Optoelectronic devices based on organic semiconductors have been the focus of increasing research over the past two decades. While many of the potential organic electronic concepts (solar cells, transistors, detectors etc.) are still in their infancy stage, organic light-emitting diodes have gained commercial acceptance for their potential in high resolution displays and solid-state lighting. However, in order for these devices to reach their full potential significant advances need to make to address their fundamental limitations, specifically: device life-time, thin-film encapsulation and scalability to a high volume manufacturing setting. The work presented in this thesis demonstrates new strategies to design and manufacture high-performance OLEDs for next generation electronics. In the first part, high-performance OLEDS using a simple three-layer organic semiconductor device structure are demonstrated. These devices utilize two novel materials (Poly-TriCZ and mCPSOB) to achieve efficient charge balance and exciton confinement in the emissive region of the device. Moreover, the electrical properties of these materials allow them to serve as a suitable ‘universal’ material combination to yield high-performance OLEDs with high-energy phosphors (i.e. blue- or deep-blue-emitting dopants). To demonstrate this feature, green- and blue-emitting OLED results are provided that define the state-of-the-art for phosphorescent OLEDs. These results are then extended to show high-performance with a new set of high-efficiency blue- and green-emitting dopants based on thermally activated delayed fluorescence (TADF), which also proceed to define the state-of-the-art in electroluminescence from TADF. The second part of this thesis continues this work and extends the results to a new class of polymeric substrates, called shape memory polymers (SMPs). SMPs provide a new alternative to flexible, polymeric substrates due to their unique mechanical properties. When an external stimuli is applied to these materials (heat), they have the ability to form a temporary phase that has a Young’s modulus orders of magnitude lower than its original state. The material can then be re- shaped, deformed or conform to any object until the stimuli is removed, at which point the Young’s modulus returns to its original state and the temporary geometric configuration is retained. Re-applying the stimulus will trigger a response in its molecular network, which induces a recovery of its original shape. By using mCPSOB in an inverted top-emitting OLED architecture, high performance green-emitting OLEDs are demonstrated on SMP substrates that define the state-of-the-art in performance for deformable light-emitting devices. The combination of the unique properties of SMP substrates with the light-emitting properties of OLEDs pave to the way for new class of applications, including conformable smart skin devices, minimally invasive biomedical devices, and flexible lighting/display technologies.

This thesis describes a number of studies on organic semiconductors as laser gain media with the aim of simplifying the excitation scheme and exploring potential applications. A hybrid device taking the advantage of high power inorganic light emitting diodes (LEDs) and low threshold organic distributed feedback lasers is demonstrated to realize a LED pumped organic laser. When the drive current is higher than 152 A, a sharp peak is clearly observed in the laser output spectrum, implying the LED successfully pumps the polymer laser above threshold. This is the first time an incoherent LED has been used as the excitation source for an organic semiconductor laser. A strategy for further improving the performance of the hybrid device is explored with the use of a luminescent concentrator made of a dye doped SU8 film, to intensify the power density from the inorganic LED. The luminescent concentrator is capable of increasing the incident power density by a factor of 9 and reducing the lasing threshold density by 4.5 times. As a preliminary investigation towards mode-locked polymer lasers, the impact of a solid state saturable absorber on a solution based organic semiconductor laser is explored. The dye doped polystyrene thin film saturable absorber exhibits a saturation intensity of a few MW/cm². When it is placed into the laser cavity, a train of short pulses is generated and the underlying mechanism is discussed. Finally, the potential of using organic semiconductor lasers in the detection of nitro-aromatic explosive vapours is studied in distributed feedback polyfluorene lasers. A high sensing efficiency and fast response from the laser prove polyfluorene lasers can be used as disposal and low cost devices in explosive chemosensing.

