We present results of printing solution-processable organic light emitting diodes (OLEDs) based on electrophosphorescent Ir(III) stellate polyhedral oligomeric silsesquioxane (POSS) macromolecules. The macromolecules are doped into a polymer-based ink containing a hole transporting polymer, poly(9-vinylcarbazole) (PVK) and an electron transporting material, 2-4-biphenylyl-5-4-tertbutyl-phenyl-1,3,4-oxadiazole (PBD), and the resulting ink is printed on a layer of poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS) spin-coated on indium tin oxide (ITO). An exciton-blocking layer consisting of 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline (BCP) is thermally evaporated onto the printed ink layers, followed by a LiF/Al cathode. While the photoluminescence (PL) spectrum of printed ink on glass indicates a significant contribution from the PVK:PBD exciplex, electroluminescence measurements (EL) suggest a much smaller effect of these states, which implies significant charge trapping at dopant molecular sites. Our latest experiments with devices printed on PEDOT:PSS/ITO/glass indicate that the devices exhibit high luminances (∼ 13,000 cd/m2 at 70 mA/cm2) and a fairly consistent quantum efficiency (∼ 2.5%) across a wide range of luminances. The corresponding figures for spin-coated devices are expectedly higher, with efficiencies ∼ 4.5% at similar levels of brightness. We use white light interferometry as a non-contact technique to quantify surface roughness and thickness of printed layers. Our current results thus indicate that inkjet printing of macromolecular phosphor doped polymer inks is suitable for fabrication of OLEDs with high brightness, in spite of the low glass transition temperature of some of the species. Our initial work with these devices on flexible ITO-coated plastic substrates shows devices with moderately high luminance values (∼ 2,500 cd/m2 at 35 mA/cm2). Our more recent devices show higher brightnesses (∼ 9, 600 cd/m2). We are working on the development of inkjet printing materials and processes for pure macromolecular OLEDs that are not performance and reliability limited by the presence of the PVK:PBD matrix with low glass transition temperatures. This requires the development of macromolecules that subsume all the functions of the host matrix and have high enough Tg to be usable in high concentrations needed. In conjunction with the inkjet printing technology demonstrated in this work, this has the potential to yield low-cost manufacturing of these devices.

Due to the advantages of low production cost, flexibility and low temperature fabrication, much effort has been devoted to the development of organic electronic devices such as light emitting diodes, photovoltaics and transistors. Organic thin film transistors have several important applications such as switching devices for active-matrix OLED displays, smart cards, identification tags and sensors [1-3]. However, the low carrier mobility in organic materials and the difficulty of integrating organic devices into inorganic processing procedures have hindered the development of organic transistors that are comparable to traditional transistors [4]. Much effort has been devoted to develop new organic materials with higher carrier mobility, while retaining the same conventional inorganic metal-oxide-semiconductor structures.

Lithium fluoride (LiF) has the largest band gap and the largest negative electron affinity of any solid, [5] making it a superb candidate for use in the insulating layer of transistors. Using LiF as the gate dielectric layer can facilitate the organic transistor fabrication. In this work, thin film transistors based on pentacene and PTCDI-C8 (N,N′-Dioctyl-3,4,9,10-perylenedicarboximide) as organic semiconductor layers and LiF as gate dielectrics are studied. The electrical properties of these devices have been investigated in atmospheric conditions and under variable light exposure. Output and transfer characteristics of several photo-responsive thin film transistors using different organic materials but with the same insulating layer will be presented and the increase of drain-source current upon illumination will be discussed based on the photoconduction properties of the transistor active layer.

High-resolution angle resolved ultraviolet photoelectron spectroscopy measurements were conducted on rubrene single crystals successfully through relief of the sample charging assisted by a laser illumination. Significant dispersion of the valence band was clearly resolved. The band width W and the hole effective mass mh* were estimated to be 0.4 eV and 0.7m0, respectively, along the most conductive direction. The present results strongly suggest that the transport nature in rubrene single crystals should be described in the band transport framework of a delocalized charge carrier.

Deep blue PHOLED was achieved in the simple device structure of ITO/SiTPA/SiCBP: FIr6 5 wt%/SiTAZ/Liq/Al, where active layers were silicon based inorganic/organic hybrid materials of the types, SiTPA, SiCBP, and SiTAZ for HTL, EML host, and ETL respectively. Silicon incorporation into organic framework not only provided necessary morphological stability, but also engaged enhanced charge transporting capability essential to achieve highly efficient deep blue PHOLEDs. As a result, high performance silicon based HTL, EML host, and ETL materials were developed, exhibiting high charge mobility in the range of 10−4 ∼ 10−3 cm2V−1s−1 and high triplet energy of 2.88 eV, 3.05 eV and 2.84 eV, respectively.

