4 deals with the ferroelectric studies of the PMN-PT/LSMO epitaxial heterostructures. Polarization hysteresis (P-E), capacitance – voltage (C-V) and pulsed polarization (PUND) measurements were carried out as functions of applied voltage, frequency and delay time to characterize the ferroelectric properties of the heterostructures. All the bilayered heterostructures exhibited robust ferroelectric response and contribution of non – remnant components to their polarization behaviour were observed from the P-E studies. The symmetric superlattices did not exhibit any ferroelectricity due to high leakage current conduction. After optimizing the LSMO and PMN-PT layer thicknesses ferroelectricity was observed in the asymmetric superlattices accompanied by substantial reduction in the leakage current conduction. The P-E loops were found to be asymmetrically shifted along the electric field axis in all the superlattices indicating the presence of dielectric passive layers and strong depolarizing fields at the interfaces between PMN-PT and LSMO. Chapter 5 deals with the ferromagnetic studies of the PMN-PT/LSMO heterostructures. All the heterostructures exhibited ferromagnetic behaviour in the temperature range of 10 K – 300 K with an in plane magnetic easy axis ([100]) compared to the out of plane ([001]) direction. The magnetization behaviour of the bilayers and superlattices as a function of magnetic field strength, temperature and different individual layer thickness of PMN-PT and LSMO are discussed in terms of the oxygen deficiency, magnetic dead layers and lattice strain effects in these engineered epitaxial heterostructures. Chapter 6 addresses the magneto-dielectric response, dielectric properties and ac conduction properties of the engineered biferroic heterostructures. In order to investigate the manifestation of strain mediated ME coupling in these heterostructures their dielectric response as a function of ac electric signal frequency have been studied under different static magnetic fields over a wide range of temperatures. The appearance of magneto-capacitance and its dependence on magnetic field strength and temperature along with the magnetoresistive characteristics of the heterostructures suggested that the charge depleted interfaces between PMN-PT and LSMO can have an effect on the observed dielectric response in addition to the probable strain mediated ME coupling. Dielectric characterization of the heterostructures performed over a wide range of temperature indicated a Maxwell-Wagner type relaxation mechanism. The manifestation of Maxwell-Wagner effect and the very low activation energy of ac conductivity obtained from the ac conduction studies revealed the strong influence of the charge depleted interfaces between PMN-PT and LSMO on the dielectric properties of the heterostructures. Chapter 7 deals with the dc leakage current conduction characteristics of the heterostructures. The leakage current characterization was performed over a wide range of temperature and analyzed in the framework of different models to investigate the leakage mechanism. All the heterostructures were found to obey the power law I∝Vα over the entire range of temperature with different values of α at different applied voltages. The bilayered heterostructures exhibited ohmic conduction in the lower electric field region and space charge limited conduction was observed at higher electric fields. On the other hand the low field dc conduction behaviour of the superlattices could not be attributed unambiguously to a single mechanism. Depending on the superlattice periodicity the low field conduction behaviour was dominated by either Poole-Frenkel (PF) emission or a combined contribution from the PF effect and ohmic conduction. At higher electric fields all the superlattices exhibited space charge limited conduction. Chapter 8 gives the summary and conclusions of the present study and also discusses about the future work that could give more insight into the understanding of the engineered epitaxial biferroic heterostructures.

Two groups of magnetic oxides were investigated in this thesis. Thin films of La2/3Sr1/3MnO3 (LSMO) deposited by pulsed laser deposition (PLD) on SrTiO3 (STO) substrates were characterized by polar and longitudinal magneto-optical (MO) Kerr spectroscopy. Experimental results were compared to theoretical calculations based on the transfer matrix formalism. A very good agreement between experimental and theoretical data revealed high magnetic ordering down to 5 nm of film thickness as well as a mechanism of suppression of double exchange interaction near the LSMO/STO interface. Magnetically doped Ce1-xCoxO2-δ films deposited by PLD on MgO (x = 0.05 and 0.10) and oxidized Si (x = 0.20) substrates were studied by combination of spectroscopic ellipsometry and MO Faraday and Kerr spectroscopy. Both diagonal and off-diagonal permittivity tensor components were obtained and verified by theoretical calculations confronted with experimental data. Diagonal spectra revealed two optical transitions from oxygen to cerium states. Off-diagonal spectra revealed two paramagnetic transitions involving cobalt ions. An essential influence of cobalt doping on the resulting ferromagnetic properties of CeO2 was observed.