Inorganic alternating current electroluminescent devices (AC-ELs) are known for their ruggedness and extreme long-term reliability, which is why they can often been found in industrial and medical equipment as well as in applications in the military sector. In contrast to the inorganic phosphors used in AC-ELs, organic materials offer a number of advantages, in particular a significantly higher efficiency, easier processibility, and a wide selection of emitter materials spanning the entire visible spectrum. Several efforts towards alternating current driven organic light-emitting devices have recently been made, however, important operating mechanism are still not well understood. In the first part of this theses, alternating current driven, capacitively coupled, pin-based organic light-emitting devices are investigated with respect to the influence of the thickness of the insulating layer and the intrinsic organic layer on the driving voltage. A three-capacitor model is employed to predict the basic behavior of the devices and good agreement with the experimental values is found. The proposed charge regeneration mechanism based on Zener tunneling is studied in terms of field strength across the intrinsic organic layers. A remarkable consistency between the measured field strength at the onset point of light emission (3–3.1 MV/cm) and the theoretically predicted breakdown field strength of around 3 MV/cm is obtained. The latter value represents the field required for Zener tunneling in wide band gap organic materials according to Fowler-Nordheim theory. In a second step, asymmetric driving of capacitively coupled OLEDs is investigated. It is found that different voltages and/or pulse lengths for positive and negative half-cycle lead to significant improvements in terms of brightness and device efficiency. Part two of this work demonstrates a device concept for highly efficient organic light-emitting devices whose emission color can be easily adjusted from, e.g., deep-blue through cold-white and warm-white to saturated yellow. The presented approach exploits the different polarities of the positive and negative half-cycles of an alternating current driving signal to independently address a fluorescent blue emission unit and a phosphorescent yellow emission unit vertically stacked on top of each other. The electrode design is optimized for simple fabrication and driving and allows for two-terminal operation by a single source. The presented approach for color-tunable OLEDs is versatile in terms of emitter combinations and meets application requirements by providing a high device efficiency of 36.2 lm/W, a color rendering index of 82 at application relevant brightness levels of 1000 cd/m², and warm-white emission color coordinates. The final part demonstrates an approach for full-color OLED pixels that are fabricated by vertical stacking of a red-, green-, and blue-emitting unit. Each unit can be addressed separately which allows to efficiently generate every color that is a superposition of spectra of the individual emission units. The device is built in a top-emission geometrywhich is highly desirable for display fabrication as the pixel can be directly deposited onto the back-plane electronics. Furthermore, the presented device design requires only three independently addressable electrodes which simplifies fabrication and electrical driving. The electrical performance of each individual unit is on par with standard pin single emission unit OLEDs, showing very low leakage currents and achieving high brightness levels at moderate voltages of around 3–4 V.

Neste trabalho é apresentado o estudo e o desenvolvimento de um sistema eletrônico de teste, para avaliação de desempenho de diodos emissores de luz poliméricos - PLEDs, ou de mostradores de informações com até 35 PLEDs em matriz passiva produzidos em laboratório. Os requisitos de acionamento e controle, baseados nas características estruturais e elétricas de PLEDs e mostradores de PLEDs, foram cuidadosamente estudados para definição dos circuitos mais adequados para o sistema de controle. O equipamento desenvolvido permite ajustar níveis de tensão e corrente elétricas, freqüência e largura de pulso do sinal de alimentação, de forma a possibilitar variações de emissão de luz nos dispositivos acionados. O sistema foi avaliado utilizando-se um mostrador de informações de PLEDs em matriz passiva, que antes passou por caracterizações estruturais e elétricas, sendo que os resultados serviram para ajuste da região de trabalho da tensão e corrente elétricas e freqüência de alimentação. Os resultados dos testes demonstraram que o circuito projetado atende a todos os requisitos de projeto e aos objetivos para os quais foi proposto. O acionamento do mostrador de referência com o sistema desenvolvido permitiu avaliar o seu desempenho em relação à emissão de luz, analisando características como luminância, cromaticidade e radiometria, frente a variações de tensão e corrente elétricas e largura de pulso do sinal de alimentação. Estas informações permitem a criação de uma base de dados que auxiliam o pesquisador durante a avaliação de desempenho e de reprodutibilidade de PLEDs ou mostradores de PLEDs construídos em laboratório. / In this work it is presented the study and development of an electronic system of test for performance evaluation of polymer light-emitting diodes - PLEDs, or displays with up to 35 PLEDs in passive-matrix produced in laboratory. The drive and control requirements, based in structural and electric characteristics of PLEDs and PLEDs displays, carefully had been studied for definition of adequate circuits for control system. The developed equipment allows adjusting voltage and current levels, frequency and pulse width of signal power, to make possible variations of light emission in the motion devices. The system was evaluated using passive-matrix PLED display, that before passed for structural and electric characterizations, being that the results had served for voltage, current and frequency adjustment of signal power. The tests results had demonstrated that projected circuit takes care of all requirements and objectives for which was considered. The drive of reference display with the developed system allowed to performance evaluate of its light-emitting characteristics, as luminance, chromaticity and photometry, front voltage, current and pulse width variations of signal power. This information allows a database creation that assists researcher during performance evaluation and reproducibility of PLEDs or PLEDs displays produced in laboratory.

