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京都大学 / 新制・課程博士 / 博士(理学) / 甲第24873号 / 理博第4983号 / 新制||理||1711(附属図書館) / 京都大学大学院理学研究科化学専攻 / (主査)教授 北川 宏, 教授 有賀 哲也, 教授 堀毛 悟史 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DGAM

[pt] Nesta tese de doutoramento apresentamos a fabricação e a caracterização de dispositivos fotovoltaicos orgânicos (OPVs) fabricados a partir de eletrodos de grafeno e de substratos híbridos flexíveis à base de polímeros recobertos com um filme fino condutor. Para isso, inicialmente sintetizamos filmes de grafeno através da técnica de deposição química em fase de vapor (CVD), seguido de modificações no processo de transferência do grafeno para o substrato desejado. Nesta etapa, desenvolvemos uma nova metodologia utilizando uma blenda condutora de EPDM-PAni que simplifica o processo de transferência e melhora as propriedades elétricas do grafeno. Em outro momento, otimizamos diferentes substratos híbridos à base de polímeros de PVC, PVA e celulose bacteriana (BC) recobertos com um filme fino condutor de ITO. Tanto os substratos híbridos flexíveis, quanto os filmes de grafeno, foram investigados por transmitância ótica e resistência de folha a fim de avaliar os seus potenciais uso para as aplicações em OPVs. Por fim, fabricamos diversas estruturas de OPVs, tanto com o grafeno como eletrodo condutor, quanto usando os substratos híbridos flexíveis. Estes dispositivos foram caracterizados principalmente através das suas curvas características JxV, no escuro e sob iluminação. Além disso, realizamos ciclos de flexão/extensão de alguns dispositivos a fim de avaliar seu comportamento frente aos esforços mecânicos a estes submetidos. Os resultados obtidos mostraram que os filmes de grafeno fabricados são promissores para a aplicação como eletrodo condutor transparente em OPVs e que os substratos híbridos investigados podem ser utilizados em dispositivos flexíveis, visto que apresentaram comportamento semelhante aos substratos inorgânicos comumente utilizados. / [en] In this doctoral thesis we present the fabrication and characterization of organic photovoltaic devices (OPVs) assembled onto graphene electrodes and flexible hybrid polymers-based substrates coated with a conductive thin film. For this, initially the graphene films were synthesized by chemical vapor deposition (CVD) technique, followed by modifications in the transfer process of the graphene to the desired substrate. In this step, we developed a new methodology using an EPDM-PAni conductive blend that simplifies the transfer process and improves the electric properties of graphene. We also used another approach which consists in optimizing different hybrid substrates based on PVC, PVA and bacterial cellulose (BC) polymers coated with an ITO conductive thin film. The flexible hybrid substrates as well as the graphene films were investigated by optical transmittance and sheet resistance in order to evaluate their potential use for OPVs applications. Finally, we fabricate various structures of OPVs, using graphene as a conducting electrode, well as using flexible hybrid substrates. Such devices were characterized mainly through their dark and light J×V characteristic curves. In addition, we performed flexion/extension cycles in some devices in order to evaluate their behavior against the mechanical stresses submitted to them. The results showed that the graphene films are a promising material for the application as a transparent conductive electrode in OPVs and the hybrid substrates investigated can be used in flexible devices, since they presented similar behavior to the commonly used inorganic substrates.

Organische Leuchtdioden weisen, verglichen mit anorganischen Leuchtdioden, viele Vorteile auf. So sind sie nicht nur energiesparender, sondern können auch in neuen flexiblen Technologien verwendet werden. Um ihr volles Potenzial auszuschöpfen, können zusätzliche Schichten und neue Materialien hinzugefügt werden. Der Ersatz spröder Elektroden durch dünne Metallschichten kann OLEDs flexibler machen, Zwischenschichten verbessern den Ladungstransport und neuartige Materialien können die Lösungsprozessierung von OLEDs vereinfachen. In den Kapiteln dieser Arbeit wurden je ein Ansatz zur Steigerung der Leistung von OLEDs untersucht. Es wurden dünne Silberschichten aus einer partikelfreien Silbertinte mittels Tintenstrahldruck hergestellt und ihre optischen sowie elektrischen charakterisiert. Die gedruckten Elektroden zeigen eine hohe Biegefestigkeit, bei gleichbleibend guten elektrischen Eigenschaften. Die damit hergestellten Leuchtdioden übertreffen in ihrer Effizienz Referenzdioden mit Indium Zinn Oxid Elektroden. Um die Effizienz organischer Leuchtdioden weiter steigern zu können wurden anschließend Zwischenschichten untersucht. Mittels einer gemischten Schicht aus Zinkoxid und einem Polymer konnte die Effizienz von invertierten Leuchtdioden signifikant gesteigert werden. Weiterhin wurden zwei neu synthetisierte Moleküle dazu verwendet, um die Benetzung von Perowskiten auf Elektroden zu verbessern und somit ihre Herstellbarkeit mittels Tintenstrahldruck zu ermöglichen. Abschließend wurde das Quervernetzen von Polymeren zur Herstellung von Mehrschichtsystemen erforscht. Hierbei wird ein die Löslichkeit eines Polymers durch verschiedene Ansätze verringert. Anhand des lichtemittierenden Polymers Super Yellow wurde dies demonstriert. Die Beständigkeit einer Schicht aus Super Yellow gegenüber Toluol konnte erfolgreich stark erhöht werden. Somit wurde eine nachfolgende Prozessierung einer zusätzlichen Schicht aus demselben Lösungsmittel ermöglicht. / Organic light-emitting diodes have many advantages compared to their inorganic counterparts. Not only can they be used more energy-efficiently, but they can also be used in new, flexible technologies. To reach their full potential, additional layers and new materials can be added. Replacing brittle electrodes with thin metal layers can make OLEDs more flexible, intermediate layers improve charge transport, and novel materials can simplify solution processing of OLEDs. In each of the chapters of this thesis, an approach to increasing the performance of OLEDs was examined. Thin silver layers were produced from a particle-free silver ink using inkjet. Their optical and electrical properties were characterized. The printed electrodes show a high flexural strength while retaining good electrical properties. The efficacy of the light-emitting diodes produced in this way exceeds that of reference diodes. To be able to further increase the efficiency of organic light-emitting diodes, intermediate layers made of new material combinations were subsequently investigated. The efficiency of inverted light-emitting diodes could be significantly increased by means of a blend intermediate layer made of zinc oxide and a polymer. Furthermore, two newly synthesized molecules were used to improve the wetting of perovskites on electrodes and thus enable their manufacturability using inkjet printing. Finally, crosslinking of polymers to fabricate multilayer devices was investigated. Here, the solubility of a polymer is reduced by various approaches. This principle was demonstrated using the light-emitting polymer Super Yellow. The resistance of a layer of Super Yellow against toluene was successfully reduced significantly. Thus, subsequent processing of an additional layer from the same solvent was made possible.