@phdthesis{Hartmann2012, author = {Hartmann, Fabian}, title = {Elektrooptische Transporteigenschaften und stochastisch aktivierte Prozesse Resonanter Tunneldioden}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-90876}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2012}, abstract = {Im Rahmen der vorliegenden Arbeit wurden elektrooptische Transporteigenschaften und stochastisch aktivierte Prozesse Resonanter Tunneldioden (RTDs) bei Raumtemperatur untersucht. Die RTDs wurden auf dem III-V Halbleitermaterialsystem AlGaAs/GaAs durch Molekularstrahlepitaxie, Elektronenstrahllithographie und trockenchemischen {\"A}tztechniken hergestellt. Im Bereich des negativen differentiellen Leitwerts konnte bistabi-les Schalten und hierbei stochastisch aktivierte Dynamik nichtlinearer Systeme untersucht werden. Die Fl{\"a}chenabh{\"a}ngigkeit der {\"A}tzrate konnte ausgenutzt werden, um RTDs mit einem Stamm und zwei Transport{\"a}sten zu realisieren, welche hinsichtlich ihrer optischen und elektrischen Eigenschaften untersucht wurden. Im ersten experimentellen Abschnitt 3.1 werden die elektrischen Transporteigenschaften Resonanter Tunneldioden bei Raum-temperatur und die Fl{\"a}chenabh{\"a}ngigkeit des koh{\"a}renten und nicht-koh{\"a}renten Elektronen-transports analysiert. Die Realisierung universeller logischer Gatter (NOR und NAND) und deren Rekonfigurierbarkeit durch einen externen Kontrollparameter wird in Abschnitt 3.2 gezeigt. In Abschnitt 3.3 wird die Lichtsensitivit{\"a}t Resonanter Tunneldioden als Photode-tektoren f{\"u}r den sichtbaren Wellenl{\"a}ngenbereich und in Abschnitt 3.4 f{\"u}r die Telekommu-nikationswellenl{\"a}nge bei λ = 1,3 µm demonstriert.}, subject = {Resonanz-Tunneldiode}, language = {de} } @phdthesis{Wagenpfahl2013, author = {Wagenpfahl, Alexander Johannes}, title = {Numerical simulations on limitations and optimization strategies of organic solar cells}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-90119}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2013}, abstract = {Continuously increasing energy prices have considerably influenced the cost of living over the last decades. At the same time increasingly extreme weather conditions, drought-filled summers as well as autumns and winters with heavier rainfall and worsening storms have been reported. These are possibly the harbingers of the expected approaching global climate change. Considering the depletability of fossil energy sources and a rising distrust in nuclear power, investigations into new and innovative renewable energy sources are necessary to prepare for the coming future. In addition to wind, hydro and biomass technologies, electricity generated by the direct conversion of incident sunlight is one of the most promising approaches. Since the syntheses and detailed studies of organic semiconducting polymers and fullerenes were intensified, a new kind of solar cell fabrication became conceivable. In addition to classical vacuum deposition techniques, organic cells were now also able to be processed from a solution, even on flexible substrates like plastic, fabric or paper. An organic solar cell represents a complex electrical device influenced for instance by light interference for charge carrier generation. Also charge carrier recombination and transport mechanisms are important to its performance. In accordance to Coulomb interaction, this results in a specific distribution of the charge carriers and the electric field, which finally yield the measured current-voltage characteristics. Changes of certain parameters result in a complex response in the investigated device due to interactions between the physical processes. Consequently, it is necessary to find a way to generally predict the response of such a device to temperature changes for example. In this work, a numerical, one-dimensional simulation has been developed based on the drift-diffusion equations for electrons, holes and excitons. The generation and recombination rates of the single species are defined according to a detailed balance approach. The Coulomb interaction between the single charge carriers is considered through the Poisson equation. An analytically non-solvable differential equation system is consequently set-up. With numerical approaches, valid solutions describing the macroscopic processes in organic solar cells can be found. An additional optical simulation is used to determine the spatially resolved