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This PDF file contains the front matter associated with SPIE Proceedings Volume 9941, including the Title Page, Copyright information, Table of Contents, Introduction (if any), and Conference Committee listing.
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Currently, the mobile display market is strongly shifting towards AMOLED technology, in order to enable curved and flexible displays. This leads to a growing demand for highly efficient OLED emitters to reduce the power consumption and increase display resolution at the same time. While highly efficient green and red OLEDs already found their place in commercial OLED-displays, the lack of efficient blue emitters is still an issue. Consequently, the active area for blue is considerably larger than for green and red pixels, to make up for the lower efficiency.
We intend to close this efficiency-gap with novel emitters based on thermally activated delayed fluorescence (TADF) technology. Compared to state-of-the-art fluorescent dopants, the efficiency of TADF-emitters is up to four times higher. At the same time, it is possible to design them in a way to maintain deep blue emission, i.e. CIE y < 0.2. These aspects are relevant to produce efficient high resolution AMOLED displays. Apart from these direct customer benefits, our TADF technology does not contain any rare elements, which allows for the fabrication of sustainable OLED technology. In this work, we highlight one of our recently developed blue TADF materials. Basic material properties as well as first device results are discussed. In a bottom-emitting device, a CIEx/CIEy coordinate of (0.16/0.17) was achieved with efficiency values close to 20% EQE.
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Organic light-emitting diodes (OLEDs) play an important role in the new generation of flat-panel displays. Conventional OLEDs employing fluorescent materials together with triplet–triplet annihilation suffer from a relatively low internal quantum efficiency (IQE) of ~62.5%. On the other hand, the IQE of OLEDs employing phosphorescent or thermally activated delayed fluorescence (TADF) materials can reach ~100%. However, these materials exhibit very broad peaks with a full-width at half-maximum (FWHM) of 70–100 nm and cannot satisfy the color-purity requirements for displays. Therefore, the latest commercial OLED displays employ blue fluorescent materials with a relatively low IQE, and efficient blue emitters with a small FWHM are highly needed. In our manuscript, we present organic molecules that exhibit ultrapure blue fluorescence based on TADF. These molecules consist of three benzene rings connected by one boron and two nitrogen atoms, which establish a rigid polycyclic framework and significant localization of the highest occupied and lowest unoccupied molecular orbitals by a multiple resonance effect. An OLED device based on the new emitter exhibits ultrapure blue emission at 467 nm with an FWHM of 28 nm, Commission Internationale de l’Eclairage (CIE) coordinates of (0.12, 0.13), and an IQE of ~100%, which represent record-setting performance for blue OLED devices.
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Here, we developed a series of pyrimidine-based TADF emitters, 2-functionalized-4,6-bis[4-(9,9-dimethyl-9,10- dihydroacridine)phenyl]pyrimidine called Ac–RPM. We introduced a phenylacridine moiety into the 4,6-position of pyrimidine core to induce a twisted structure leading to a high PLQY of ~80%, and a small singlet and triplet excited energy difference of <0.20 eV. The optimized device realized a power efficiency of 62 lm W−1, a high EQEmax of 25%, light-blue emissions with the Commission Internationale de l’Eclairage chromaticity (CIE) coordinates of (0.19, 0.37) and a low turn-on voltage of <3.0 V. Further, we investigated the strucutre–property relationship to unlock the potential of pyrimidine-based emitter. Consequently, we developed a green emitter realizing a power efficiency of over 110 lm W−1 while maintaining extremely low voltages of 2.2 V at 1 cd m−2 and 3.0 V at 1000 cd m−2 at CIE of (0.36, 0.58). Apparently, these performances exceed those of previous TADF devices and are comparable to those of their state-of-the-art phosphorescent devices.
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We describe intense and efficient deep blue (430 – 440 nm) exciplex emission from NPB/TPBi:PPh3O OLEDs where the luminous efficiency approaches 4 Cd/A and the maximal brightness exceeds 22,000 Cd/m2. Time resolved PL measurements confirm the exciplex emission from NPB:TPBi, as studied earlier by Monkman and coworkers [Adv. Mater. 25, 1455 (2013)]. However, the inclusion of PPh3O improves the OLED performance significantly. The effect of PPh3O on the EL and PL will be discussed.
The NPB/TPBi:PPh3O-based OLEDs were also studied by optically and electrically detected magnetic resonance (ODMR and EDMR, respectively). In particular, the amplitude of the negative (EL- and current-quenching) spin 1/2 resonance, previously attributed to enhanced formation of strongly EL-quenching positive bipolarons, increases as the OLEDs degrade in a dry nitrogen atmosphere. This degradation mechanism is discussed in relation to degradation induced by hot polarons that are energized by exciton annihilation.
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We hereby report the results of our direct investigation into the excited-state dynamics of thermally activated delayed fluorescence (TADF) molecules in solution using pump-probe transient absorption spectroscopy (TAS). We found that the charge-transfer (CT) state commonly stated for TADF molecules encompasses two forms: localized and delocalized CT states. A highly efficient TADF molecule, 4CzIPN [Uoyama et al., Nature, 492, 234-238 (2012)], showed both the localized and delocalized CT states, while an inefficient TADF molecule, 2CzPN, exhibited only a localized CT state. By analyzing the time profile of triplet species observed in TAS, we propose that the reverse intersystem crossing (RISC) of 4CzIPN occurs via a mutual interaction in multiple energy levels of localized neutral and CT states, and delocalized CT states.
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Detailed photophysical measurements of intramolecular charge transfer (ICT) states have been made both in solution and solid state. Temperature dependent time resolved emission, delayed emission and photoinduced absorption are used to map the energy levels involved in molecule decay, and through detailed kinetic modelling of the thermally activated processes observed, true electron exchange energies and other energy barriers of the systems determined with the real states involved in the reversed intersystem crossing mechanism elucidated.
