Optimizing Interfacial Energetics for Conjugated Polyelectrolyte Electron Injection Layers in High Efficiency and Fast Responding Polymer Light Emitting Diodes.

Modification of the π-conjugated backbone structure of conjugated polyelectrolytes (CPEs) for use as electron injection layers (EILs) in polymer light emitting diodes (PLEDs) has previously brought conflicted results in the literature in terms of device efficiency and turn-on response time. Herein, we determine the energetics at the CPE and the light emitting polymer (LEP) interface as a key factor for PLED device performance. By varying the conjugated backbone structure of both the LEP and CPE, we control the nature of the CPE/LEP interface in terms of optical energy gap offset, interfacial energy level offset, and location of the electron-hole recombination zone. We use a wide gap CPE with a shallow LUMO (F8im-Br) and one with a smaller gap and deeper LUMO (F8imBT-Br), in combination with three different LEPs. We find that the formation of a type II heterojunction at the CPE/LEP interfaces causes interfacial luminance quenching, which is responsible for poor efficiency in PLED devices. The effect is exacerbated with increased energy level offset from ionic rearrangement and hole accumulation occurring near the CPE/LEP interface. However, a deep CPE LUMO is found to be beneficial for fast current and luminance turn-on times of devices. This work provides important CPE molecular design rules for EIL use, offering progress toward a universal PLED-compatible CPE that can simultaneously deliver high efficiency and fast response times. In particular, engineering the LUMO position to be deep enough for fast device turn-on while avoiding the creation of a large energy level offset at the CPE/LEP interface is shown to be highly desirable.

Controlling Molecular Conformation for Highly Efficient and Stable Deep-Blue Copolymer Light-Emitting Diodes.

We report a novel approach to achieve deep-blue, high-efficiency, and long-lived solution-processed polymer light-emitting diodes (PLEDs) via a simple molecular level conformation change of an emissive conjugated polymer. We introduce rigid ß-phase segments into a 95% fluorene-5% arylamine copolymer emissive layer. The arylamine moieties at low density act as efficient exciton formation sites in PLEDs, whereas the conformational change alters the nature of the dominant luminescence from a broad, charge transfer like emission to a significantly blue-shifted and highly vibronically structured excitonic emission. As a consequence, we observe a significant improvement in the Commission International de L'Eclairage ( x, y) coordinates from (0.149, 0.175) to (0.145, 0.123) while maintaining high efficiency and improved stability. We achieve a peak luminous efficiency, η = 3.60 cd/A, and a luminous power efficiency, ηw = 2.44 lm/W, values that represent state-of-the-art performance for single copolymer deep-blue PLEDs. These values are 5-fold better than for otherwise-equivalent, ß-phase poly(9,9-dioctylfluorene) PLEDs (0.70 cd/A and 0.38 lm/W). This report represents the first demonstration of the use of molecular conformation as a simple but effective method to control the optoelectronic properties of a fluorene copolymer; previous examples have been confined to homopolymers.

High-Efficiency Polymer LEDs with Fast Response Times Fabricated via Selection of Electron-Injecting Conjugated Polyelectrolyte Backbone Structure.

Imidazolium ionic side-group-containing fluorene-based conjugated polyelectrolytes (CPEs) with different π-conjugated structures, poly[(9,9-bis(8'-(3″-methyl-1″-imidazolium)octyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)] dibromide (F8im-Br) and poly[(9,9-bis(8'-(3″-methyl-1″-imidazolium)octyl)-2,7-fluorene)-alt-(benzo(2,1,3)thiadiazol-4,8-diyl) dibromide (F8imBT-Br), are synthesized and utilized as an electron injection layer (EIL) in green-emitting F8BT polymer light-emitting diodes (PLEDs). Both CPE EIL devices significantly outperform Ca cathode devices; 17.9 cd A(-1) (at 3.8 V) and 16.6 lm W(-1) (at 3.0 V) for F8imBT-Br devices, 11.1 cd A(-1) (at 4.2 V) and 9.1 lm W(-1) (at 3.4 V) for F8im-Br devices, and 7.2 cd A(-1) (at 3.6 V) and 7.0 lm W(-1) (at 3.0 V) for Ca devices. Importantly, unlike the F8im-Br EIL devices, F8imBT-Br PLEDs exhibit much faster electroluminescence turn-on times (<10 µs) despite both EILs possessing the same tethered imidazolium and mobile bromide ions. The F8imBT-Br devices represent, to the best of our knowledge, the highest efficiency in thin (70 nm) single-layer F8BT PLEDs in conventional device architecture with the fastest EL response time using CPE EIL with mobile ions. Our results clearly indicate the importance of an additional factor of EIL materials, specifically the conjugated backbone structure, to determine the device efficiency and response times.

Bendable inorganic thin-film battery for fully flexible electronic systems.

High-performance flexible power sources have gained attention, as they enable the realization of next-generation bendable, implantable, and wearable electronic systems. Although the rechargeable lithium-ion battery (LIB) has been regarded as a strong candidate for a high-performance flexible energy source, compliant electrodes for bendable LIBs are restricted to only a few materials, and their performance has not been sufficient for them to be applied to flexible consumer electronics including rollable displays. In this paper, we present a flexible thin-film LIB developed using the universal transfer approach, which enables the realization of diverse flexible LIBs regardless of electrode chemistry. Moreover, it can form high-temperature (HT) annealed electrodes on polymer substrates for high-performance LIBs. The bendable LIB is then integrated with a flexible light-emitting diode (LED), which makes an all-in-one flexible electronic system. The outstanding battery performance is explored and well supported by finite element analysis (FEA) simulation.

In situ ligand exchange of thiol-capped CuInS2/ZnS quantum dots at growth stage without affecting luminescent characteristics.

An aliphatic thiol ligand of CuInS(2)/ZnS core/shell quantum dots is replaced with a hydroxyl-terminated thiol ligand by utilizing 'on-off state' of ligands during growth stage of the quantum dots. After the ligand-exchange, negligible differences were observed on both photoluminescence spectrum and luminescent quantum efficiency. The reason for the high retention of luminescent efficiency comes from no local agglomeration and no surface deterioration of QDs. It is also observed that 70% of initial ligands are exchanged by the replacing ligand, determined by FT-IR and (1)H NMR. The proposed method provides the quantum dots with an excellent dispersibility in polar solvents, supported by identical luminescence decay characteristics of the QDs.

Poly(3,4-ethylenedioxythiophene) Derived from Poly(ionic liquid) for the Use as Hole-Injecting Material in Organic Light-Emitting Diodes.

We report that poly(3,4-ethylenedioxythiophene) derived from poly(ionic liquid) (PEDOT:PIL) constitutes a unique polymeric hole-injecting material capable of improving device lifetime in organic light-emitting diodes (OLEDs). Imidazolium-based poly(ionic liquid)s were engineered to impart non-acidic and non-aqueous properties to PEDOT without compromising any other properties of PEDOT. A fluorescent OLED was fabricated using PEDOT:PIL as a hole-injection layer and subjected to a performance evaluation test. In comparison with a control device using a conventional PEDOT-based material, the device with PEDOT:PIL was found to achieve a significant improvement in terms of device lifetime. This improvement was attributed to a lower indium content in the PEDOT:PIL layer, which can be also interpreted as the effective protection characteristics of PEDOT:PIL for indium extraction from the electrodes.