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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

Theory of Spectral Function and Optical Conductivity for Half-Metallic Double Perovskites

Janczak, Julia 20 December 2012 (has links)
No description available.
2

Terahertz Dynamics of Quantum-Confined Electrons in Carbon Nanomaterials

January 2012 (has links)
The terahertz (THz) frequency range. 0.1 - 20 THz, exists between the microwave and infrared ranges and contains abundant information on the dynamics of charge and spin carriers in condensed matter systems. Since its advent two decades ago, THz spectroscopy has been extensively used to study a wide range of solid state materials, including typical semiconductors, conducting polymers, insulators, superconductors, and artificially grown structures such as quantum wells. In these systems, electronic and photonic events tend to occur on the time scale of tens to hundreds of femtoseconds, which results in many important excitations, resonances and dynamical phenomena in the THz frequency range. In this dissertation work, we have developed a typical THz time-domain spectroscopy (TDS) system to investigate the THz dynamics of quantum-confined electrons in two important types of carbon nanomaterial: single-walled carbon nanotubes (SWNTs) and graphene. Polarization dependent THz transmission measurements were conducted on a highly-aligned SWNT film on a sapphire substrate, revealing extremely high anisotropy: virtually no attenuation was observed when the polarization of the THz beam was perpendicular to the nanotube axis, while the THz beam was strongly absorbed when its polarization was parallel to the tube axis. From the measured absorption anisotropy, we calculated the reduced linear dichrosim to be 3, corresponding to a nematic order parameter of 1. These observations are a direct result of the one-dimensional nature of conduction electrons in the nanotubes and at the same time, demonstrate that any misalignment of nanotubes in the film mast have characteristic length scales much smaller than the wavelengths used in these experiments (1.5 mm - 150 μm). Based on this work, an ideal THz linear polarizer built with parallel stacks of such aligned SWNT films was synthesized, exhibiting a degree of polarization of 99.9% throughout the frequency range 0.2 - 2.2 THz and a high extinction ratio of 10 -3 (or 30 dB). The THz complex conductivity of the thin SWNT film was extracted through a proper model directly from the TDS data without Kramers-Kronig analysis. Both real and imaginary parts of the conductivity showed a non-Drude frequency dependence, indicating the presence of plasmon-dipole resonance at higher frequencies. Finally, the optical conductivity of large-area. graphene grown from solid state carbon source was studied in a wide spectral range (7 cm -1 - 9500 cm -1 ) using THz-TDS and Fourier transform infrared spectroscopy. We observed that the Fermi level E f of graphene could be tuned by both electrical gating and thermal annealing. The optical conductivity measured at different carrier concentrations exhibited Drude-like frequency dependence, and different 2 E f onsets in the spectrum were probed as well.
3

Graphene Casimir Interactions and Some Possible Applications

Phan, Anh Duc 01 January 2012 (has links)
Scientific development requires profound understandings of micromechanical and nanomechanical systems (MEMS/NEMS) due to their applications not only in the technological world, but also for scientific understanding. At the micro- or nano-scale, when two objects are brought close together, the existence of stiction or adhesion is inevitable and plays an important role in the behavior operation of these systems. Such effects are due to surface dispersion forces, such as the van der Waals or Casimir interactions. The scientific understanding of these forces is particularly important for low-dimensional materials. In addition, the discovery of materials, such as graphitic systems has provided opportunities for new classes of devices and challenging fundermental problems. Therefore, invesigations of the van der Waals or Caismir forces in graphene-based systems, in particular, and the solution generating non-touching systems are needed. In this study, the Casimir force involving 2D graphene is investigated under various conditions. The Casimir interaction is usually studied in the framework of the Lifshitz theory. According to this theory, it is essential to know the frequency-dependent reflection coefficients of materials. Here, it is found that the graphene reflection coefficients strongly depend on the optical conductivity of graphene, which is described by the Kubo formalism. When objects are placed in vacuum, the Casimir force is attractive and leads to adhesion on the surface. We find that the Casimir repulsion can be obtained by replacing vacuum with a suitable liquid. Our studies show that bromobenzene is the liquid providing this effect. We also find that this long-range force is temperature dependent and graphene/bromobenzene/metal substrate configuration can be used to demonstrate merely thermal Casimir interaction at room temperature and micrometer distances. These findings would provide good guidance and predictions for practical studies.
4