Diese Dissertation unter dem Titel Experimentelle Bestimmung der elektronischen Eigenschaften anwendungsrelevanter Grenzflächen organischer Halbleiter mittels Photoelektronenspektroskopie wurde am Leibniz Institut für Festkürper- und Werkstoffforschung (IFW) Dresden am Institut für Festkörperforschung (IFF) unter der Betreuung von Prof. Dr. B. Büchner angefertigt. Zur wissenschaftlichen Untersuchung kamen hierbei zwei Typen anwendungsrelevanter Grenzflächen. Zum einem wurde der Einfluss einer Elektrodenpräparation unter Normalbedingungen mittels ex-situ Reinigungsverfahren im Vergleich zu insitu präparierten Kontakten auf das elektronische Verhalten des organischen Halbleiters Sexithiophen an Grenzflächen zu metallischen Substraten studiert. Als Substratmaterialien kamen hierbei die Metalle Silber, Palladium, Gold und Platin zum Einsatz. In einer zweiten Studie wurden die Grenzflächen der organischen Halbleiter Sexithiophen und Kupfer(II)- Phthalocyanin in Kontakt zu dünnen Filmen des Übergangsmetalloxides La0.7Sr0.3MnO3 untersucht. Auch hier wurde eine vergleichende Untersuchung für ex-situ und in-situ gereinigte La0.7Sr0.3MnO3-Kontakte durchgeführt. Die hierzu verwendeten Filme wurden im IFW Dresden am Institut für Metallische Werkstoffe (IMW) hergestellt. Auch im Rahmen dieser Untersuchungen stand der Einfluss von Sauerstoff auf das elektronische und chemische Verhalten an den Grenzflächen im Vordergrund.

No description available.