As microalgas são candidatas promissoras para a produção em larga escala de biocombustíveis devido a sua alta eficiência fotossintética. No entanto, os custos relativamente altos de produção por baixas produtividades em lipídios têm sido um dos principais obstáculos que impedem sua produção comercial. Portanto, é necessário focar a pesquisa no aumento da biomassa e na produtividade em lipídios, através do desenvolvimento de biorreatores e técnicas de cultivo inovadoras. Numa primeira fase, este estudo mostra a otimização dos regimes de adição de nutrientes no cultivo de Neochloris oleoabundans em fotobiorreatores tubulares, determinando que a melhor metodologia de adição de CO2 é adicionando-o de forma intermitente e automatizada, enquanto que o melhor processo de alimentação de nitrogênio é por meio de um processo em batelada alimentada tomando como uma referência a produtividade diária de biomassa. Na segunda etapa, foi testada a influência de agentes estressores adicionados ao cultivo sob carência de nitrogênio, tais como tiossulfato de sódio como agente redutor e cloreto de sódio e glicerina como agentes de choque osmótico, buscando um acúmulo de lipídios na biomassa. Os resultados mostraram que o tiossulfato de sódio em 1,2 mM e o cloreto de sódio em 2,2 mM aumentaram o total de lipídios em 21% e 25%, respectivamente. Finalmente, foram testados diferentes regimes de luz, com um esquema 12:12, sendo 12 horas de luz fluorescente e 12 horas com um sistema distinto: escuro, diodos emissores de luz (LED) vermelha e LED branca. Os melhores resultados foram obtidos com LED branca, com um acúmulo de lipídios de até 27% da biomassa seca e uma concentração final de células de 2335mg/L, estabelecendo assim um método de iluminação econômica com alta produtividade (145mg / L dia). / Microalgae are promising candidates for large-scale global biofuel production because of their high photosynthetic efficiency. However, relatively high production costs due to low lipid productivity have been one of the major obstacles impeding their commercial production. Therefore, it is necessary to accurate the research into an increase in biomass and oil productivity, by means of novel bioreactors\' design and cultivation techniques. On a first stage, this study shows the optimization of nutrients\' addition regimes in Neochloris oleoabundans cultivation in tubular photobioreactors, finding that the best CO2 addition methodology is an automatized intermittent adding and the best feeding process for nitrogen is a fed-batch process taking as a reference the daily biomass productivity. On the second step, it was tested the influence of stressing agents added to the culture under nitrogen starvation, such as sodium thiosulphate for reducing environment and sodium chloride and glycerol for osmotic shock, aiming lipid accumulation in the biomass. The results showed that sodium thiosulphate at 1,2mM and sodium chloride at 2,2mM raised the total lipids up to 21% and 25% respectively. Finally, there were tested different light regimes, with a scheme 12:12, being 12 hours of fluorescent light and 12 hours of a singular system: dark, red light-emitting-diodes (LED) and white LED. The best results were obtained with white LED, with an accumulation up to 27% of dry biomass and a final cell concentration up to 2335mg/L, establishing an economic illumination method with high productivity.

Gallium nitride (GaN) and its related semiconductor alloys are attracting tremendous interest for their wide range of applications in blue and green LEDs, diode lasers, high-temperature and high-power electronics. Nanomaterials such as InGaN/GaN core-shell three-dimensional nanostructures are seen as a breakthrough technology for future solid-state lighting and nano-electronics devices. In a core-shell LED, the active semiconductor layers grown around a GaN core enable control over a wide range of wavelengths and applications. In this thesis the capability for the heteroepitaxial growth of a proof-of-principle core-shell LED is advanced. A design that can be applied at the wafer scale using metalorganic vapor phase epitaxy (MOVPE) crystal growth on highly uniform GaN nanorod (NR) structures is proposed. This project demonstrates understanding over the growth constraints of active layers and dopant layers. The impact of reactor pressure and temperature on the morphology and on the incorporated InN mole fraction was studied for thick InGaN shells on the different GaN crystal facets. Mg doping and effectiveness of the p-n junction for a core-shell structure was studied by extensive growth experiments and characterization. Sapphire and Si substrates were used, and at all the stages of growth and fabrication. The structures were optimized to achieve geometry homogeneity, high-aspect-ratio, incorporation homogeneity for InN and Mg dopant. The three-dimensional nature of NRs and their light emission provided ample challenges which required adaptation of characterization and fabrication techniques for a core-shell device. Finally, an electrically contacted core-shell LED is demonstrated and characterized. Achieving a proof-of-principle core-shell device could be the starting point in the development of nanostructure-based devices and new physics, or in solving technical problems in planar LEDs, such as the polarization of emitted light, the quantum-confined Stark effect, efficiency droop, or the green gap.