charge carrier generation rates due to interference. Concepts regarding organic semiconductors and solar cells are introduced in the first part of this work. All chapters are based on previous ones and logically outline the basic physics, device architectures, models of charge carrier generation and recombination as well as the mathematic and numerical approaches to obtain valid simulation results. In the second part, the simulation is used to elaborate issues of current interest in organic solar cell research. This includes a basic understanding of how the open circuit voltage is generated and which processes limit its value. S-shaped current-voltage characteristics are explained assigning finite surface recombination velocities at metal electrodes piling-up local space charges. The power conversion efficiency is identified as a trade-off between charge carrier accumulation and charge extraction. This leads to an optimum of the power conversion efficiency at moderate to high charge carrier mobilities. Differences between recombination rates determined by different interpretations of identical experimental results are assigned to a spatially inhomogeneous recombination, relevant for almost all low mobility semiconductor devices.}, subject = {Organische Solarzelle}, language = {en} } @phdthesis{Kern2013, author = {Kern, Julia}, title = {Field Dependence of Charge Carrier Generation in Organic Bulk Heterojunction Solar Cells}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-91963}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2013}, abstract = {In the field of organic photovoltaics, one of the most intensely researched topics to date is the charge carrier photogeneration in organic bulk heterojunction solar cells whose thorough understanding is crucial for achieving higher power conversion efficiencies. In particular, the mechanism of singlet exciton dissociation at the polymer-fullerene interface is still controversially debated. This work addresses the dissociation pathway via relaxed charge transfer states (CTS) by investigating its field dependence for reference material systems consisting of MDMO-PPV and one of the fullerene derivatives PC61BM, bisPCBM and PC71BM. Field dependent photoluminescence (PL(F)) and transient absorption (TA(F)) measurements give insight into the recombination of charge transfer excitons (CTE) and the generation of polarons, respectively. Optically detected magnetic resonance and atomic force microscopy are used to characterize the morphology of the samples. The comparison of the experimental field dependent exciton recombination recorded by PL(F) and the theoretical exciton dissociation probability given by the Onsager-Braun model yields the exciton binding energy as one of the key parameters determining the dissociation efficiency. The binding energies of both the singlet exciton in neat MDMO-PPV and the CTE in MDMO-PPV:PC61BM 1:1 are extracted, the latter turning out to be significantly reduced with respect to the one of the singlet exciton. Based on these results, the field dependence of CTE dissociation is evaluated for MDMO-PPV:PC61BM blends with varying fullerene loads by PL(F) and TA(F). For higher PC61BM contents, the CTE binding energies decrease notably. This behavior is ascribed to a larger effective dielectric constant for well-intermixed blends and to an interplay between dielectric constant and CTE delocalization length for phase separated morphologies, emphasizing the importance of high dielectric constants for the charge carrier photogeneration process. Finally, the CTE binding energies are determined for MDMO-PPV blends with different fullerene derivatives, focusing on the influence of the acceptor LUMO energy. Here, the experimental results suggest the latter having no or at least no significant impact on the binding energy of the CTE. Variations of this binding energy are rather related to different trap levels in the acceptors which seem to be involved in CTS formation.