For specific donor acceptor molecules, the CT singlet and local triplet states (of donor or acceptor) are found to be the lowest lying excited states of the molecule with very small energy barrier between them kT. In these cases the decay kinetics of the molecules become significantly different to normal molecules, and the effect of rapid recycling between CT singlet and local triplet states is observed which gives rise to the true triplet harvesting mechanism in TADF. Using a series of different TADF emitters we will show how the energy level ordering effects or does not effect TADF and how ultimate OLED performance is dictated by energy level ordering, from 5% to 22% external quantum efficiency. From this understanding, we are able to define three criterion for TADF in different molecules and these will be discussed.
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Discovering new OLED emitters requires many experiments to synthesize candidates and test performance in devices. Large scale computer simulation can greatly speed this search process but the problem remains challenging enough that brute force application of massive computing power is not enough to successfully identify novel structures. We report a successful High Throughput Virtual Screening study that leveraged a range of methods to optimize the search process. The generation of candidate structures was constrained to contain combinatorial explosion. Simulations were tuned to the specific problem and calibrated with experimental results. Experimentalists and theorists actively collaborated such that experimental feedback was regularly utilized to update and shape the computational search. Supervised machine learning methods prioritized candidate structures prior to quantum chemistry simulation to prevent wasting compute on likely poor performers. With this combination of techniques, each multiplying the strength of the search, this effort managed to navigate an area of molecular space and identify hundreds of promising OLED candidate structures. An experimentally validated selection of this set shows emitters with external quantum efficiencies as high as 22%.
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Materials with thermally activated delayed fluorescence (TADF) have recently emerged as new fluorescent emitters for highly efficient organic light-emitting diodes (OLEDs). Molecule with TADF behavior needs to have a small singlet–triplet energy difference (ΔES-T) that allows the up-conversion from nonradiative triplet state (T1) to radiative singlet state (S1) via reverse intersystem crossing (RISC) process. Generally, molecules with small ΔES-T can be obtained via carefully manipulate the degree of “intramolecular” charge transfer (ICT) between electron-donating and -accepting components, such that the electron exchange energy that contributes to ΔES-T, can be minimized. Alternatively, excited state with small ΔES-T can be feasibly realized via “intermolecular” charge transfer occurring at the interface between spatially separating donor (D) and acceptor (A) molecules. Because the exchange energy decreases as the HOMO-LUMO separation distance increases, theoretically, the intermolecular D/A charge transfer state (or exciplex) should have rather small ΔES-T, leading to efficient TADF. However, it is still a challenge to access highly efficient exciplex systems. This is mainly because exciplex formation is commonly accompanied with a large red shift of emission spectra and long radiative lifetime, which tend to diminish photoluminescence quantum yield (PLQY) as well as electroluminescence (EL) performance. Until now, exciplex-based OLEDs with external quantum efficiency (EQE) above 10% are still limited. By judicious selection of donor and acceptor, the formation of efficient exciplex can be feasibly achieved. In this conference, our recent efforts on highly efficient exciplexes using C3-symmetry triazine acceptors and various donors, and their device characteristics will be presented.
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In this talk, we will discuss recent advances in the science and engineering of organic light-emitting diodes (OLEDs). First, we will focus on materials in which light emission involves the process of thermally activated delayed fluorescence (TADF). In these materials, triplet excited states can convert into optically emissive singlet excited states by reverse intersystem crossing, allowing for nearly 100% internal quantum efficiency. This process can be used to design a new class of materials that are all organic, offering a lower cost alternative to conventional electrophosphorescent materials that contain heavy and expensive elements such as Pt and Ir. We will discuss molecular design strategies and present examples of materials that can be used as emitters or hosts in the emissive layer.
In a second part of this talk, we will review recent progress in fabricating OLEDs on shape memory polymer substrates (SMPs). SMPs are mechanically active, smart materials that can exhibit a significant drop in modulus once an external stimulus such as temperature is applied. In their rubbery state upon heating, the SMP can be easily deformed by external stresses into a temporary geometric configuration that can be retained even after the stress is removed by cooling the SMP to below the glass transition temperature. Reheating the SMP causes strain relaxation within the polymer network and induces recovery of its original shape. We will discuss how these unique mechanical properties can also be extended to a new class of OLEDs.
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In this report, several benzoylpyridine-carbazole based fluorescence materials bearing carbazolyl or 4-(t-butyl)carbazolyl groups at the ortho, meta and para carbons of the benzoyl ring, were synthesized and studied for their TADF properties. Some of these molecules show very small ΔEST < 0.05 eV and transient PL characteristics indicate that they are thermally activated delayed fluorescence (TADF) materials. In general, they show low fluorescence efficiencies in solutions, but the efficiencies increase drastically in the thin films with some reaching more than 90%. For examples, o- and m-dicarbazolyl substituted DCBPy (2,5-di(9H-carbazol-9-yl)phenyl)(pyridin-4-yl)methanone) and DTCBPy ((3,5-bis(3,6-di-tert-butyl-9H-carbazol-9-yl)phenyl)(pyridin-4-yl)methanone) in cyclohexane show fluorescence efficiencies of 14 and 36%, but in the thin films, the values increase to 88.0 and 91.4%, respectively. Based on the TDDFT calculation, the HOMOs of DCBPy and DTCBPy are mainly distributed over the two carbazolyl groups and slightly extended to the phenyl ring. The LUMOs are mostly localized on the BPy core and slightly extended to the phenyl ring. There is a small degree of spatial overlap between the HOMO and LUMO in these two molecules. The OLEDs using DCBPy and DTCBPy as dopants emit blue and green light with EQEs of 24.0 and 27.2%, respectively, and with low efficiency roll-off at practical brightness level. The crystal structure of DTCBPy reveals a substantial interaction between the ortho donor (carbazolyl) and acceptor (4-pyridylcarbonyl) unit. The interaction between donor and acceptor substituents likely plays a key role to achieve very small ΔEST with high photoluminescence. In addition to the above two compounds, we also prepared a series of different benzoylpyridine-carbazole derivatives, the results will also be reported.