As microalgas são candidatas promissoras para a produção em larga escala de biocombustíveis devido a sua alta eficiência fotossintética. No entanto, os custos relativamente altos de produção por baixas produtividades em lipídios têm sido um dos principais obstáculos que impedem sua produção comercial. Portanto, é necessário focar a pesquisa no aumento da biomassa e na produtividade em lipídios, através do desenvolvimento de biorreatores e técnicas de cultivo inovadoras. Numa primeira fase, este estudo mostra a otimização dos regimes de adição de nutrientes no cultivo de Neochloris oleoabundans em fotobiorreatores tubulares, determinando que a melhor metodologia de adição de CO2 é adicionando-o de forma intermitente e automatizada, enquanto que o melhor processo de alimentação de nitrogênio é por meio de um processo em batelada alimentada tomando como uma referência a produtividade diária de biomassa. Na segunda etapa, foi testada a influência de agentes estressores adicionados ao cultivo sob carência de nitrogênio, tais como tiossulfato de sódio como agente redutor e cloreto de sódio e glicerina como agentes de choque osmótico, buscando um acúmulo de lipídios na biomassa. Os resultados mostraram que o tiossulfato de sódio em 1,2 mM e o cloreto de sódio em 2,2 mM aumentaram o total de lipídios em 21% e 25%, respectivamente. Finalmente, foram testados diferentes regimes de luz, com um esquema 12:12, sendo 12 horas de luz fluorescente e 12 horas com um sistema distinto: escuro, diodos emissores de luz (LED) vermelha e LED branca. Os melhores resultados foram obtidos com LED branca, com um acúmulo de lipídios de até 27% da biomassa seca e uma concentração final de células de 2335mg/L, estabelecendo assim um método de iluminação econômica com alta produtividade (145mg / L dia). / Microalgae are promising candidates for large-scale global biofuel production because of their high photosynthetic efficiency. However, relatively high production costs due to low lipid productivity have been one of the major obstacles impeding their commercial production. Therefore, it is necessary to accurate the research into an increase in biomass and oil productivity, by means of novel bioreactors\' design and cultivation techniques. On a first stage, this study shows the optimization of nutrients\' addition regimes in Neochloris oleoabundans cultivation in tubular photobioreactors, finding that the best CO2 addition methodology is an automatized intermittent adding and the best feeding process for nitrogen is a fed-batch process taking as a reference the daily biomass productivity. On the second step, it was tested the influence of stressing agents added to the culture under nitrogen starvation, such as sodium thiosulphate for reducing environment and sodium chloride and glycerol for osmotic shock, aiming lipid accumulation in the biomass. The results showed that sodium thiosulphate at 1,2mM and sodium chloride at 2,2mM raised the total lipids up to 21% and 25% respectively. Finally, there were tested different light regimes, with a scheme 12:12, being 12 hours of fluorescent light and 12 hours of a singular system: dark, red light-emitting-diodes (LED) and white LED. The best results were obtained with white LED, with an accumulation up to 27% of dry biomass and a final cell concentration up to 2335mg/L, establishing an economic illumination method with high productivity.