Pr$_{1-x}$Ca$_x$MnO$_x$ for Catalytic Water Splitting - Optical Properties and In Situ ETEM Investigations

Mildner, Stephanie 05 August 2015 (has links)
Gegenstand der vorliegenden Dissertation ist die Untersuchung von Ca-dotierten PrMnO3 (PCMO) als Katalysator für die (photo)elektrochemische Wasseroxidation. Im Fokus der Untersuchungen stehen die folgenden elementaren Schritte des Gesamtprozesses: i) Die optische Absorption in PCMO wird zunächst als Funktion der Ca-Dotierung und der Temperatur untersucht mit dem Ziel, den Einfluß von Korrelationseffekten auf die optischen Eigenschaften zu verstehen. Die präsentierten Ergebnisse zeigen, dass die Bildung kleiner Polaronen im PCMO als Folge starker Korrelationswechselwirkungen in breites Absorptionsmaximum im Nah-Infrarot bis sichtbarem Energiebereich verursacht, welches im Rahmen eines Photonen-assistierten Polaronenhüpfprozesses und einer Anregung zwischen Jahn-Teller-aufgespaltenen Zuständen diskutiert wird. Weiterhin legt die Dotierungsabhängigkeit der Spektren nahe, dass O 2p und Mn 3d Hybridzustände die Fermienergie-nahe elektronische Struktur bestimmen, wobei der relative Anteil von O 2p mit der Ca-Dotierung variiert. ii) Der aktive Zustand von PCMO in Kontakt mit Wasser bzw. Wasserdampf wird mit Hilfe von Zyklovoltammetrie und in situ ‚environmental‘ Transmissionselektronenmikroskopie (ETEM) für verschiedene Dotierlevels untersucht. Die Ergebnisse beider Methoden ergeben, dass die katalysierte Wasseroxidation gemäß $2\text{H}_2\text{O} \rightarrow \text{O}_2 + 4 \text{H}^+$ mit einem Korrosionsprozess in Form einer Pr/Ca Verarmung und Amorphisierung der PCMO-Elektrode konkurriert. Die höchste katalytische Aktivität sowie Korrosionsstabilität werden im mittleren Dotierungsbereich gefunden. Auf Basis der in situ ETEM Ergebnisse wird außerdem gezeigt, dass durch Zufügen von Monosilan zu Wasserdampf-basierten Elektrolyten im ETEM eine Elektronenstrahl-induzierte Wasseroxidation an aktiven PCMO Oberflächen über die Sekundärreaktion $\text{SiH}_4+2\text{O}_2\rightarrow\text{SiO}_2+2\text{H}_2\text{O}$ nachgewiesen werden kann. Elektronenenergieverlustspektroskopie von PCMO vor und nach der Reaktion in Wasserdampf ergeben, dass der aktive Zustand von PCMO die Bildung und Ausheilung von Sauerstoffleerstellen im Rahmen einer Interkalation des bei der Wasseroxidation freiwerdenden Sauerstoffs beinhaltet. Die Rolle des Elektronenstrahls als Triebkraft für die Wasseroxidation im ETEM wird mithilfe von Elektronenholographie und elektrischen Experimenten sowie theoretischer Modellierung basierend auf Sekundärelektronenemissionen als ein positives Elektronenstrahl-induziertes elektrisches Potential identifiziert.
5

Optinio ZnMgRE kvazikristalų atsako tyrimai / Optical Response of ZnMgRE Quasicrystals