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High efficiency OLEDs based on phosphorescent, thermally activated delayed fluorescent (TADF) and fluorescent emitters will be presented. We will show that EQEs over 60% is achievable if OLEDs are fabricated using organic semiconductors with the refractive indices of 1.5 and fully horizontal emitting dipoles without any extra light extracting structure. We will also show that reverse intersystem crossing RISC rate plays an important role to reduce the efficiency roll-off in efficient TADF and fluorescent OLEDs and a couple to methods will be presented to increase the RISC rate in the devices.
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A new type of organic light-emitting diode (OLED) has emerged that shows enhanced operational stability and large internal quantum efficiency approaching 100%, which is based on exciplexes in donor-acceptor (D-A) blends having thermally activated delayed fluorescence (TADF) when doped with fluorescent emitters. We have investigated magnetoelectroluminescence (MEL) and magneto-conductivity in such TADF-based OLEDs, as well as magnetophotoluminescence (MPL) in thin films based on the OLEDs active layers, with various fluorescence emitters. We found that both MEL and MPL responses are thermally activated with substantially lower activation energy compared to that in the pristine undoped D-A exciplex host blend. In addition, both MPL and MEL steeply decrease with the emitters’ concentration. This indicates the existence of a loss mechanism, whereby the triplet charge-transfer state in the D-A exciplex host blend may directly decay to the lowest, non-emissive triplet state of the additive fluorescent emitter molecules.
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The OLED is one of the key devices for realizing next-generation displays and lighting. The efficiency of OLEDs has been improved markedly by employing phosphorescent emitters. However, there are two main issues in the practical application of phosphorescent OLEDs (PHOLEDs): the relatively short operational lifetime of green/blue devices and the relatively high cost owing to the use of a costly emitter with a concentration of about 10% in the emitting layer. Here, we report on our success in resolving these issues by the utilization of thermally activated delayed fluorescent (TADF) materials as the host materials for phosphorescent emitters. Operationally stable green PHOLEDs are demonstrated by employing a TADF material as the host since the triplet excitons of the host, which are key elements in operational degradation, are transferred rapidly to the emitter following the Förster process via reverse intersystem crossing from the triplet to singlet states. In this case, the concentration of the emitter can be reduced to 1–3 wt%, similar to that in fluorescent OLEDs. Although an external quantum efficiency (EQE) of about 20% is obtained in many PHOLEDs regardless of the TADF host, the operational lifetime strongly depends on the host. Our optimized green PHOLED employing only 1 wt% phosphorescent emitter exhibits an EQE of over 20%, a small efficiency roll-off, and a long operational lifetime on the order of 10,000 h with an initial luminance of 1,000 cd/m2.
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This study investigates an organic light-emitting diode (OLED) utilizing energy transfer from an excited complex (exciplex) comprising donor and acceptor molecules to a phosphorescent dopant. An exciplex has a very small energy gap between the lowest singlet and triplet excited states (S1 and T1). Thus, both S1 and T1 energies of the exciplex can be directly transferred to the T1 of the phosphorescent dopant by adjusting the emission energy of the exciplex to the absorption-edge energy of the dopant. Such an exciplex‒triplet energy transfer (ExTET) achieves high efficiency at low drive voltage because the electrical excitation energy of the exciplex approximates the T1 energy of the dopant. Furthermore, the efficiency of the reverse intersystem crossing (RISC) of the exciplex does not affect the external quantum efficiency (EQE) of the ExTET OLED. The RISC of the exciplex is inhibited when the T1 energy of either donor or acceptor molecules is close to or lower than that of the exciplex itself. Even in this case, however, the ExTET OLED maintains its high efficiency because the T1 energy of each component of the exciplex or the T1 energy of the exciplex itself can be transferred to the dopant. We also varied the emission colors of ExTET OLEDs from sky-blue to red by introducing various phosphorescent dopants. These devices achieved high EQEs (≈30%), low drive voltages (≈3 V), and extremely long lifetimes (e.g., 1 million hours for the orange OLED) at a luminance of 1,000 cd/m2.
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Chrysene, which has a wide band gap, was selected as an emission core to develop and study new materials that emit ultra-deep-blue light with high efficiency. Six compounds introducing various side groups were designed and synthesized: 6, 12-bis(30,50-diphenylphenyl)chrysene (TP-C-TP), 6-(30,50-diphenylphenyl)-12-(3,5-diphenylbiphenyl-400-yl)chrysene (TP-C-TPB) and 6,12-bis(300,500-diphenylbiphenyl-40-yl)chrysene (TPB-C-TPB), which contained bulky aromatic si de groups; and N,N,N0 ,N0-tetraphenyl-chrysene-6,12-diamine (DPA-C-DPA), [12-(4-diphenylamino-phenyl)-chrysene-6-yl]-diphenylamine(DPA-C-TPA) and 6,12-bis[4-(diphenylamino)phenyl]chrysene (TPA-C-TPA), which contained aromatic amine groups, were designed to afford improved hole injection properties. The synthesized materials showed maxi mum absorption wavelengths at 342–402 nm in the film state and exhibited deep-blue photoluminescence (PL) emission s at 417–464 nm. The use of TP-C-TPB in a non-doped organic light emitting diode (OLED) device resulted in ultra-deep-blue emission with an external quantum efficiency (EQE) of 4.02% and Commission Internationale de L’Eclairage coo rdinates (CIE x, y) of (0.154, 0.042) through effective control of the internal conjugation length and suppression of the p –p* stacking. The use of TPA-C-TPA, which includes an aromatic amine side group, afforded an excellent EQE of 4.83 % and excellent color coordinates CIE x, y of (0.147, 0.077).
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In this article, we demonstrated an exceptional palladium complex that exhibits both phosphorescence and delayed fluorescence for use as an efficient emitter in OLEDs. Devices employing PdN3N achieved external quantum efficiencies in excess of 22% and remarkable device operational lifetime to 90% initial luminance estimated at over 30,000 h at a practical luminance of 100 cd/m2. Further tuning of the phosphorescent and delayed fluorescent emission should have a great impact in the development of efficient and stable emitters for deep blue or white OLEDs.