Les systèmes d’information actuels reposent fortement sur les technologies micro-ondes utilisées pour les communications hertziennes. L’amélioration des performances des MEMS radio fréquence aptes à fonctionner dans la bande X (8 GHz et 12 GHz) est un enjeu important pour des applications de télécommunications mais aussi pour les applications radar. Pour y parvenir l’intégration de matériaux ferroélectriques à haute constante diélectrique est requise. Les matériaux qui possèdent de telles propriétés et qui sont les plus adaptés, sont les composés qui dérivent de la structure pérovskite. Intégrer ce type de matériaux dans des commutateurs radio-fréquence (MEMS-RF) pose de nouveaux chalenges en termes de maîtrise du matériau et de compatibilité avec les technologies MEMS existantes. Cette thèse s’est portée sur le composé PMN-PT avec la composition 65/35 qui possède une permittivité relative supérieure à 10000 sous forme de matériau massif.Ce travail de thèse a été consacré à l’étude de l’intégration du composé PMN-PT dans des composants passifs que sont les commutateurs MEMS. Dans la gamme de fréquence d’intérêt, de 500 MHz jusqu’à 20 GHz, les propriétés de ces matériaux ont été peu étudiées sur les matériaux massifs et encore moins sous forme de films minces. L’objectif de cette thèse était de réaliser les couches minces ferroélectriques et de tester leur compatibilité dans l’ensemble du fonctionnement d’un composant MEMS mais aussi de mener une étude réciproque : l’analyse des FeMEMS (MEMS basé sur les ferroélectriques) permettant de compléter les connaissances de ces matériaux dans cette gamme de fréquence. Ce travail est d’intérêt pour l’industrie de la technologie MEMS mais aussi pour la science des matériaux ferroélectriques mais aussi par la compréhension des mécanismes physiques gouvernant aux propriétés diélectriques en termes de pertes notamment dans ce domaine de fréquences.Les caractérisations des MEMS-RF présentées dans cette thèse ont démontré la compatibilité du MEMS PMN-PT dans la gamme de fréquence entre 500MHz et 10 GHz avec de très bonnes performances. En utilisant cette adaptation, la technologie actuelle est ainsi capable de couvrir tous les bandes de fréquence les plus importantes : la bande de télécommunication civile de 1 GHz à 5 GHz en utilisant le PMN-PT, la bande X pour les satellites entre 5 GHz et 15 GHz avec PZT et la bande de haute fréquence de 15 GHz à 40 GHz pour la défense avec les diélectriques traditionnels (Si3N4). / The current information systems depend strongly on the microwave technology used for wireless communications. The enhanced performance of MEMS radio frequency capacity in X-band (8 GHz and 12 GHz) is an important issue not only for Telecom applications but also for Radar applications. The integration of ferroelectric materials with high-k t is highly demanded to replace the traditional dielectrics. This high-k property is accessible for compounds derived from the perovskite structure. Incorporating such materials in switches radio-frequency (RF-MEMS) impose however new chalenges in terms of the compatibility with the existing MEMS technologies. This thesis is focused on the compound PMN-PT with composition 65/35, which has a relative permittivity greater than 10,000 in the form of bulk material.This thesis has been devoted to the study of the integration of PMN-PT thin films in passive components such as MEMS switches. In the frequency range of interest, 500 MHz to 20 GHz, the properties of these materials have not been studied in bulk materials and even less in the form of thin films. The aim of this thesis was to fabricate the ferroelectric thin films and test their compatibility in the overall operation of a MEMS component. This study provides a reciprocal analysis FeMEMS (MEMS based on ferroelectrics) to complete knowledge of these materials in this frequency range. This work makes interest to both the industry and MEMS ferroelectric materials science who is trying to understand the physical mechanisms governing the dielectric properties in terms of losses in this particular range of frequencies.The characterizations of RF-MEMS presented in this thesis have demonstrated the compatibility of MEMS PMN-PT in the frequency range between 500MHz to 10 GHz with very good performance. Using this adaptation, the current technology is able to cover the most important frequency bands: the civil band telecommunication 1 GHz to 5 GHz using the PMN-PT, the X-band satellites between 5 GHz and 15 GHz with PZT and high frequency band of 15 GHz to 40 GHz for the defense with traditional dielectric (Si3N4).

No description available.

Les systèmes d'information actuels reposent fortement sur les technologies micro-ondes utilisées pour les communications hertziennes. L'amélioration des performances des MEMS radio fréquence aptes à fonctionner dans la bande X (8 GHz et 12 GHz) est un enjeu important pour des applications de télécommunications mais aussi pour les applications radar. Pour y parvenir l'intégration de matériaux ferroélectriques à haute constante diélectrique est requise. Les matériaux qui possèdent de telles propriétés et qui sont les plus adaptés, sont les composés qui dérivent de la structure pérovskite. Intégrer ce type de matériaux dans des commutateurs radio-fréquence (MEMS-RF) pose de nouveaux chalenges en termes de maîtrise du matériau et de compatibilité avec les technologies MEMS existantes. Cette thèse s'est portée sur le composé PMN-PT avec la composition 65/35 qui possède une permittivité relative supérieure à 10000 sous forme de matériau massif.Ce travail de thèse a été consacré à l'étude de l'intégration du composé PMN-PT dans des composants passifs que sont les commutateurs MEMS. Dans la gamme de fréquence d'intérêt, de 500 MHz jusqu'à 20 GHz, les propriétés de ces matériaux ont été peu étudiées sur les matériaux massifs et encore moins sous forme de films minces. L'objectif de cette thèse était de réaliser les couches minces ferroélectriques et de tester leur compatibilité dans l'ensemble du fonctionnement d'un composant MEMS mais aussi de mener une étude réciproque : l'analyse des FeMEMS (MEMS basé sur les ferroélectriques) permettant de compléter les connaissances de ces matériaux dans cette gamme de fréquence. Ce travail est d'intérêt pour l'industrie de la technologie MEMS mais aussi pour la science des matériaux ferroélectriques mais aussi par la compréhension des mécanismes physiques gouvernant aux propriétés diélectriques en termes de pertes notamment dans ce domaine de fréquences.Les caractérisations des MEMS-RF présentées dans cette thèse ont démontré la compatibilité du MEMS PMN-PT dans la gamme de fréquence entre 500MHz et 10 GHz avec de très bonnes performances. En utilisant cette adaptation, la technologie actuelle est ainsi capable de couvrir tous les bandes de fréquence les plus importantes : la bande de télécommunication civile de 1 GHz à 5 GHz en utilisant le PMN-PT, la bande X pour les satellites entre 5 GHz et 15 GHz avec PZT et la bande de haute fréquence de 15 GHz à 40 GHz pour la défense avec les diélectriques traditionnels (Si3N4).