This thesis consists of three main studies: magnetic field effects in thermally activated delayed fluorescent (TADF) organic light emitting diodes (OLEDs), magnetic field effects in bipolar and unipolar polythiophene (P3HT) devices and a study of hybrid organic/inorganic perovskite devices. Spin-dependent transport and recombination processes of spin-pair species have been detected by magnetic field effect (MFE) technique in carbon-based semi- conductor devices. Magneto-electroluminescence (MEL) and magneto-conductivity have been measured as a function of the applied magnetic field, B, in light emitting diodes. TADF materials have been used instead of simple fluorescent materials in OLEDs. We have observed very large magnetic response with TADF materials. The second study is magnetic field effects of regio-regular P3HT based OLED devices. P3HT is a well known semiconducting polymer, and its electrical properties such as magneto-conductance can be affected by an applied magnetic field. P3HT was chosen because it exhibits a sign change in magnetoresistance (MR) as the bias is increased. Unipolar and bipolar devices have been fabricated with different electrode materials to understand which model can be best to explain organic magnetoresistance effect, possibly depending on the operating regime of the device. Transport and luminescence spectroscopies were studied to isolate the different mechanisms and identify their fingerprints. The third study is on hybrid organic-inorganic perovskite devices. With the potential of achieving very high efficiencies and the very low production costs, perovskite solar cells have become commercially attractive. Scanning electron microscopy (SEM) images and absorption spectrum of the films were compared in single-step solution, two-step solution and solution-assisted vapor deposition techniques. Grain size, morphology and thickness parameters of perovskite films were studied within these techniques. Perovskite solar cells were fabricated and their efficiencies were measured.

Organic semiconductors (OSCs) have already been shown to have great potential to play an important role in the future of clean energy generation (organic solar cells) and provide energy efficient lighting (organic light-emitting diodes, OLED). Prior research has found that the light-emission efficiency of OLED is severely limited by the magnetic state (technically the spin-configuration) of the light-emission process. In this thesis, we work on the processes using external magnetic fields that can overcome these magnetic limitations. A major focus of this research is to enhance the performance of OLED, while at the same time to unravel the scientific mechanisms by which magnetic fields act on OSCs devices. Thermally activated delayed fluorescence (TADF) is a next-generation OLED emission technology which enables nearly 100% light-emission efficiency without using heavy precious metals. TADF characteristics depend on the probability of reverse intersystem crossing (RISC) from the triplet excited states (T1) to singlet excited states (S1). The conversion (T1 to S1) process depends strongly on spin dynamics, thus we predict a dramatic magnetic field effects (MFEs) in such TADF OLED devices. In subsequent experiments we observed that changes in TADF devices due to various forms of electrical stress can lead to enormous increases in magnetic field effects (MFEs) on the current (> 1400%) and electroluminescence (> 4000%). Our work provides a flexible and inexpensive pathway towards magnetic functionality and field sensitivity in current organic devices. Such OLED pave the way for novel magnetic sensitive OSCs devices with integrated optical, electronic and magnetic characteristics. Organic magnetoresistance (OMAR) has been observed to alter the current and efficiency of OLED without any ferromagnetic components. Here we utilizes slight alterations to the device properties, the addition of a radical-doped functional layer, in which the spin-relaxing effects of localized nuclear spins and electronic spins interfere, to address the assumption about the importance of the hyperfine interaction and to attempt to differentiate between the different models for OMAR. A feature where the magnitude of OMAR exhibits a plateau over a wide range of doping fraction was observed at all temperatures investigated. This phenomenon is well explained by a theory in which a single dopant spin strongly interacts, by exchange, with one of the bottleneck sites. A similar can be used to explain the efficiency increases observed in organic solar cells for certain doping fractions.

Aluminum Gallium Nitride (AlGaN) / Gallium Nitride (GaN) based deep ultraviolet (DUV) light emitting didoes (LEDs) with emission wavelengths between 200-280 nm enable key emerging technologies such as water/air purification and sterilization, covert communications and portable bio-agent detection/identification systems for homeland security, and surface and medical device sterilization. These devices produce a large amount of undesired heat due to low quantum efficiencies in converting electrical input to optical output. These low efficiencies are attributed to difficulties in the growth&doping of AlₓGa₁₋ₓN materials and UV absorbing substrates leading to excessive joule heating, which leads to device degradation and a spectral shift in the emission wavelength. With this regard, effective thermal management in these devices depends on the removal of this heat and reduction of the junction temperature. This is achieved by decreasing the package thermal resistance from junction-to-air with cost-effective solutions. The use of heat sinks, thermal interface materials, and high conductivity heat spreaders is instrumental in the reduction of the overall junction-to-air thermal resistance. This thesis work focuses on thermal modeling of flip-chip packaged deep UV LEDs to gain a better understanding of the heat propagation through these devices as well as the package parameters that have the biggest contributions to reducing the overall thermal resistance. A parametric study focusing on components of a lead frame package is presented to ascertain the thermal impacts of various package layers including contact metallizations, thermal spreading sub-mounts, and thermal interface materials. In addition the use of alternative thermal interface materials such as phase change materials and liquid metals is investigated experimentally.