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Controlling the energy level alignment at the ubiquitous interfaces in modern organic light emitting diodes, i.e., organic/electrode and organic/organic, is mandatory for achieving highest performance. While for some interfaces the understanding has matured over the past years – often with the help of photoelectron spectroscopy investigations, a lack of material-overarching and general models seems to persist. In this context, it is interesting to note that photoelectron experiments reported by different groups often returned a different level alignment for a given interface, which certainly should be unsettling for device engineers. It turns out that Fermi-level pinning and its consequences for charge density re-distribution across a device stack is an overarching mechanism that should always be considered. For intrinsic organic heterojunctions of materials with moderate acceptor/donor character the electrostatic potential across the interface changes only marginally – if at all. This situation, however, can be significantly altered when at least one of the two semiconductors is Fermi-level pinned by the "effective work function" of the other one, which is established by the contact to the electrode. Consequently, device engineering has to fully take into account the effect of adding the electrodes to a device stack, otherwise correlations between assumed electronic structure and device performance remain uncertain.
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Many electron transport layer materials (ETL) employed in state of the art organic light emitting diodes (OLEDs) are known to be polar. We combine for the first time simulations and electrical characterization of OLEDs based on polar ETL, in order to understand the impact of such materials on the device operation. Depending on the orientation of the dipole orientation, simulations predict either a benefit or a disadvantage of the polar ETL for the device performance. We also show that OLEDs featuring a polar material are perfectly suited for extracting mobility activation energy and Injection barrier from the anode to the ETL.
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We investigated a correlation between lifetime and the halogen element concentration in an organic light-emitting diode (OLED) and conducted experiments and simulations to discuss degradation mechanisms due to the halogen. OELD is generally formed of high-purity materials. Since the synthesis of high-purity materials takes time and cost, quantitative understanding of the kind, amount, and influence of impurities in OLED devices is expected. The results of combustion ion chromatography show that, if the chlorine concentration in the host material is more than several parts per million, the lifetime of the device is drastically reduced. The chlorine element, which is derived from the chlorinated by-product of the host material, is found to be transferred from the chloride to other materials (e.g., an emissive dopant) according to the results of LC-MS analysis. In addition, the electron transport layer including such impurities is also found to adversely affect the lifetime. The results of TOF-SIMS analysis suggest that the dissociated chlorine element diffuse to the light-emitting layer side when the device is driven. The results of simulations (Gaussian 09) and electrochemical analyses (cyclic voltammetry and electrolysis) reveal that the halogen element is easy to dissociate from halide by excitation or reduction. The halogen element can repeat reactions with the peripheral materials by excitation or reduction and cause damages, e.g., generate radicals or further reaction products due to the radicals. The results of simulation suggest that, such compounds have low energy level and become quenchers.
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Although the electroluminescence (EL) stability of phosphorescent organic light-emitting devices (PHOLEDs) has long been known to depend on the stability of the phosphorescent guest emitter, we recently found that the host also plays an important role. More specifically, we found that interactions between excitons and polarons to result in molecular aggregation of the host material, a phenomenon that appears to play a significant role in the deterioration in efficiency with electrical aging in these devices. The question of whether it is the guest or the host that plays the more leading role in device stability becomes therefore quite relevant. In this work we present data from a comparative systematic study on various host and guest materials used in PHOLEDs. The host materials include CBP, 26DCzPPy and TAPC, and the guest materials include Ir(ppy)3, Ir(ppy)2(acac), Ir(piq)3 and FIrpic. Changes in EL and time resolved photoluminescence characteristics are used in order to understand the interplay between the host and the guest under various electrical and thermal stress conditions. Results suggest that the host plays a more dominant role in determining PHOLED stability. They also shed some light on the interplay between host and guest materials and the effect on device stability. Results from this work will be presented and analyzed.
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Organic light-emitting diodes (OLEDs) have made tremendous progress in recent years. The internal quantum efficiency was continuously improved and is nowadays close to the ideal value of unity in state-of-the-art OLEDs. However, still only a small fraction of the internally generated power can be used for lighting aspects as most of the light is captured inside the device due to low outcoupling factors of typically 25%. One promising approach to increase this limiting factor is using an anisotropic orientation of the dye molecules. In particular, horizontal orientation of transition dipole vectors (TDV) of the emitting species is a powerful tool to improve the efficiency of OLEDs.
In order to understand the underlying mechanisms for emitter orientation of heteroleptic phosphors, we compared the anisotropy factor of emissive guest/host systems prepared by thermal evaporation using different Ir-complexes incorporating coumarin and phenylpyridin based ligands. These molecules exhibit similar high permanent dipole moments and electrostatic surface potentials but differ in their molecular structure.
Interestingly, only molecules with both aromatic and aliphatic ligands show non-isotropic distributions of their TDVs when co-deposited with a matrix material. From these findings we conclude that molecular orientation of heteroleptic Ir-complexes occurs instantaneously at the surface of the growing film and is driven by chemical interactions with the surrounding media, i.e. the vacuum and the aromatic matrix side.
Furthermore, it is possible to predict the anisotropy factor for arbitrary molecular orientation with a mathematical model taking into account the geometrical distribution of the TDV on the molecules.
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Organic light emitting diodes (OLED) are today a mature techology and have reached high efficiency both in monochrome and white devices. One of the main research areas for further improvement is still the optical design which enables many new approaches to enhance efficiency and realize special emission properties. In this talk, I will review our recent work on OLED outcoupling, in particular for devices encapsulated in microcavities and patterned structures.
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Organic light-emitting diodes (OLEDs) have drawn increasing attention as the next generation displays and lighting sources. High efficiency and long lifetime are necessary for OLEDs in practical applications. In conventional OLEDs, the charge carriers are directly injected into the organic transport layers from electrodes, the injection barriers between the organic transport layers and electrodes are unavoidable due to the mismatch between the work function of metal electrode and the energy level of charge-transport layer, which greatly affects the performance of fabricated OLEDs. Furthermore, tandem OLEDs, which are fabricated by vertically connecting several individual electroluminescent (EL) units together in series via an appropriate charge generation layer (CGL) with the entire device driven by a single power source can significantly enhance current efficiency and stability, but their performance is strongly dependent on the used CGL, especially the power efficiency is difficult to enhance due to the increase of working voltage. Recently we found that organic semiconductor heterojunctions show efficient charge generation effect and as CGL, not only double the luminance and current efficiency, but also greatly improve the power efficiency, which is difficult in tandem OLEDs based on conventional CGLs. We also realized electrode-independent charge injection by using organic semiconductor heterojuncrions as injectors in OLEDs, and obtained comparable electroluminescent (EL) performance with that of conventional OLEDs. Here, we report the results of tandem OLEDs based on organic semiconductor heterojunctions as CGL and OLEDs using organic semiconductor heterojunctions as injectors, and discuss this working mechanism in detail.