}, subject = {Organische Solarzelle}, language = {en} } @phdthesis{Rauh2013, author = {Rauh, Daniel}, title = {Impact of Charge Carrier Density and Trap States on the Open Circuit Voltage and the Polaron Recombination in Organic Solar Cells}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-90083}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2013}, abstract = {The focus of this work is studying recombination mechanisms occurring in organic solar cells, as well as their impact on one of their most important parameters — the open circuit voltage Voc. Firstly, the relationship between Voc and the respective charge carrier density n in the active layer under open circuit conditions is analyzed. Therefor, a model after Shockley for the open circuit voltage is used, whose validity is proven with the aid of fits to the measured data. Thereby, it is emphasized that the equation is only valid under special conditions. In the used reference system P3HT:PC61BM the fits are in agreement with the measurement data only in the range of high temperatures (150 - 300 K), where Voc increases linearly with decreasing temperature. At lower temperatures (50 - 150 K), the experiment shows a saturation of Voc. This saturation cannot be explained with the model by the measured falling charge carrier density with decreasing temperatures. In this temperature range Voc is not directly related to the intrinsic properties of the active layer. Voc saturation is due to injection energy barriers at the contacts, which is ascertained by macroscopic simulations. Furthermore, it is observed that Voc in the case of saturation is equivalent to the so-called built-in potential. The difference between the built-in potential and the energy gap corresponds thereby to the sum of the energy barriers at both contacts. With the knowledge of the Voc(n) dependency for not contact limited solar cells, it is possible to investigate the recombination mechanisms of charge carriers in the active layer. For Langevin recombination the recombination rate is Rn2 (recombination order RO = 2), for Shockley-Read-Hall (SRH) Rn1 (RO=1); in various publications RO higher than two is reported with two main explanations. 1: Trap states for charge carriers exist in the respective separated phases, i.e. electrons in the acceptor phase and holes in the donor phase, which leads to a delayed recombination of the charge carriers at the interface of both phases and finally to an apparent recombination order higher than 2. 2: The enhanced R(n) dependency is attributed to the so called recombination prefactor, which again is dependent from n dependent mobility µ. It is shown that for the system P3HT:PC61BM at room temperature the µ(n) dependency does nearly completely explain the higher RO but not at lower temperatures which in this case supports the first explanation. In the material system PTB7:PC71BM the increased RO cannot be explained by the µ(n) dependency even at room temperature. To support the importance of trap states in combination with a phase separation for the explanation of the enhanced RO, additional trap states were incorporated in the solar cells to investigate their influence on the recombination mechanisms. To achieve this, P3HT:PC61BM solar cells were exposed to synthetic air (in the dark and under illumination) or TCNQ was added in small concentrations to the active layer which act as electron traps. For the oxygen degraded solar cell the recombination order is determined by a combination of open Voc-transients and Voc(n) measurements. Thereby, a continuous increase of the recombination order from 2.4 to more than 5 is observed with higher degradation times. By the evaluation of the ideality factor it can be shown that the impact of SRH recombination is increasing with higher trap concentration in relation to Langevin recombination. A similar picture is revealed for solar cells with TCNQ as extrinsic trap states. Finally, a phenomenon called s-shaped IV-curves is investigated, which can sometimes occur for solar cells under illumination. As course of this a reduced surface recombination velocity can be found. Experimentally, the solar cells were fabricated using a special plasma treatment of the ITO contact. The measured IV-curves of such solar cells are reproduced by macroscopic simulations, where the surface recombination velocity is reduced. Hereby, it has to be distinguished between the surface recombination of majority and minority charge carriers at the respective contacts. The theory can be experimentally confirmed by illumination level dependent IV-curves as well as short circuit current density and open circuit voltage transients.