Even with the simple four layer device structure of PHOLEDs comprising silicon based active layers, maximum external quantum efficiency (EQE) of 17 % and CIE coordinates of (0.15, 0.22) were achieved. Moreover, an EQE of 15% was recorded at a luminance of 1000 cd m−1, which was the result of reduced efficiency roll-off due to the efficient confinement of FIr6 triplet energy by surrounding silicon based inorganic/organic hybrid materials developed in this work. Structures of inorganic/organic hybrid materials and their photo-physical properties as well as device physics for high performance deep blue PHOLEDs will be presented.

We study the optical gain for various doping concentrations in a dye doped polymer (poly-[9,9-dioctylfluorene] with 6,6'-[2,2'-octyloxy-1,1'-binaphthyl] spacer groups (BN-PFO) doped by the stilbene dye 1,4-bis[2-[4-[N,N-di[p-tolyl]amino]phenyl]vinyl-benzene] (DPAVB)). In such a guest-host-system (GHS) the occupation of the upper laser level (dopant site) is due to Förster energy transfer (FET), which strongly depends on the donor acceptor distance and hence on the concentration of the laser dye. Therefore, the doping concentration is varied over a wide range and the gain coefficients are measured at various excitation densities to analyze the stimulated emission cross section.

For the investigated GHS maximum gain coefficients up to ∼340 1/cm were found at absorbed pump energy densities of around 50 μJ/cm2. It will be shown that the stimulated emission cross section (σ = 1.8 × 10−16 cm2) is concentration independent which is quite different to a recently investigated small molecule based GHS. These effects will be discussed considering the rate and exciton diffusion constants.

The complex [Ir(ppy)2(dpbpy)][PF6] (Hppy = 2-phenylpyridine, dpbpy = 6,6'-diphenyl-2,2'-bipyridine) has been prepared and evaluated as an electroluminescent component for light-emitting electrochemical cells (LECs). The complex exhibits two intramolecular face-to-face π-stacking interactions and long-lived LECs have been constructed; the device characteristics are not significantly improved in comparison to analogous LECs with 6-phenyl-2,2'-bipyridine with only one π-stacking interaction.

Attractiveness of organic field-effect transistors are in their low-cost and easy fabrication processes as well as their mechanical flexibility, while a significant drawback has been their poorer transistor performances than those of silicon and oxide semiconductors because of lower carrier mobility in organic semiconductors. We have developed an easy MEMS-based process to fabricate three-dimensional organic transistors with metal-insulator-semiconductor structures of multiple vertical channels on plastic platforms. The design maximizes the space availability and the output current per area. The flexible three-dimensional organic transistors indeed present outstanding current of ∼ 0.5 A/cm2, which is more than sufficient for driving pixels of typical organic light-emitting diodes. High on-off ratio up to 107 is also demonstrated.

We have recently developed a flexible battery using two common, inexpensive ingredients: cellulose and salt. This lightweight, rechargeable battery uses thin pieces of paper—originating from cellulose fibers from the environmentally polluting Cladophora sp.algae—as electrodes, while a solution of sodium chloride acts as the electrolyte. Conducting polymers for battery applications have been subject to numerous investigations during the last decades. However, the functional charging rates and the cycling stabilities have so far been found to be insufficient for practical applications. These shortcomings can, at least partially, be explained by the fact that thick layers of the conducting polymers have been used to obtain sufficient capacities of the batteries. We now introduce a novel nanostructured high-surface area electrode material for energy storage applications composed of cellulose fibers of algal origin individually coated with a 50 nm thin layer of polypyrrole. Our results show the hitherto highest reported charge capacities and charging rates for an all polymer paper-based battery. The composite conductive paper material is shown to have a specific surface area of 80 m2/g and batteries based on this material can be charged with currents as high as 600 mA/cm2. The aqueous-based batteries, which are entirely based on cellulose and polypyrrole and exhibit charge capacities between 25 and 33 mAh/g or 38-50 mAh/g per weight of the active material, open up new possibilities for the production of environmentally friendly, cost efficient, up-scalable and lightweight energy storage systems.

Conducting polymers have attracted attention in many areas of materials chemistry due to their tunability and wide range of applications. We are interested in utilizing the thermo-switchable properties of precursor PPV polymers to develop capacitor dielectrics that will fail at specific temperatures due to the material irreversibly converting from an insulating to a conducting state. Here, we report the synthesis and characterization of a new halophenyl substituted PPV polymer. We show that the precursor polymer has good dielectric properties over a range of temperatures, but will fail at high temperatures due to the polymer backbone conjugating. By utilizing thermo-switchable dielectrics in capacitors, the unintentional discharge of electricity in the event of a fire or overheating could be averted, providing a fundamental safety mechanism for high-voltage electronics.