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Conducting polymers, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) has been widely used as the hole injection layer (HIL) in many applications. However, in OLEDs the commonly used PEDOT:PSS has been found to have serious problems due to its inefficient holeinjection, inefficient electron-blocking, and substantial quenching of excitons close to the PEDOT:PSS. In the literature, tetrafluoroethylene-perfluoro-3,6-dioxa-4-methyl-7-octene-sulfonic acid copolymer, one of perfluorinated ionomers (PFI), was introduced into the PEDOT:PSS layer to develop a gradient work function (WF) by self-organization of the PFI. In this contribution, the self-organized gradient effect of this novel PEDOT:PSS:PFI layer were studied using multiscale analysis and dissipative particle dynamics (DPD) simulation. The DPD inter particle repulsion parameters and intramolecular bonding parameters were obtained by reverse mapping of a series of molecular dynamics simulations similar to that used in the earlier contributions. The calculated Flory-Huggins parameters indicated that the Nafion portion of the copolymer attracts PSS while the entire PFI molecule repulses PEDOT, which results in a PFI rich interface and a vertical gradient concentration distribution of PEDOT along the vertical direction of the film layer.
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Ir(III) complexes are often used as triplet emitter dopants in phosphorescent organic light-emitting diodes (PhOLEDs). Optimizing their photoluminescence quantum yields (PLQY) at room temperature and controlling the light-outcoupling is key to attain highly performant PhOLEDs.[1] This work demonstrates that the quantum chemical modelling of phosphors is a helpful tool to: i) attain quantitative predictions of their PLQY and ii) rationalize the amount of light-outcoupling. More in details, we show that the quantitative prediction of the PLQY of blue-to-green Ir(III) complexes can be derived exclusively from electronic structure calculations and the use of simplified kinetic models.[2] Within these models, only a few calculations are needed: computing the radiative rate from the emissive state and characterizing the potential energy surfaces of the temperature-dependent non-radiative deactivation channels. This approach is extremely beneficial for the in silico prescreening of promising deep blue PhOLED emissive materials. Finally, the accurate calculation of the singlet-triplet transition dipole moments provides important insights into the design of Ir(III) complexes with improved outcoupling factors.
[1] Computational insights into the photodeactivation dynamics of phosphors for OLEDs: a perspective. D. Escudero and D. Jacquemin, Dalton Trans., 2015, 44, 8346.
[2] Quantitative prediction of photoluminescence quantum yields of phosphors from first principles. D. Escudero, Chem. Sci., 2016, 7, 1262.
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Design and development of highly efficient organic and organometallic dopants is one of the central challenges in the organic light-emitting diodes (OLEDs) technology. Recent advances in the computational materials science have made it possible to apply computer-aided evaluation and screening framework directly to the design space of organic lightemitting diodes (OLEDs). In this work, we will showcase two major components of the latest in silico framework for development of organometallic phosphorescent dopants – (1) rapid screening of dopants by machine-learned quantum mechanical models and (2) phosphorescence lifetime predictions with spin-orbit coupled calculations (SOC-TDDFT). The combined work of virtual screening and evaluation would significantly widen the design space for highly efficient phosphorescent dopants with unbiased measures to evaluate performance of the materials from first principles.
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We will review the progress in modeling of charge transport in disordered organic semiconductors on various length-scales, from atomistic to macroscopic. This includes evaluation of charge transfer rates from first principles, parametrization of coarse-grained lattice and off-lattice models, and solving the master and drift-diffusion equations. Special attention is paid to linking the length-scales and improving the efficiency of the methods. All techniques will be illustrated on an amorphous organic semiconductor, DPBIC, a hole conductor and electron blocker used in state of the art organic light emitting diodes (OLEDs). The outlined multiscale scheme can be used to predict OLED properties without fitting parameters, starting from chemical structures of compounds.
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Organic light-emitting diode (OLED) devices are under widespread investigation to displace or complement inorganic optoelectronic devices for solid-state lighting and active displays. The materials in these devices are selected or designed according to their intrinsic and extrinsic electronic properties with concern for efficient charge injection and transport, and desired stability and light emission characteristics. The chemical design space for OLED materials is enormous and there is need for the development of computational approaches to help identify the most promising solutions for experimental development. In this work we will present examples of simulation approaches available to efficiently screen libraries of potential OLED materials; including first-principles prediction of key intrinsic properties, and classical simulation of amorphous morphology and stability. Also, an alternative to exhaustive computational screening is introduced based on a biomimetic evolutionary framework; evolving the molecular structure in the calculated OLED property design space.
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The achievement of organic semiconductors with both high mobility and strong fluorescence emission remains a challenge. High mobility requires molecules which pack densely and periodically, while serious fluorescence quenching typically occurs when fluorescent materials begin to aggregate (aggregation-induced quenching (AIQ)). Indeed, classical materials with strong fluorescent emission always exhibit low mobility, for example, tris(8-hydroxyquinoline) aluminium (ALQ) and phenylenevinylene-based polymers with mobility only 10-6-10-5 cm2V-1s-1, and benchmark organic semiconductors with high mobility demonstrate very weak emission, for example, rubrene exhibits a quantum yield﹤1% in crystalline state and pentacene shows very weak fluorescence in the solid state. However, organic semiconductors with high mobility and strong fluorescence are necessary for the achievement of high efficiency organic light-emitting transistors (OLETs) and electrically pumped organic lasers. Therefore, it is necessary for developing high mobility emissive organic/polymeric semiconductors towards a fast mover for the organic optoelectronic integrated devices and circuits.