}, subject = {Organische Solarzelle}, language = {en} } @phdthesis{Kraus2014, author = {Kraus, Hannes}, title = {Optically Detected Magnetic Resonance on Organic and Inorganic Carbon-Based Semiconductors}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-106308}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2014}, abstract = {In dieser Arbeit werden drei verschiedene kohlenstoffbasierte Materialsysteme behandelt: (i) Organische Halbleiter und kleine Molek{\"u}le, in Kombination mit Fullerenen f{\"u}r Anwendungen in der organischen Photovoltaik (OPV), (ii) Halbleitende Einzelwand-Kohlenstoffnanor{\"o}hren und (iii) Siliziumkarbid (SiC), dessen Defekte erst seit kurzem als Kandidaten f{\"u}r Quantenapplikationen gehandelt werden. Alle Systeme wurden mit optisch detektierter Magnetresonanzspektroskopie (ODMR) untersucht. Im OPV-Kapitel, die intrinsischen Parameter und Orientierungen von Exzitonen mit hohem Spin wurden f{\"u}r die Materialsysteme P3HT, PTB7 und DIP untersucht. Speziell der Einfluss von Ordnung diesen organischen Systemen wurde diskutiert. Der zweite Teil des Kapitels besch{\"a}ftigt sich mit Triplettgeneration mittels Elektronenr{\"u}cktransfer im leistungsf{\"a}higen Materialsystem PTB7:PC71BM. Das Kohlenstoffnanor{\"o}hren-Kapitel zeigt zuert den ersten zweifelsfreien Nachweis von Triplettexzitonen in halbleitenden (6,5) Einzelwandkohlenstoffnanor{\"o}hren (SWNT), mittels ODMR-Spektroskopie. Ein Modell f{\"u}r die Anregungskinetik, die intrinsischen Parameter des Exzitons und Abh{\"a}ngigkeit von der Orientierung der R{\"o}hren wurden diskutiert. Der letzte Teil der Arbeit gilt Spinzentren in Siliziumkarbid. Nach einer kurzen Einf{\"u}hrung in das Materialsystem wird die Spinmultiplizit{\"a}t f{\"u}r die V2 und V3 Siliziumfehlstellen, sowie eines Frenkelpaars und eines noch nicht zugeordneten Defekts (UD) in 6H SiC, weiterhin f{\"u}r die V2 Fehlstelle und das Frenkelpaar in 4H SiC, durchg{\"a}ngig zu S=3/2 festgestellt. Das spinpolarisierte Bef{\"u}llen der 3/2-Zust{\"a}nde des Grundzustands der Siliziumfehlstellen erlaubt stimulierte Mikrowellenemission. Ausserdem wurde f{\"u}r UD und Frenkelpaar in 6H SiC eine große Temperaturabh{\"a}ngigkeit der Nullfeldparameter festgestellt, w{\"a}hrend die Siliziumfehlstellen temperaturunabh{\"a}ngig sind. Anwendung des UD und Frenkelpaars als Temperatursensor, und der Vakanzen als Vektormagnetometer wurden diskutiert.}, subject = {ODMR-Spektroskopie}, language = {en} } @phdthesis{Gorenflot2014, author = {Gorenflot, Julien Fran{\c{c}}ois}, title = {Optical study of the excited states in the semiconducting polymer poly(3-hexylthiophene) for photovoltaic applications}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-116730}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2014}, abstract = {In the course of this dissertation, we have presented the interest of using spectroscopic methods to unravel the physics of polymer semiconductors in photovoltaic applications. Applying photoluminescence and photoinduced absorption spectroscopy to the reference system P3HT:PCBM has enabled us to study the major steps of photocurrent generation in organic bulk heterojunctions, from excitons generation to charges extraction and loss mechanisms and thus to improve the understanding of those mechanisms. The exciton binding energy, is the first obstacle to overcome for photocurrent generation in organic solar cell and the reason for the use of two materials, whose heterojunction act as a driving force for charge separation. We developed an original photoluminescence-detected field-induced exciton quenching method to investigate this energy. Absorption and photoluminescence spectra of pure P3HT show that, while both amorphous and crystalline domains participate in absorption, the energy is then transferred to the crystalline domains, from where the photoluminescence is exclusively originating. The field dependence of this photoluminescence showed that an energy of no less than 420 meV is necessary to split excitons into non photon-emitting species. Comparing those results with energy levels obtained by absorption and photoelectron spectroscopies, confirmed that the formation of those species is only a first step toward dissociation into free charges. Indeed, photoemission spectroscopy and the onset of photocurrent upon increasing the photon energy in a pure P3HT solar cell, concomitantly show that the energy level of a pair of free polarons is located 0.7 eV above the one of the exciton. The comprehensive analysis of those results originating from those different method enable us to draw a global picture of the states and energies involved in free