This thesis deals with theoretical studies of the electronic structure of molecules used in the context of molecular electronics. Both studies with model Hamiltonians and first principle calculations have been performed. The materials studied include molecular crystals of pentacene and DNA, which are used as active material in field-effect transistors and as tentative molecular wires, respectively. The molecular magnet compound TCNE and surface modification by means of chemisorption of TDAE on gold are also studied. Molecular crystals of pentacene are reported to have the highest field-effect mobility values for organic thin film field-effect transistors. The conduction process in field-effect transistors applications occurs in a single layer of the molecular crystal. Hence, in studies of transport properties molecular crystals of pentacene can be considered as a two dimensional system. An open question of these system is if the charge transport is bandlike or if as a result of disorder is a hopping process. We address this question in two of the included papers, paper I and paper II. The conducting properties of DNA are of interest for a broad scientific community. Biologist for understanding of oxidatively damaged DNA and physicist and the electronics community for use as a molecular wire. Some reports on the subject classifies DNA as a conductor while other report insulating behavior. The outcome of the investigations are heavily dependent on the type of DNA being studied, clearly there is a big difference between the natural and more or less random sequence in, e.g., λ-DNA and the highly ordered syntethic poly(G)-poly(C) DNA. It has been suggested that long-range correlation would yield delocalized states, i.e., bandlike transport, in natural DNA, especially in the human chromosome 22. In paper III we show that this is not the case. In general our results show that DNA containing an approximately equal amount of the four basis is an insulator in a static picture. An emerging research field is spintronics. In spintronic devices the spin of the charge carrier is as important as the charge. One can envision a device where spin alone is the carrier of information. In realizing spintronic devices, materials that are both magnetic and semiconducting are needed. Systems that exhibit both these properties are organic-based magnets. In paper IV the electronic structure of the molecular magnet compound TCNE is studied, both experimentally and theoretically. The injection of carriers from metal contacts to organic semiconductors is central to the performance of organic based devices. The interface between the metal contact and the organic material has been pointed out to be one of the device parameters that most significantly influences the device performance. This relates to the process of injection of charge carriers in to the organic material. In some contact and organic material combinations the energy barrier for charge injection can be very high. The barrier can be reduced by modify the interface dipole, this is achieved by a monolayer of adsorbed molecules at the interface. The molecule TDAE chemisorbed on gold is studied in paper V.

Submitted by (ana.araujo@ufrpe.br) on 2016-05-25T14:39:16Z No. of bitstreams: 1 Barbara Camboim Lopes de Figueiredo.pdf: 2032958 bytes, checksum: d463c6ab534a96f1ce5aac33c2dde210 (MD5) / Made available in DSpace on 2016-05-25T14:39:16Z (GMT). No. of bitstreams: 1 Barbara Camboim Lopes de Figueiredo.pdf: 2032958 bytes, checksum: d463c6ab534a96f1ce5aac33c2dde210 (MD5) Previous issue date: 2014-02-24 / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPES / The study of climate has great importance, given that a variation of climatic elements affect the economy of a certain region and life of the inhabitants. Climate variables temperature, humidity, atmospheric pressure, solar radiation, precipitation and wind can be affected by geophysical and environmental factors such as latitude, altitude, air mass, proximity to sea, sea currents and vegetation. Wind is the most complex climate element representing the natural phenomenon of turbulence, it is characterized by high temporal and spatial variability. Wind is generated by atmospheric air mass movement, and has influence on various environmental phenomena such as soil erosion, pollutant dispersal and transport of pollen and seeds. Knowing wind speed temporal and spatial distribution is crucial to evaluate the potential for generation of eolic energy. In this work we study long-term correlations in wind speed temporal series registered at twelve meteorological stations in the state of Pernambuco, Brazil. To this end we apply Multifractal Detrended Fluctuation Analysis (MF-DFA) on hourly wind speed data for the period 2008-2011. All the analyzed series exhibit multifractal properties with generalized Hurst exponents above 0.5 indicating persistent temporal dynamics for both, small and large fluctuations. We also calculate other multifractal measures Rényi exponent and singularity spectrum, and complexity parameters, position of maximum, width and asymmetry of multifractral spectrum. No correlation was detected between complexity parameters and the geographic parameters longitude, latitude and altitude of the station, except for asymmetry of multifractal spectrum: negative correlation with longitude for maximum wind speed and negative correlation with latitude for average wind speed. However for all stations the strength of multifractality (indicated by width of multifractal spectrum) is greater for maximum wind speed then for average wind speed. These results contribute to a better understanding of the nature of stochastic processes governing wind dynamics which is necessary for development of more accurate predictive models for wind speed temporal variability and diverse phenomena influenced by wind. / O estudo do clima tem grande importância visto que a variação em elementos climáticos afeta a economia de uma região e a vida das pessoas que ali habitam. As variáveis climáticas temperatura, umidade, pressão atmosférica, radiação solar, precipitação e vento podem ser influenciadas por diversos fatores, geofísicos e ambientais, tais como latitude, altitude, massas de ar, continentalidade e maritmidade, relevo e vegetação. Um dos mais complexos elementos do clima é o vento, pelo fato de representar um fenômeno natural de turbulência, caracterizado por uma grande variabilidade temporal e espacial. O vento é gerado pelo movimento das massas de ar e pode influenciar vários fenômenos ambientais como erosão do solo, dispersão de poluentes e transporte de pólen e sementes. O conhecimento da distribuição temporal e espacial da velocidade do vento é crucial para avaliação do potencial eólico de uma região. Neste trabalho estudaram-se correlações de longo alcance das séries temporais de velocidade do vento registradas em 12 estações meteorológicas durante o período de 2008 a 2011 no estado de Pernambuco aplicando-se o método Multifractal Detrended Fluctuation Analysis (MF-DFA) nas séries temporais horárias. Todas as séries analisadas mostram as propriedades multifractais com valores de expoente generalizado de Hurst acima de 0,5 indicando uma dinâmica persistente para pequenas e grande flutuações. Foram calculadas também as outras medidas multifractais, o expoente Rényi e o espectro multifractal bem como os parâmetros de complexidade: posição do máximo, largura e assimetria do espectro multifractal. Não foram encontradas correlação entre os parâmetros de complexidade e as coordenadas geográficas: longitude, latitude e altitude, exceto a medida de assimetria do espectro multifractal: correlação negativa entre a rajada e longitude e entre velocidade e latitude. Para todas estações as larguras do espectro multifractal foram maiores para a rajada que para a velocidade, indicando uma multifractalidade mais forte. Estes resultados contribuem para uma melhor compreensão da natureza dos processos estocásticos geradores da dinâmica do vento, necessária para o desenvolvimento de modelos confiáveis para predição da variabilidade temporal do vento e dos diversos fenômenos influenciados pelo mesmo.