Tumėnas, Saulius 30 September 2013 (has links)
Pagrindinis disertacijos tikslas – optinio ZnMgRE (RE = Y, Ho, Er) kvazikristalų atsako tyrimais atskleisti jų elektroninės posistemės ypatumus. Disertaciją sudaro eksperimentiniai rentgeno-difrakciniai (XRD) ir optiniai spektroskopiniai tyrimai, kvazikristalų elektroninės posistemės modelio konstravimas ir teorinis jų optinio atsako aprašymas. Atliktais eksperimentiniais XRD tyrimais buvo siekiama atskleisti kvazikristalų atvirkštinės gardelės vektorius, apibrėžiančius potencinį kvazikristalinį lauką, veikiantį į elektroninę posistemę. Optiniai spektroskopiniai tyrimai buvo atlikti kombinuotu spektroskopinės elipsometrijos ir atspindžio spektroskopijos metodu, paremtu darbe pasiūlyta inkaro lango duomenų analizės schema. Naudotas spektroskopinių tyrimų metodas įgalino atskleisti patikimus ZnMgRE optinio laidumo spektrus plačioje, 0.01 – 6 eV, spektrinėje srityje. Darbe išplėstas ZnMgRE elektronų posistemės modelis, kuris anksčiau buvo pasiūlytas kvazikristalų fotoemisinio atsako analizei. Nepriklausomų Fermi paviršiaus sankirtų su Bragg’ų plokštumomis schema formuluota išplėstiniame juostiniame atvaizdavime. Teorinė optinio laidumo skaičiavimų schema, anksčiau pasiūlyta kristalinių junginių optinio laidumo skaičiavimams, šiame darbe išplėsta įskaitant įvairias Fermi lygmens padėtis pseudotarpo atžvilgiu. Teoriniai ZnMgRE optinio laidumo skaičiavimai, atlikti darbe pasiūlyto elektroninės posistemės modelio rėmuose, detaliai atkartoja eksperimentinius optinio laidumo spektrus... [toliau žr. visą tekstą] / The main goal of the dissertation was to reveal the electronic structure of ZnMgRE (RE = Y, Ho, Er) quasicrystals by investigations of their optical response. The thesis comprises experimental X-ray diffraction (XRD) and optical spectroscopy studies of the quasicrystals, a construction of their electron subsystem model, and a theoretical description of their optical response. The XRD studies were carried out to determine the reciprocal quasicrystalline lattice vectors, which define the atomic potential field acting on an electron subsystem. The optical spectroscopy studies were carried out by the combined spectroscopic ellipsometry and reflectance spectroscopy technique, based on a suggested anchor-window method. High-accuracy ZnMgRE optical conductivity spectra were recorded in the wide, 0.01 – 6 eV, spectral range. The model of ZnMgRE electron energy spectrum, previously suggested for an interpretation of experimental ZnMgRE photoemission spectra, was developed. The nearly-free-electron gas model of independent intersections was formulated in the extended zone presentation. A scheme of the theoretical optical conductivity calculations was extended to account for various positions of the Fermi level with respect to a pseudogap. The experimental ZnMgRE optical conductivity spectra can be reproduced in detail by theoretical calculations performed within the framework of the suggested electron energy spectrum model. The set of the electron energy spectrum parameters determined... [to full text]
6

Optical Response of ZnMgRE Quasicrystals / Optinio ZnMgRE kvazikristalų atsako tyrimai