Organic conducting and semiconducting materials are promising as thermoelectric conversion materials in flexible and wearable electronics because they have large Seebeck coefficients and small thermal conductivities. Since there have been only a limited number of studies on the thermoelectricity of organic materials to date, precise evaluation of Seebeck coefficient and electrical conductivity of various organic conducting/semiconducting thin films is important to examine what kind of material is the most effectual. To carry out such experiments, a specially designed instrument for organic thin films has been developed. Its ability to measure Seebeck coefficients of highly resistive materials was confirmed and Seebeck coefficients and power factors of several typical organic functional materials were preliminary evaluated.

We will show the synthesis of new donor-acceptor copolymers based on 2,7-carbazole or 2,7-dibenzosilole and acenaphtho[1,2-b]thieno[3,4-e]pyrazine. After the synthesis of these new copolymers, we have characterized the materials by UV-vis, DSC, and XRD to determine the degree of organization. Afterward, we have fabricated and investigated field-effect transistors and photovoltaic cells from these polymers. The optimization of the thin film by thermal treatment have led to a field-effect mobility of 0.04 cm2/(V.s) and power conversion efficiency of 0.44%.

Over the past few decades, metallic nanoparticles (NPs) have been of great interest due to their unique properties which distinguish them from those of bulk metals. Many attempts have been conducted to investigate the characteristics of NPs and their applications. However, the sintering process which converts metallic NPs to conductive film was not established yet. In this study, the microstructure evolution of Au NPs after sintering under different thermal condition was examined and the film quality was studied based on densification, organic residues and electrical resistivity. Au NP ink dispersed in a toluene were spin coated on Ni-plated FCCL or Si substrates and thermally treated in a furnace under different sintering profiles under various types of flows such as air, nitrogen (N2), or reducing atmosphere of formic acid (FA). The Au ink was consisted of Au NPs coated with an organic capping molecule. The capping molecules not only help NPs to disperse but prevent aggregation and precipitation of NPs out of solution. When the NPs are treated by thermal process, the surface ligands from capping molecule start to decompose and necking and melting of NPs occur producing the film with the electrical conductivity. The diameter of Au NPs was approximately between 5-7 nm with spherical shape. The Au film sintered under air showed only necking between neighboring Au NPs without further grain growth. When Au NPs films were sintered under N2 atmosphere, NPs fused together in clusters. Under sintering with flows of FA, a larger area of pores due to the volume shrinkage of the film was observed since an agglomeration and melting of NPs were considerably progressed compared to the film sintered under N2. Sintering with a flow of a single gas such as air or N2 showed organic residues in the film indicated by C-H or C-O stretch peaks. However, when mixed flows of FA and N2 were applied, there was no IR peaks from organic substances observed in the film. It is assumed that the organic capping molecules surrounding the Au NPs were removed significantly with sintering with two flows of FA and N2. The microstructure showed less pore distribution and lower level of organic residues compared to those sintered under air, N2, or FA atmospheres. The electrical resistivity was about twice of bulk value of 2.44 μΩ -cm. Overall Au NPs film sintered under FA and N2 resulted in a better sintering effect based on densification of the film and level of residual organics, translating into a relatively high electrical conductivity.

Fluorinated carbazoles as host materials have been investigated for highly efficient organic light emitting diodes (OLEDs). By molecular orbital calculations, we found that fluorinations at position 2, 4, 5 and 7 of carbazole ring were effective for widening HOMO-LUMO energy gap. The energy gaps of our synthesized 2,7-difluorocarbazole (F2-Cz) and 2,4,5,7-tetrafluorocarbazole (F4-Cz), were estimated to be 3.71 eV and 3.87 eV by the absorption spectra, respectively. These energy gaps were higher than that of the non-substituted carbazole (Cz, 3.59 eV). We synthesized poly(N-vinyl-2,7-difluorocarbazole) (F2-PVK) and poly(N-vinyl-2,4,5,7-tetrafluorocarbazole) (F4-PVK) as solution processable polymer host materials. However, the F4-PVK was found to be an unsolved polymer. The F2-PVK could be compared with non substituted poly(N-vinylcarbazole) (PVK) in OLEDs. The emission layer (EML) contained iridium(III) bis [(4,6-di-fluorophenyl)-pyridinato-N,C2′] picolinate (FIrpic) as a blue phosphorescent dopant, and iridium(III) bis [2-(9,9-dihexylfluorenyl)-1-pyridine] acetylacetonate as a yellow dopant. The white OLED with the F2-PVK showed 1.4 times higher luminous current efficiency (24 cd/A) than the PVK (17 cd/A). These data show that the excitation energy is confined on dopants by using fluorinated polymer host material with higher T1 corresponding to wider HOMO-LUMO energy gap.