Multiferroic materials exhibit unique properties such as simultaneous existence of two or more of coupled ferroic order parameters (ferromagnetism, ferroelectricity, ferroelasticity or their anti-ferroic counterparts) in a single material. Recent years have seen a huge research interest in multiferroic materials for their potential application as high density non-volatile memory devices. However, the scarcity of these materials in single phase and the weak coupling of their ferroic components have directed the research towards multiferroic heterostructures. These systems operate by coupling the magnetic and electric properties of two materials, generally a ferromagnetic material and a ferroelectric material via strain. In this work, horizontal heterostructures of composite multiferroic materials were grown and characterized using pulsed laser ablation technique. Alternate magnetic and ferroelectric layers of cobalt ferrite and lead zirconium titanate, respectively, were fabricated and the coupling effect was studied by X-ray stress analysis. It was observed that the interfacial stress played an important role in the coupling effect between the phases. Doped zinc oxide (ZnO) heterostructures were also studied where the ferromagnetic phase was a layer of manganese doped ZnO and the ferroelectric phase was a layer of vanadium doped ZnO. For the first time, a clear evidence of possible room temperature magneto-elastic coupling was observed in these heterostructures. This work provides new insight into the stress mediated coupling mechanisms in composite multiferroics.

The electronic and magnetic structure of the colossal magneto resistance material La1-xSrxMnO3, the high-k and strain tailoring compounds REScO3 (Sm, Gd, Dy) and the multiferroic LuFe2O4 was investigated by means of x-ray spectroscopic techniques. SQUID measurements of La1-xSrxMnO3 (x = 0.125, 0.17, 0.36) were compared with XMCD results. The very good agreement between these two experiments proofs the applicability of the correction factor for the spin magnetic moment and the importance of charge transfer. The magnetic moment measured by SQUID and that determined from XMCD proofs that the magnetic moment is completely localized at the Mn ions for different temperatures and magnetic fields. For x = 0.125 the orbital magnetic moment determined from XMCD corresponds to the structural changes in the phase diagram. Additionally the measured orbital moments correspond to anomalies in magnetization versus temperature curves. The magnetic and electronic structure of the rare earth scandates (SmScO3, GdScO3 and DyScO3) were investigated by means of XPS, XES, XAS, SQUID and neutron powder diffraction. The magnetic measurements reveal antiferromagnetic coupling at low temperatures in agreement with neutron diffraction data. With XAS and XES at the O K-edge in comparison with band structure calculations of the unoccupied oxygen states, the band gaps of REScO3 were determined and it was found that these values are corresponding to the Sc-O mean distances. The electronic and magnetic structure of LuFe2O4 was presented. The valence state of Fe ions was determined to 50% divalent and 50% trivalent by XPS of Fe 2p and 3s levels. The big orbital magnetic moment found by XMCD could explain a discrepancy between the magnetic measurements and the spin configuration, which was confirmed by XMCD.