Tumėnas, Saulius 30 September 2013 (has links)
The main goal of the dissertation was to reveal the electronic structure of ZnMgRE (RE = Y, Ho, Er) quasicrystals by investigations of their optical response. The thesis comprises experimental X-ray diffraction (XRD) and optical spectroscopy studies of the quasicrystals, a construction of their electron subsystem model, and a theoretical description of their optical response. The XRD studies were carried out to determine the reciprocal quasicrystalline lattice vectors, which define the atomic potential field acting on an electron subsystem. The optical spectroscopy studies were carried out by the combined spectroscopic ellipsometry and reflectance spectroscopy technique, based on a suggested anchor-window method. High-accuracy ZnMgRE optical conductivity spectra were recorded in the wide, 0.01 – 6 eV, spectral range. The model of ZnMgRE electron energy spectrum, previously suggested for an interpretation of experimental ZnMgRE photoemission spectra, was developed. The nearly-free-electron gas model of independent intersections was formulated in the extended zone presentation. A scheme of the theoretical optical conductivity calculations was extended to account for various positions of the Fermi level with respect to a pseudogap. The experimental ZnMgRE optical conductivity spectra can be reproduced in detail by theoretical calculations performed within the framework of the suggested electron energy spectrum model. The set of the electron energy spectrum parameters determined... [to full text] / Pagrindinis disertacijos tikslas – optinio ZnMgRE (RE = Y, Ho, Er) kvazikristalų atsako tyrimais atskleisti jų elektroninės posistemės ypatumus. Disertaciją sudaro eksperimentiniai rentgeno-difrakciniai (XRD) ir optiniai spektroskopiniai tyrimai, kvazikristalų elektroninės posistemės modelio konstravimas ir teorinis jų optinio atsako aprašymas. Atliktais eksperimentiniais XRD tyrimais buvo siekiama atskleisti kvazikristalų atvirkštinės gardelės vektorius, apibrėžiančius potencinį kvazikristalinį lauką, veikiantį į elektroninę posistemę. Optiniai spektroskopiniai tyrimai buvo atlikti kombinuotu spektroskopinės elipsometrijos ir atspindžio spektroskopijos metodu, paremtu darbe pasiūlyta inkaro lango duomenų analizės schema. Naudotas spektroskopinių tyrimų metodas įgalino atskleisti patikimus ZnMgRE optinio laidumo spektrus plačioje, 0.01 – 6 eV, spektrinėje srityje. Darbe išplėstas ZnMgRE elektronų posistemės modelis, kuris anksčiau buvo pasiūlytas kvazikristalų fotoemisinio atsako analizei. Nepriklausomų Fermi paviršiaus sankirtų su Bragg’ų plokštumomis schema formuluota išplėstiniame juostiniame atvaizdavime. Teorinė optinio laidumo skaičiavimų schema, anksčiau pasiūlyta kristalinių junginių optinio laidumo skaičiavimams, šiame darbe išplėsta įskaitant įvairias Fermi lygmens padėtis pseudotarpo atžvilgiu. Teoriniai ZnMgRE optinio laidumo skaičiavimai, atlikti darbe pasiūlyto elektroninės posistemės modelio rėmuose, detaliai atkartoja eksperimentinius optinio laidumo spektrus... [toliau žr. visą tekstą]
7

Optical Study of Inter-band Transitions in Topological Insulators Bi2Se3, Bi2Te3, and Sb2Te3

Adhikari, Pan P. January 2017 (has links)
No description available.
8

Spectral And Transport Properties Of Falicov-Kimball Related Models And Their Application To Manganites