polarons generation in pure material. This work has been widely acknowledged by the scientific community, published in Physical Review B in 2010 [1] and presented in national [2] and international [3] conferences. The spectroscopy of excited states is used to detect the presence of wanted species (charges) and potentially unwanted neutral species upon photoexcitation. As such, it offers us the possibility to qualify the efficiency of charge generation and, if any, identify the competing processes and the generation of unwanted species. In the frame of the European Marie Curie Research Network SolarNType,[4] this possibility was used - in combination with morphological, charge transport and devices characterizationsn - to study a number of new donor:acceptor blends. Thanks to those techniques, we were able to not only quantify the potential of those blends, but also to provide the chemist laboratories with a precious and detailed feedback on the strengths and weakness of the molecules, regarding charge generation, transport and extraction. The detailed study of terrylene-3,4:11,12-bis(dicarboximide) as electron acceptor for solar cells application was published in the peer review journal Synthetic Metals and was chosen to illustrate the cover page of the issue [5]. Finally, in the last chapter, we have used time resolved photoinduced absorption to improve the understanding of the charge carrier loss mechanisms in P3HT:PCBM active layers. This comprehension is of prime importance because, the fact that this recombination is far weaker than expected from the Langevin theory, enable polarons to travel further without recombining and thus to build thicker and more efficient devices. A comprehensive analysis of steady-state PIA spectra of pure P3HT, indicates that probing at 980 nm at a temperature between 140 and 250 K enables to monitor specifically polaron densities in both neat P3HT and P3HT:PCBM. Applying this finding to transient absorption enabled us to monitor, for the first time, the bimolecular recombination in pure P3HT, and to discover that - in sharp contrast with the blend - this recombination was in agreement with the Langevin theory. Moreover, it enables us to pinpoint the important role played by the existence of two materials and of energetical traps in the slow recombination and high recombination orders observed in the blend. This work has been published in the Journal of Applied Physics.[6] Those new insights in the photophysics of polymer:fullerene photoactive layers could have a strong impact on the future developement of those materials. Consistent measurements of the binding energy of excitons and intermediate species, would enable to clarify the role played by excess thermal energy in interfacial states dissociation. Better understanding of blends morphology and its influence on solar cells parameters and in particular on recombination could enable to reproduce the conditions of limited recombination on material systems offering some promising performances but with only limited active layer thicknesses. However, due to the number of parameters involved, further experimentation is required, before we can reach a quantitative modeling of bimolecular recombination. [1] Deibel et al., Phys. Rev. B, 81:085202, 2010 [2] Gorenflot et al., Deutsche Physikalische Gesellschaft Fr{\"u}hjahrstagung 2010, CPP20:10, Regensburg, Germany, 2010 [3] Gorenflot et al., International Conference of Synthetic Metals, 7Ax:05, Kyoto, Japan, 2010 [4] Marie-Curie RTN "SolarNTyp" Contract No. MRTN-CT-2006-035533 [5] Gorenflot et al., Synth. Met., 161(23{24):2669-2676, 2012 [6] Gorenflot et al., J. Appl. Phys., 115(14):144502, 2014}, subject = {Organische Solarzelle}, language = {en} } @phdthesis{Gieseking2014, author = {Gieseking, Bj{\"o}rn}, title = {Excitation Dynamics and Charge Carrier Generation in Organic Semiconductors}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-101625}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2014}, abstract = {The transport of optically excited states, called excitons, as well as their conversion into charges define the two major steps allowing for the operation of organic photovoltaic (OPV) devices. Hence, a deep understanding of these processes, the involved mechanisms as well as possible loss channels is crucial for further improving the efficiency of organic solar cells. For studying the aforementioned processes spectroscopic methods