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Among various laser architectures currently used to make lasers out of organic materials (distributed feedback lasers or organic vertical cavity surface-emitting lasers, ....), vertical EXTERNAL cavities have several distinctive features that enable making lasers with a high brightness, resulting from a combination of high efficiency and good beam quality, and also offer a superior flexibility to monitor the laser spectrum.
In this talk I will highlight a few recent results on external-cavity organic lasers and reveal their potential through the example of a single mode organic laser device with an ultranarrow linewidth (< pm) corresponding to coherence lengths of several meters under diode pumping (typically 2-3 orders of magnitude longer than the state-of-the-art). From the material point of view, I will also show how ink-jet printing can be successfully used in vertical external-cavity organic lasers to make thick and optical-quality films that have the potential to be easily produced with a high throughput.
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Organic solid state lasers (OSLs) based on semiconducting polymers or small molecules have seen some significant progress over the past decade. Highly efficient organic gain materials combined with high-Q resonator geometries (distributed feedback (DFB), VCSEL, etc.) have enabled OSLs, optically pumped by simple inorganic laser diodes or even LEDs. However, some fundamental goals remain to be reached, like continuous wave (cw) operation and injection lasing. I will address various loss mechanisms related to accumulated triplet excitons or long-lived polarons that in combination with the particular photo-physics of organic gain media state the dominant road-blocks on the way to reach these goals. I will discuss the recent progress in fundamental understanding of these loss processes, which now provides a solid basis for modelling, e.g. of laser dynamics. Avenues to mitigate these fundamental loss mechanisms, e.g. by alternative materials will be presented. In this regard, a class of gain materials based on organo-lead halide perovskites re-entered the scene as light emitters, recently. Enjoying a tremendous lot of attention as active material for solution processed solar cells with a 20+% efficiency, they have recently unveiled their exciting photo-physics for lasing applications. Optically pumped lasing in these materials has been achieved. I will discuss some of the unique properties that render this class of materials a promising candidate to overcome some of the limitations of “classical” organic gain media.
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Two of the most successful microresonator concepts are the vertical cavity surface emitting laser (VCSEL), comprising a vertical cavity of highly reflective DBRs sandwiching an active layer, and the distributed feedback (DFB) laser, where a periodic optical grating selects laser modes from an active waveguide (WG) layer. Here, an organic microcavity is coupled with in-plane periodic photonic wires or dots to facilitate a coherent interaction between waveguided and vertically emitting modes as well as creating an additional in-plane confinement. The vertical positioning of such patterning plays a crucial role in the observable features. While embedding metallic or dielectric wires directly in the cavity layer leads to a strong lateral confinement as well as the observation of photonic Bloch states [1,2], the deposition of the full VCSEL stack on top of a periodic grating reveals novel features. In such a device, we demonstrate the coherent coupling between parabolic VCSEL and linear WG modes in the angle-resolved far field emission. In this system, lasing occurs not only at the VCSEL parabola apex but also at points of hybridization, when the dispersion of modes cross, showing a drastically enhanced in-plane coherence [3]. The coherent coupling of two conceptually different devices with perpendicular propagation directions paired with the macroscopic coherence facilitate a multitude of new applications.
[1] Adv. Opt. Mater. 2(8), 746 (2014)
[2] Phys. Rev. Appl. 3, 064016 (2015).
[3] Adv. Opt. Mater. under review (2016).
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Since the discovery of organic solid-state lasers, great efforts have been devoted to the development of continuous-wave (cw) lasing in organic materials. However, the operation of organic solid-state lasers under optical cw excitation or pulse excitation at a very high repetition rate (quasi-cw excitation) is extremely challenging. In this work, we have demonstrated quasi-continuous-wave (quasi-cw) surface-emitting lasing in a distributed feedback device which combines a second-order grating with an organic thin film of a host material 4,4’-bis(N-carbazolyl)-1,1’-biphenyl (CBP) blended with an organic laser dye 4,4’-bis[(N-carbazole)styryl]biphenyl (BSBCz). When pumping the device with optical picosecond pulse excitation, the quasi-cw laser operation maintained up to a repetition rate of 8 MHz. The lasing threshold was around 0.25 J cm−2 which was almost independent of the repetition rates. For our laser devices, the maximum repetition rate (8 MHz) is the highest ever reported, and the lasing threshold (0.25 J cm−2) is the lowest ever reported. These superior quasi-cw lasing characteristics in BSBCz are accomplished by the less generation of triplet excitons via intersystem crossing because a photoluminescence quantum yield of the blend film is nearly 100% and there is no significant spectral overlap between laser and triplet absorption.[1,2] Triplet quenchers, generally used for the fabrication of organic thin-film lasers, were not necessary in our devices because of negligible accumulation of triplet excitons and a small spectral overlap between emission and triplet absorption. Therefore, we believe that BSBCz is the most promising candidate for the first realization of electrically pumped organic laser diodes in terms of optical characteristics. However, electrical characteristics such as charge carrier mobility, charge carrier capture cross section, etc., are also extremely important and will need further investigation and enhancement for realization of electrically pumped organic lasers.
1. Aimono, T.; Kawamura, Y.; Goushi, K.; Yamamoto, H.; Sasabe, H.; Adachi, C. Appl. Phys. Lett. 2005, 86, 071110–071112.
2. Nakanotani, H.; Adachi, C.; Watanabe, S.; Katoh, R. Appl. Phys. Lett. 2007, 90, 231109.
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Metal film is an essential part of the electrically pumped organic semiconductor lasers. But the large loss is the most important factor restricting the electrical pumping. In this paper, we investigate optically pumped amplified spontaneous emission (ASE) in the presence of metal films. The ASE threshold of device with metallic film is reduced by 2.5 times in comparison with that of the metal-free devices. The SiO2 space layer with optimizing thickness between gain media and metal film can effectively prevent absorption loss but also provides a proper waveguide effect. Furthermore, the metal film can prevent the light leaking to the substrate and reflect the lights back into the media, which increases the intensity of pumping and emission again.