Pakhira, Nandan 04 1900 (has links)
From the time of the unexpected discovery of the insulating nature of NiO by Verwey half a century ago, Oxide materials have continued to occupy the centre stage of condensed matter physics. The recent discovery of high temperature superconductivity in doped cuprates has given a new impetus to the study of the strongly correlated electron systems. Besides, the occurrence of Colossal Magneto-Resistance (CMR) in doped rare earth manganite has also created renewed interest in these rather old systems. Understanding of the rich and complex phase diagram of these materials and their sensitivity to small perturbations e.g. external magnetic field of a few Tesla, temperature, change in isotope etc. are of great theoretical interest and also these materials have many potential technological applications. A common feature of all these oxide materials is that the transition metal ions have partially filled d-shells. Unlike s and p-electrons which gives rise to hybridized Bloch states, the d-electrons retain their atomic nature in a solid. This gives rise to strong Coulomb interaction among d-electrons which may be comparable or more than its kinetic energy. The strong correlation effects are evident from the experimental fact that the undoped parent compounds are insulators rather than metals as suggested by band theory, which favours a metallic state for systems with one electron per unit cell since this gives rise to partially filled bands (and hence a metallic state). These insulators termed Mott insulators, arise solely due to strong electron-electron correlations as compared to the band insulators which arise due to complete filling of one electron bands thereby giving rise to a gap (band gap)in the excitation spectra. The delicate competition between the kinetic energy and the Coulomb energy for d-electrons is broadly responsible for the wide variety of phenomena like Mott metal-insulator transition (MIT), magnetic transitions, charge ordering, orbital ordering, ferro/antiferroelectricity, and most interestingly the observation of high Tc superconductivity in doped cuprates. In this thesis we will restrict our interest to one such class of oxide materials, namely the doped rare earth manganites. In Chapter 1 we give a brief overview of the structure and basic interactions present in the doped manganites. Also, in the same Chapter we give a brief introduction to the phenomenology of manganites, particularly its phase diagram in the doping and temperature plane and various experimental features, e.g. the wide variety of phase transitions and phenomena particularly the observation of CMR, charge ordering and incipient meso-scale phase separations etc.. Then we briefly introduce a recently proposed microscopic model which is believed to be a minimal model which, for the first time, includes the three most important interactions present in the manganites namely the following -1)coupling of the orbitally degenerate eg electrons to local lattice distortions of Jahn-Teller type which gives rise to two species of electrons. The one denoted by by ℓ is associated with Jahn-Teller effects and hence is localized whereas the other denoted by b is an extended state and propagates through the lattice. 2) The strong Hund’s couplingof ℓ and b electrons to the t2g core spin and 3) the strong Coulomb correlation between the two species of electrons. Additionally, the model includes a new doping dependent ferromagnetic exchange between the t2g core spins which can arise from “virtual double exchange” mechanism which will be discussed in great detail in Chapter 1 . Finally, we give a brief account on Dynamical Mean Field Theory (DMFT) and Numerical Renormalization Group (NRG) as an impurity solver for the single impurity problem arising under single site DMFT approximation. In Chapter 2 we study the effect of inter-site ℓ - b hybridization on the ‘ℓ - b’ model. The single impurity problem arising under DMFT approximation has close connection with the Vigman-Finkelshtein (VF)model. Then we briefly introduce the VF model and bring out its close connection with the impurity problem. We consider both the particle-hole symmetric as well as the U → ∞ particle-hole asymmetric cases. We derive various spectral functions at T = 0K and discuss the nature of fixed points under various circumstances. We explicitly show that for the particle-hole symmetric case the Hamiltonian flows from X-ray edge singularity fixed point to Free Electron fixed point under Renormalization Group transformation. This is evident from the spectral properties of the model. We write down the effective Hamiltonian at the free electron fixed point. For the particle-hole asymmetric case the model flows from X-ray edge singularity fixed point to Free Electron/Strong Coupling fixed point with additional potential scattering terms. We write down the effective Hamiltonian at this fixed point and derive various leading order deviations. We found all of them to be irrelevant in nature also most interestingly the quasi-particles describing the under lying Fermi liquid state are found to be asymptotically non-interacting. We also calculate the Fermi liquid parameter, z, by analyzing the energy level structure of a non-interacting Hamiltonian with effective renormalized parameter. Also, we consider the case of ‘self consistent bath hybridization’ without ℓ - b hybridization for Bethe lattice with infinite coordination. Low energy qualitative features are found to be same but some of the high energy features get qualitatively modified. In Chapter 3 we discuss the transport properties of doped manganites in the insulating phases and also the Hall effect in the metallic phase. In the first part of this chapter we calculate the resistivity based on the ‘ℓ - b’model and try to fit it to the semiconducting form: ρ(T )= ρ0(T /T0)−nexp[Δ(T )/kBT ] and extract the “transport gap”, Δ(T ). This gap can be characterized in terms of the “spectral gap” which can be defined for the ℓ - b model. It is found that the transport gap in the paramagnetic phase can be characterized in terms of the near constant “spectral gap” in this phase whereas the same in the ferromagnetic phase can be characterized in terms of the zero temperature spectral gap. In the last part of this chapter we calculate the Hall resistivity (ρxy) of these materials in the metallic phase. Ρxy is found to be negative and linear in applied field -quite consistent with the experimental findings but this fails to explain the positive linear Hall resistivity at low temperatures and its crossover as a function of field and temperature. We then present a reasonable explanation for this discrepancy and support it by calculating the Hall density of states for a two band “toy model” involving inter species hybridization. In Chapter 4 we calculate the optical conductivity, σ(ω), in ℓ - b model. σ(ω) arises from two independent processes. One of the processes involves ‘b’ electrons only and termed as ‘b - b channel’ and this gives rise to a Drude peak in the low frequency region. another process termed as the ‘ℓ - b channel’ involves hopping of an ℓ-electron to a neighbouring empty site and transforms into a ‘b’like state. This process gives rise to a broad mid-infrared peak. The total conductivity is the sum of contributions from these two incoherent channels. Calculated σ(ω) for metallic systems shows lot of similarities with experimental observations particularly the temperature evolution of the mid-infrared peak and the spectral weight transfer between the two peaks. But for the insulating systems the calculated optical conductivity showed trends similar to more recent experimental observations on some insulating systems (x =0.125) but contradicts with earlier experimental observations on some other insulating system (x =0.1). Finally, in the concluding chapter, we summarize results from all the chapters and also sketch some possible future directions of investigations.
9