like absorption and emission measurements are useful tools. As many of the processes take place on a sub-nanosecond (ns) timescale ultrafast spectroscopic methods are required. Due to this reason two experiments based on a femtosecond laser system were built and employed in this work, namely picosecond (ps) time-resolved photoluminescence (PL) and transient absorption (TA) spectroscopy. By analyzing the PL decay dynamics in the prototypical organic semiconductor rubrene, the feasibility of a new approach for improving the efficiency of organic solar cells by harvesting triplet excitons generated by singlet fission was examined. Singlet fission describes a process where two triplet excitons are generated via a photoexcited singlet exciton precursor state if the energy of the two triplets is comparable with the energy of the singlet. For this purpose the influence of characteristic length scales on the exciton dynamics in different rubrene morphologies exhibiting an increasing degree of confinement was analyzed. The results show that the quenching at interfacial states efficiently suppresses the desired fission process if these states are reached by excitons during migration. Since interfacial states are expected to play a significant role in thin film solar cells and are easily accessible for the migrating excitons, the results have to be considered for triplet-based OPV. While the aforementioned approach is only investigated for model systems so far, the efficiency of disordered organic bulk heterojunction (BHJ) solar cells could be significantly enhanced in the last couple of years by employing new and more complex copolymer donor materials. However, little is known about the photophysics and in particular the excitation dynamics of these systems. By carrying out a systematic optical study on the prominent copolymer PCDTBT and its building blocks we were able to identify the nature of the two characteristic absorption bands and the coupling mechanism between these levels. The latter mechanism is based on an intrachain partial charge transfer between two functional subunits and our time-resolved measurements indicate that this coupling governs the photophysical properties of solar cells based on these copolymers. The efficient coupling of functional subunits can be seen as a key aspect that guarantees for the success of the copolymer approach. Another important issue concerns the optimization of the morphology of BHJ solar cells. It arises from the discrepancy between the exciton diffusion length \mbox{(\$\approx\$ 10 nm)} and the absorption length of solar irradiation (\$\approx\$ 100 nm). Due to this reason, even for devices based on new copolymer materials, processing parameters affecting the morphology like annealing or employing processing additives are of major importance. In our combined optical, electrical and morphological study for solar cells based on the high-efficient copolymer PBDTTT-C we find a direct correlation between additive content and intermixing of the active layer. The observed maximum in device efficiency can be attributed to a morphology guaranteeing for an optimized balance between charge generation and transport. Our results highlight the importance of understanding the influence of processing parameters on the morphology of the BHJ and thus on the efficiency of the device.}, subject = {Organische Solarzelle}, language = {en} } @phdthesis{Wolf2015, author = {Wolf, Nadine}, title = {Synthese, Charakterisierung und Modellierung von klassischen Sol-Gel- und Nanopartikel-Funktionsschichten auf der Basis von Zinn-dotiertem Indiumoxid und Aluminium-dotiertem Zinkoxid}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-112416}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2015}, abstract = {Das Ziel dieser Arbeit ist neben der Synthese von Sol-Gel-Funktionsschichten auf der Basis von transparent leitf{\"a}higen Oxiden (transparent conducting oxides, TCOs) die umfassende infrarotoptische und elektrische Charakterisierung sowie Modellierung dieser Schichten. Es wurden sowohl {\"u}ber klassische Sol-Gel-Prozesse als auch {\"u}ber redispergierte Nanopartikel-Sole spektralselektive Funktionsschichten auf Glas- und Polycarbonat-Substraten appliziert, die einen m{\"o}glichst hohen Reflexionsgrad im infraroten Spektralbereich und damit einhergehend einen m{\"o}glichst geringen Gesamtemissionsgrad sowie einen niedrigen elektrischen Fl{\"a}chenwiderstand