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The development of Organic Light Emitting Diode (OLED), using an optically transparent substrate material and organic semiconductor materials, has been widely utilized by the electronic industry when producing new technological products. The OLED are the base Poly(3,4-ethylenedioxythiophene), PEDOT, Poly(p-phenylenevinylene), PPV, and Polyaniline, PANI, were deposited in Indium Tin Oxide, ITO, and characterized by UV-Visible Spectroscopy (UV-Vis), Optical Parameters (OP) and Scanning Electron Microscopy (SEM). In addition, the thin film obtained by the deposition of PANI, prepared in perchloric acid solution, was identified through PANI-X1. The result obtained by UV-Vis has demonstrated that the PET/ITO/PEDOT/PPV/PANI-X1/Al layer does not have displacement of absorption for wavelengths greaters after spin-coating and electrodeposition. Thus, the spectral irradiance of the OLED informed the irradiance of 100 W/m2, and this result, compared with the standard Light Emitting Diode (LED), has indicated that the OLED has higher irradiance. After 1200 hours of electrical OLED tests, the appearance of nanoparticles visible for images by SEM, to the migration process of organic semiconductor materials, was present, then. Still, similar to the phenomenon of electromigration observed in connections and interconnections of microelectronic devices, the results have revealed a new mechanism of migration, which raises the passage of electric current in OLED.
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Electrical doping is an important method in organic electronics to enhance device efficiency by controlling Fermi level, increasing conductivity, and reducing injection barrier from electrode. To understand the charge generation process of dopant in doped organic semiconductors, it is important to analyze the charge transfer complex (CTC) formation and dissociation into free charge carrier. In this paper, we correlate charge generation efficiency with the CTC formation and dissociation efficiency of n-dopant in organic semiconductors (OSs). The CTC formation efficiency of Rb2CO3 linearly decreases from 82.8% to 47.0% as the doping concentration increases from 2.5 mol% to 20 mol%. The CTC formation efficiency and its linear decrease with doping concentration are analytically correlated with the concentration-dependent size and number of dopant agglomerates by introducing the degree of reduced CTC formation. Lastly, the behavior of dissociation efficiency is discussed based on the picture of the statistical semiconductor theory and the frontier orbital hybridization model.
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We have fabricated blue organic light-emitting devices (OLEDs) with higher color purity and stability by optimizing the structure of the Glass/ITO/NPB(50 nm)/ BCzVBi (30 nm)/ TPBi (x nm)/Alq3(20 nm)/LiF/Al. The results show that the introducing of hole blocking layer(HBL) TPBi greatly can improve not only the color purity but the color stability, which owe to its higher the Highest Occupied Molecular Orbital (HOMO) energy levels of 6.2 eV. We expect our work will be useful to optimizing the blue OLEDs structure to enhancing the color property.
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Recently, many studies have been conducted to improve the electroluminescence (EL) performance of organic lightemitting diodes (OLEDs) by using appropriate organic or inorganic materials as charge generation layer (CGL) for their application such as full color displays, backlight units, and general lighting source. In a stacked tandem white organic light-emitting diodes (WOLEDs), a few emitting units are electrically interconnected by a CGL, which plays the role of generating charge carriers, and then facilitate the injection of it into adjacent emitting units. In the present study, twostacked WOLEDs were fabricated by using tungsten oxide (WO3) as inorganic charge generation layer and 1,4,5,8,9,11- hexaazatriphenylene hexacarbonitrile (HAT-CN) as organic charge generation layer (P-CGL). Organic P-CGL materials were used due to their ease of use in OLED fabrication as compared to their inorganic counterparts. To obtain high efficiency, we demonstrate two-stacked tandem WOLEDs as follows: ITO/HIL/HTL/HTL′/B-EML/ETL/N-CGL/P-CGL (WO3 or HAT-CN)/HTL″/YG-EML/ETL/LiF/Al. The tandem devices with blue- and yellow-green emitting layers were sensitive to the thickness of an adjacent layer, hole transporting layer for the YG emitting layer. The WOLEDs containing the WO3 as charge generation layer reach a higher power efficiency of 19.1 lm/W and the current efficiency of 51.2 cd/A with the white color coordinate of (0.316, 0.318) than the power efficiency of 13.9 lm/W, and the current efficiency of 43.7 cd/A for organic CGL, HAT-CN at 10 mA/cm2, respectively. This performance with inserting WO3 as CGL exhibited the highest performance with excellent CIE color coordinates in the two-stacked tandem OLEDs.
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The feasibility of applying a five-inch diagonal white organic light-emitting diode (WOLED) as a desk lamp was experimentally investigated by quantitatively comparing its two-dimensional (2D) optical intensity profile to that of a traditional 3M desk lamp equipped with optical diffuser. The 2D optical distribution patterns as the function of vertical distances to a surface of a five-inch diagonal WOLED were obtained by using rapid rotating measurement technique consisted of a sample holder on a rotational stage and a fixed photo detector with optical power meter. The 2D optical intensity profile on a surface can be rapidly established in a relatively small space by recording the reading from the fixed photo detector as rotating the sample holder. This rapid measurement technique is suitable for practical application in quality engineering without larger space. A WOLED is a compact and thin lighting source with planar device structure without additional optical components. Its optical intensity profile on a plane is expected to be different from traditional lighting sources. The optical distribution pattern of a desk lamp requires a relatively large area on a surface with relatively uniformed intensity distribution. The quantitative analysis of the similarity between WOLED and 3M desk lamp was conducted by comparing the optimal zones defined as the area within 75% of the maximum intensity in 2D optical distribution pattern. Our preliminary result showed that the optimal zone of a five-inch diagonal WOLED at 45cm vertical distance is highly similar to that of the 3M desk lamp with optical diffuser.
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In this study, we demonstrate a blue OLED with the EQE of 34% and power efficiency of 79.6 lm W-1 using low refractive index electron transporting layer which are the highest efficiencies ever reported in blue OLEDs. In addition, we quantitatively calculated maximum achievable outcoupling efficiencies according to change of refractive indices, which can be used to estimate the achievable outcoupling efficiency of OLEDs without fabrication. The simulation indicates that EQE over 60% can be achievable in PhOLEDs if refractive indices of consisting organic materials’ are close to 1.5.