Ladungsanregungen in niedrigdimensionalen Übergangsmetallverbindungen / Charge excitations in low-dimensional transition metal compounds

Hübsch, Arnd 17 July 2001 (has links) (PDF)
Charge excitations in different 3d transition metal compounds are studied. In particular, the influence of the lattice geometry on the character of these excitations is investigated. For this purpose, the momentum dependent loss function of electron energy-loss spectroscopy (EELS) as well as the optical conductivity are calculated and compared with the experimental data of NaV$_{2}$O$_{5}$, LiV$_{2}$O$_{5}$, Sr$_{2}$CuO$_{3}$, and CuGeO$_{3}$ . A quarter-filled extended Hubbard model on a system of coupled ladders provides a qualitative explanation for the highly anisotropic charge excitations of NaV$_{2}$O$_{5}$ and LiV$_{2}$O$_{5}$. These ladder compounds do not only differ from the charge ordering pattern but also from the coupling between different ladders: In LiV$_{2}$O$_{5}$ one finds a strong inter-ladder hopping which is very small in NaV$_{2}$O$_{5}$. On the other hand, in NaV$_{2}$O$_{5}$ the ladders are coupled by a strong inter-ladder Coulomb interaction. The charge excitations of quasi one-dimensional cuprates reflect both the properties of the CuO$_{4}$ plaquettes and the character of the coupling between different plaquettes. Independently from the geometry of the cuprat chains, the local excitation of the copper hole onto the adjacent oxygen orbitals is always found. Further transitions with an excitation energy below the local excitation of a single plaquette result from a hole transfer to another plaquette. These excitations with hole delocalization dominate the spectra of the corner-shared Sr$_{2}$CuO$_{3}$. In contrast to this, the hole transfer leads only to a pre-peak in the spectra of the edge-shared CuGeO$_{3}$. Furthermore, it is shown that the hole transfer is determined by the geometry of the edge-shared CO. / Gegenstand dieser Arbeit ist die theoretische Analyse von Ladungsanregungen in verschiedenen niedrigdimensionalen 3d-Übergangsmetallverbindungen, wobei insbesondere der Einfluß der Gittergeometrie auf die Charakteristik der Anregungen untersucht wurde. Mit Hilfe des Lanczos-Algorithmus' wurden dazu sowohl die impulsabhängige Verlustfunktion der Elektron-Energie-Verlust-Spektroskopie (EELS) als auch die optische Leitfähigkeit für NaV$_{2}$O$_{5}$, LiV$_{2}$O$_{5}$, Sr$_{2}$CuO$_{3}$ und CuGeO$_{3}$ berechnet und mit den experimentellen Ergebnissen verglichen. Unter der Verwendung eines Modells viertelgefüllter Leitern kann man die Ladungsanregungen sowohl für NaV$_{2}$O$_{5}$ als auch LiV$_{2}$O$_{5}$ sehr gut beschreiben. In diesen Materialien findet man nicht nur unterschiedliche Ladungsordnungen sondern vor allem auch verschiedene Kopplungsarten zwischen den Leitern. Während die Leitern im NaV$_{2}$O$_{5}$ durch die Coulomb-Wechselwirkung miteinander gekoppelt sind, existiert im LiV$_{2}$O$_{5}$ ein Austausch aufgrund einer starken Hybridisierung zwischen den Leitern. Die Ladungsanregungen von quasi eindimensionalen Kupratketten spiegeln sowohl die Plaketteneigenschaften als auch die Plakettenkopplung wider. Unabhängig von der Geometrie der Ketten findet man stets die lokale Anregung des Kupferloches auf die umliegenden Sauerstofforbitale. Aus einem möglichen Lochtransfer zu benachbarten Plaketten resultieren außerdem noch Anregungen, die energetisch unterhalb der Plakettenanregung liegen und unmittelbar von der Kettengeometrie abhängen. Während im eckenvernetzten Sr$_{2}$CuO$_{3}$ diese Anregungen die Spektren dominieren, spielt der Lochtransfer im kantenvernetzten CuGeO$_{3}$ nur eine untergeordnete Rolle.
10