aufweisen. Zu diesem Zweck wurden dotierte Metalloxide, n{\"a}mlich einerseits Zinn-dotiertes Indiumoxid (tin doped indium oxide, ITO) und andererseits Aluminium-dotiertes Zinkoxid (aluminum doped zinc oxide, AZO)verwendet. Im Rahmen dieser Arbeit wurden vertieft verschiedene Parameter untersucht, die bei der Pr{\"a}paration von niedrigemittierenden ITO- und AZO-Funktionsschichten im Hinblick auf die Optimierung ihrer infrarot-optischen und elektrischen Eigenschaften sowie ihrer Transmission im sichtbaren Spektralbereich von Bedeutung sind. Neben der Sol-Zusammensetzung von klassischen Sol-Gel-ITO-Beschichtungsl{\"o}sungen wurden auch die Beschichtungs- und Ausheizparameter bei der Herstellung von klassischen Sol-Gel-ITO- sowie -AZO-Funktionsschichten charakterisiert und optimiert. Bei den klassischen Sol-Gel- ITO-Funktionsschichten konnte als ein wesentliches Ergebnis der Arbeit der Gesamtemissionsgrad um 0.18 auf 0.17, bei in etwa gleichbleibenden visuellen Transmissionsgraden und elektrischen Fl{\"a}chenwiderst{\"a}nden, reduziert werden, wenn anstelle von (optimierten) Mehrfach-Beschichtungen Einfach-Beschichtungen mit einer schnelleren Ziehgeschwindigkeit anhand des Dip-Coating-Verfahrens hergestellt wurden. Mit einer klassischen Sol-Gel-ITO-Einfach-Beschichtung, die mit einer deutlich erh{\"o}hten Ziehgeschwindigkeit von 600 mm/min gedippt wurde, konnte mit einem Wert von 0.17 der kleinste Gesamtemissionsgrad dieser Arbeit erzielt werden. Die Gesamtemissionsgrade und elektrischen Fl{\"a}chenwiderst{\"a}nde von klassischen Sol-Gel-AZOFunktionsschichten konnten mit dem in dieser Arbeit optimierten Endheizprozess deutlich gesenkt werden. Bei Neunfach-AZO-Beschichtungen konnten der Gesamtemissionsgrad um 0.34 auf 0.50 und der elektrische Fl{\"a}chenwiderstand um knapp 89 \% auf 65 Ω/sq verringert werden. Anhand von Hall-Messungen konnte dar{\"u}ber hinaus nachgewiesen werden, dass mit dem optimierten Endheizprozess, der eine erh{\"o}hte Temperatur w{\"a}hrend der Reduzierung der Schichten aufweist, mit N = 4.3·1019 cm-3 eine etwa doppelt so hohe Ladungstr{\"a}gerdichte und mit µ = 18.7 cm2/Vs eine etwa drei Mal so große Beweglichkeit in den Schichten generiert wurden, im Vergleich zu jenen Schichten, die nach dem alten Endheizprozess ausgeh{\"a}rtet wurden. Das deutet darauf hin, dass bei dem optimierten Heizschema sowohl mehr Sauerstofffehlstellen und damit eine h{\"o}here Ladungstr{\"a}gerdichte als auch Funktionsschichten mit einem h{\"o}heren Kristallisationsgrad und damit einhergehend einer h{\"o}heren Beweglichkeit ausgebildet werden. Ein Großteil der vorliegenden Arbeit behandelt die Optimierung und Charakterisierung von ITO-Nanopartikel-Solen bzw. -Funktionsschichten. Neben den verwendeten Nanopartikeln, dem Dispergierungsprozess, der Beschichtungsart sowie der jeweiligen Beschichtungsparameter und der Nachbehandlung der Funktionsschichten, wurde erstmals in einer ausf{\"u}hrlichen Parameterstudie die Sol-Zusammensetzung im Hinblick auf die Optimierung der infrarot-optischen und elektrischen Eigenschaften der applizierten Funktionsschichten untersucht. Dabei wurde insbesondere der Einfluss der verwendeten Stabilisatoren sowie der verwendeten L{\"o}sungsmittel auf die Schichteigenschaften charakterisiert. Im Rahmen dieser Arbeit wird dargelegt, dass die exakte Zusammensetzung der Nanopartikel-Sole einen große Rolle spielt und die Wahl des verwendeten L{\"o}sungsmittels im Sol einen gr{\"o}ßeren Einfluss auf den Gesamtemissionsgrad und die elektrischen Fl{\"a}chenwiderst{\"a}nde der applizierten Schichten hat als die Wahl des verwendeten Stabilisators. Allerdings wird auch gezeigt, dass keine pauschalen Aussagen dar{\"u}ber getroffen werden k{\"o}nnen, welcher Stabilisator oder welches L{\"o}sungsmittel in den Nanopartikel-Solen zu Funktionsschichten mit kleinen Gesamtemissionsgraden und elektrischen Fl{\"a}chenwiderst{\"a}nden f{\"u}hrt. Stattdessen muss jede einzelne Kombination von verwendetem Stabilisator und L{\"o}sungsmittel empirisch getestet werden, da jede Kombination zu Funktionsschichten mit anderen Eigenschaften f{\"u}hrt. Zudem konnte im Rahmen dieser Arbeit erstmals stabile AZO-Nanopartikel-Sole {\"u}ber verschiedene Rezepte hergestellt werden. Neben der Optimierung und Charakterisierung von ITO- und AZO- klassischen Sol-Gel- sowie Nanopartikel-Solen und -Funktionsschichten wurden auch die infrarot-optischen Eigenschaften dieser Schichten modelliert, um