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In this paper, we will discuss the characteristics of the flexible sandwich electrode. We fabricate the MoO3/Ag grids/MoO3 via thermal deposition method. We will measure the bending test and the optical and electric characteristics. The conclusion of the MoO3/Ag grids/MoO3 will compare with the MoO3/Ag film/MoO3 and ITO flexible electrodes. This sandwich electrode will increase the transmittance by less silver coverage but the MoO3/Ag grids/MoO3 have lower sheet resistance compared with MoO3/Ag film/MoO3. Therefore, we propose this new electrode structure is proper for application of OLEDs.
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Organic p-i-n diodes enable the development of highly efficient organic devices such as organic light-emitting diodes. Understanding charge carrier trapping in these diodes is essential to comprehensively describe their electrical behaviors and increase their efficiency further. Here, a new bias stress protocol is developed to study charge trapping and the influence of trapping on molecular doping in organic p-i-n diodes. The results are discussed with the help of a novel analytical model, which is capable of quantifying the density of trapped charges and the doping efficiency from capacitance spectroscopy. We propose that this combined experimental/modeling approach is versatile and can lead to an advanced understanding of trapping in organic electronic devices.
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In this study, the efficiency of organic light-emitting diodes (OLEDs) was enhanced by depositing a CeF3 film as an ultra-thin buffer layer between the ITO and NPB hole transport layer, with the structure configuration ITO/CeF3 (1 nm)/NPB (40 nm)/Alq3 (60 nm)/LiF (1 nm)/Al (150 nm). The enhancement mechanism was systematically investigated via several approaches. The work function increased from 4.8 eV (standard ITO electrode) to 5.2 eV (1-nm-thick UV-ozone treated CeF3 film deposited on the ITO electrode). The turn-on voltage decreased from 4.2 V to 4.0 V at 1 mA/cm2, the luminance increased from 7588 cd/m2 to 10820 cd/m2, and the current efficiency increased from 3.2 cd/A to 3.5 cd/A when the 1-nm-thick UV-ozone treated CeF3 film was inserted into the OLEDs.
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OLEDs(Organic Light Emitting Diodes) has been applied to lighting and display fields. OLEDs has many advantages such as no viewing angle and fast reaction rate and so on. However, OLEDs still has low brightening issue in lighting field. This research fabricates a simple and fast production line, to produce light extraction film of the OLED. Microparticles in light extraction film were provided to enhance light luminance efficiency of the OLED up to 90%. A simple and fast production line was designed and fabricated by mechanical processing mode. It can produce 20 pieces light extraction films within 1hour.
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We report a newly developed deep-blue phosphorescent iridium complex exhibiting a narrow emission spectrum. The use of this complex resulted in a deep-blue organic light-emitting diode (OLED) with an external quantum efficiency (EQE) exceeding 30%. Two iridium complexes with a 4H-1,2,4-triazole ligand which has an adamantyl group at the 4-position were synthesized, with the resulting effects of the adamantyl group on photoluminescence (PL) behavior investigated. [Ir(Adm1)3] having a 1-adamantyl group did not exhibit any emissions at room temperature, whereas [Ir(Adm2)3] having a 2-adamantyl group exhibited a blue emission with a peak wavelength of 459 nm and a high PL quantum yield of 0.94. Structural transformations between the ground state and excited state were estimated by molecular orbital calculations, which suggests that [Ir(Adm1)3] undergoes a considerably more extensive change than [Ir(Adm2)3]. It is therefore probable that [Ir(Adm1)3] ultimately experiences thermal deactivation owing to structural relaxation. Furthermore, an OLED was fabricated using [Ir(Adm2)3] as a dopant. The associated electroluminescence spectrum had an emission peak at 457 nm and a relatively small shoulder peak at 485 nm, which are consistent with the PL spectrum. A narrowed emission spectrum with a full width at half maximum of 58 nm was obtained, leading to a deep-blue emission with high color purity (CIE, x = 0.15, y = 0.22). This device ultimately exhibited an extremely high EQE of 32% at 2 mA/cm2, which was likely attributable to an increase in outcoupling efficiency via molecular orientation.
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In this study, direct and inverted OLEDs (iOLEDs) were fabricated by using the polymer Super Yellow (SY) as the emissive material. By adding a 5 nm-thick layer of polyethylenimine ethoxylated (PEIE) on top of ITO/ZnO (indium tin oxide/zinc oxide) in the iOLEDs, its cathode work function was reduced of 1 eV. A thin layer of 1,3,5-tris(Nphenylbenzimidazol- 2-yl)benzene (TPBi) was further added by wet-process in the iOLEDs, blocking the holes at the PEIE/SuperYellow interface, so that the iOLEDs could finally reach much higher luminance compared to the direct OLEDs, maximum 40 000 cd/m2, with a constant maximum efficiency of 15 cd/A (13 cd/A maximum for the direct OLEDs). Temperature dependent transient electroluminescence measurements were conducted in order to compare charge carriers mobilities and disorder in direct OLEDs and iOLEDs. It was shown that the holes mobilities are higher for direct OLEDs (4 10-6 cm²/(V.s)) than iOLEDs (1.5 10-6 cm²/(V.s)) while the width of the distribution of energy states (DOS), σ, and the positional disorder parameter, Σ, are comparable for both structures.
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The scientific community and some sectors of industry have been working with organic dyes for successful applications in OLED´s, OSC´s, however, most of the used dyes and pigments are synthetic. In this work is investigated the use of natural dyes for its application in organic light emitting diodes, some of the studied species are chili, blackberry, guayacan flower, cochinilla, tree tomato, capuli, etc. In this study the dyes are deposited by direct deposition and SOL-GEL process doped with the natural organic dye, both methods show good performance and lower fabrication costs for dye extraction, this represents a new alternative for the fabrication of OLED devices with low requirements in technology. Most representative results are presented for Dactylopius Coccus Costa (cochinilla) and raphanus sativus´ skin.
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