Ladungsanregungen in niedrigdimensionalen Übergangsmetallverbindungen

Hübsch, Arnd 26 July 2001 (has links)
Charge excitations in different 3d transition metal compounds are studied. In particular, the influence of the lattice geometry on the character of these excitations is investigated. For this purpose, the momentum dependent loss function of electron energy-loss spectroscopy (EELS) as well as the optical conductivity are calculated and compared with the experimental data of NaV$_{2}$O$_{5}$, LiV$_{2}$O$_{5}$, Sr$_{2}$CuO$_{3}$, and CuGeO$_{3}$ . A quarter-filled extended Hubbard model on a system of coupled ladders provides a qualitative explanation for the highly anisotropic charge excitations of NaV$_{2}$O$_{5}$ and LiV$_{2}$O$_{5}$. These ladder compounds do not only differ from the charge ordering pattern but also from the coupling between different ladders: In LiV$_{2}$O$_{5}$ one finds a strong inter-ladder hopping which is very small in NaV$_{2}$O$_{5}$. On the other hand, in NaV$_{2}$O$_{5}$ the ladders are coupled by a strong inter-ladder Coulomb interaction. The charge excitations of quasi one-dimensional cuprates reflect both the properties of the CuO$_{4}$ plaquettes and the character of the coupling between different plaquettes. Independently from the geometry of the cuprat chains, the local excitation of the copper hole onto the adjacent oxygen orbitals is always found. Further transitions with an excitation energy below the local excitation of a single plaquette result from a hole transfer to another plaquette. These excitations with hole delocalization dominate the spectra of the corner-shared Sr$_{2}$CuO$_{3}$. In contrast to this, the hole transfer leads only to a pre-peak in the spectra of the edge-shared CuGeO$_{3}$. Furthermore, it is shown that the hole transfer is determined by the geometry of the edge-shared CO. / Gegenstand dieser Arbeit ist die theoretische Analyse von Ladungsanregungen in verschiedenen niedrigdimensionalen 3d-Übergangsmetallverbindungen, wobei insbesondere der Einfluß der Gittergeometrie auf die Charakteristik der Anregungen untersucht wurde. Mit Hilfe des Lanczos-Algorithmus' wurden dazu sowohl die impulsabhängige Verlustfunktion der Elektron-Energie-Verlust-Spektroskopie (EELS) als auch die optische Leitfähigkeit für NaV$_{2}$O$_{5}$, LiV$_{2}$O$_{5}$, Sr$_{2}$CuO$_{3}$ und CuGeO$_{3}$ berechnet und mit den experimentellen Ergebnissen verglichen. Unter der Verwendung eines Modells viertelgefüllter Leitern kann man die Ladungsanregungen sowohl für NaV$_{2}$O$_{5}$ als auch LiV$_{2}$O$_{5}$ sehr gut beschreiben. In diesen Materialien findet man nicht nur unterschiedliche Ladungsordnungen sondern vor allem auch verschiedene Kopplungsarten zwischen den Leitern. Während die Leitern im NaV$_{2}$O$_{5}$ durch die Coulomb-Wechselwirkung miteinander gekoppelt sind, existiert im LiV$_{2}$O$_{5}$ ein Austausch aufgrund einer starken Hybridisierung zwischen den Leitern. Die Ladungsanregungen von quasi eindimensionalen Kupratketten spiegeln sowohl die Plaketteneigenschaften als auch die Plakettenkopplung wider. Unabhängig von der Geometrie der Ketten findet man stets die lokale Anregung des Kupferloches auf die umliegenden Sauerstofforbitale. Aus einem möglichen Lochtransfer zu benachbarten Plaketten resultieren außerdem noch Anregungen, die energetisch unterhalb der Plakettenanregung liegen und unmittelbar von der Kettengeometrie abhängen. Während im eckenvernetzten Sr$_{2}$CuO$_{3}$ diese Anregungen die Spektren dominieren, spielt der Lochtransfer im kantenvernetzten CuGeO$_{3}$ nur eine untergeordnete Rolle.

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