die optischen Konstanten sowie die Schichtdicken zu bestimmen. Dar{\"u}ber hinaus wurden auch kommerziell erh{\"a}ltliche, gesputterte ITO- und AZO-Funktionsschichten modelliert. Die Reflexionsgrade dieser drei Funktionsschicht-Typen wurden einerseits ausschließlich mit dem Drude-Modell anhand eines selbstgeschriebenen Programmes in Sage modelliert, und andererseits mit einem komplexeren Fit-Modell, welches in der kommerziellen Software SCOUT aus dem erweiterten Drude-Modell, einem Kim-Oszillator sowie dem OJL-Modell aufgebaut wurde. In diesem Fit-Modell werden auch die Einfl{\"u}sse der Glas-Substrate auf die Reflexionsgrade der applizierten Funktionsschichten ber{\"u}cksichtigt und es k{\"o}nnen die optischen Konstanten sowie die Dicken der Schichten ermittelt werden. Dar{\"u}ber hinaus wurde im Rahmen dieser Arbeit ein Ellipsometer installiert und geeignete Fit-Modelle entwickelt, anhand derer die Ellipsometer-Messungen ausgewertet und die optischen Konstanten sowie Schichtdicken der pr{\"a}parierten Schichten bestimmt werden k{\"o}nnen.}, subject = {Transparent-leitendes Oxid}, language = {de} } @phdthesis{Spaeth2015, author = {Sp{\"a}th, Florian Leonhard}, title = {Pr{\"a}paration und Charakterisierung einwandiger Kohlenstoffnanorohr-Polyfluoren-Komplexe}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-123874}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2015}, abstract = {Im Fokus dieser Arbeit standen (6,5)-SWNT-PFO-BPy-Komplexe als Vertreter f{\"u}r polyfluorenstabilisierte, einwandige Kohlenstoffnanor{\"o}hren. In einem ersten Projekt wurden pr{\"a}parative Verfahren zur Dispergierung und Abscheidung dieser Proben weiterentwickelt. Es ist gelungen, die Ansatzgr{\"o}ße von 15 mL auf 200 mL hochzuskalieren sowie d{\"u}nne SWNT-Filme {\"u}ber Rotationsbeschichtung herzustellen. Des Weiteren wurde die lichtinduzierte Dynamik in halbleitenden SWNTs von der ps- bis zur µs-Zeitskala untersucht. Hier wurde ein umfassendes Bild zur Singulett- und Triplett-Exzitonendynamik in halbleitenden Kohlenstoffnanor{\"o}hren gezeichnet, welches maßgeblich durch diffusionslimitierte Prozesse gepr{\"a}gt ist. Abschließend wurde eine Methode vorgestellt, mit der sich Informationen zur Struktur von SWNT-Polymer-Komplexen und anderen supramolekularen Systemen gewinnen lassen. Diese basiert auf der Kombination von polarisationswinkelaufgel{\"o}ster Absorptionsspektroskopie an anisotropen Proben und globaler Datenanalyse.}, subject = {Kohlenstoff-Nanor{\"o}hre}, language = {de} } @phdthesis{Fuchs2015, author = {Fuchs, Franziska}, title = {Optical spectroscopy on silicon vacancy defects in silicon carbide}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-124071}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2015}, abstract = {This work sheds light on different aspects of the silicon vacancy in SiC: (1) Defect creation via irradiation is shown both with electrons and neutrons. Optical properties have been determined: the excitation of the vacancy is most efficient at excitation wavelengths between 720nm and 800nm. The PL decay yields a characteristic excited state lifetime of (6.3±0.6)ns. (2) Defect engineering, meaning the controlled creation of vacancies in SiC with varying neutron fluence. The defect density could be engineered over eight orders of magnitude. On the one hand, in the sample with highest emitter density, the huge PL signal could even be enhanced by factor of five via annealing mechanisms. On the other hand, in the low defect density samples, single defects with photostable room temperature NIR emission were doubtlessly proven. Their lifetime of around 7ns confirmed the value of the transient measurement. (3) Also electrical excitation of the defects has been demonstrated in a SiC LED structure. (4) The investigations revealed for the first time that silicon vacancies can even exist SiC nanocrystals down to sizes of about 60 nm. The defects in the nanocrystals show stable PL emission in the NIR and even magnetic resonance in the 600nm fraction. In conclusion, this work ascertains on the one hand basic properties of the silicon vacancy in silicon carbide. On the other hand, proof-of-principle measurements test the potential for various defect-based applications of the vacancy in SiC, and confirm the feasibility of e.g. electrically driven single photon sources or nanosensing applications in the near future.}, subject = {Siliciumcarbid}, language = {en} }