Novel Ir(III) Complexes with NHC-Based Ancillary Ligands for Efficient Nondoped OLEDs.

Nondoped organic light-emitting diodes (OLEDs) are of paramount importance for display and lighting applications owing to their advantages of facile fabrication and outstanding stability. However, nondoped OLEDs achieving extraordinary electroluminescence (EL) performance and low turn-on voltage (Von) remain sparse. Here, three Ir(III) complexes featuring N-heterocyclic carbene (NHC) auxiliary ligands functionalized with electron-deficient aromatic sulfonyl or phosphine oxide groups are reported as promising emitters for nondoped OLEDs. All Ir(III) complexes exhibit green emission with relatively high neat film efficiency. Although the photoluminescence spectra of three complexes reveal similarities, there are distinct differences in the nondoped EL performance. The nondoped device N3 based on tBu-Ir-ISO displays the most eminent EL performances and presents a low Von of 2.1 V, a power efficiency of 30.7 lm W-1, and a maximum current efficiency of 27.0 cd A-1, which can be attributed to steric hindrance and balanced carrier-transporting ability induced by electron-deficient substituents. Moreover, doped devices D1-D3 also realize excellent EL performance. It is believed that the strategy reported herein is a simple and efficient way of constructing excellent Ir(III) complexes for nondoped phosphorescent OLEDs.

Centimeter-scale hole diffusion and its application in organic light-emitting diodes.

In conventional organic light-emitting diodes (OLEDs), current balance between electron and hole transport regions is typically achieved by leakage of the major carrier through the devices or by accumulation of the major carrier inside the devices. Both of these are known to reduce performances leading to reduction of efficiency and operation stability due to exciton-polaron annihilation, etc. We found that hole diffusion in a centimeter-scale can be achieved in a PEDOT:PSS layer via composition and interface engineering. This ultralong distance hole diffusion enables substantially enhanced hole diffusion current in the lateral direction perpendicular to the applied electric field in typical organic optoelectronic devices. By introducing this lateral hole diffusion layer (LHDL) at the anode side of OLEDs, reduced carrier accumulation, improved efficiency, and enhanced operation stability are demonstrated. The application of the LHDL provides a third strategy for current balancing with much reduced harmful effects from the previous two approaches.

Rational Design of Ir(III) Phosphors to Strategically Manage Charge Recombination for High-Performance White Organic Light-Emitting Diodes.

Constructing high-quality white organic light-emitting diodes (WOLEDs) remains a big challenge because of high demands on the electroluminescence (EL) performance including high efficiency, excellent spectral stability, and low roll-off simultaneously. To achieve effective energy transfer and trap-assisted recombination in the emissive layer, herein, four Ir(III) phosphors, namely, mOMe-Ir-PI (1), pOMe-Ir-PI (2), mOMe-Ir-PB (3), and pOMe-Ir-PB (4), were strategically designed via simple regulation of the substituent moiety and π conjugation of the chelated ligands. Their photophysical and EL properties were systematically investigated. When these phosphors are employed as doped emitters, the monochromic green organic light-emitting diodes not only exhibit a superior performance with the characteristics of 50.2 cd A-1, 39.2 lm W-1, and 15.1%, but also maintain a negligible roll-off ratio of 0.2% at 1000 cd m-2, which are better than those of commercial green Ir(ppy)2acac and Ir(ppy)3 in the same device configuration. Inspired by these outstanding performances, we successfully fabricated the warm WOLED utilizing 2 as a green component, affording a peak efficiency of 42.0 cd A-1, 29.3 lm W-1, and 18.6% and retaining at 39.9 cd A-1, 23.7 lm W-1, and 17.4% even at 1000 cd m-2. The results herein demonstrate the superiority of the molecular design and propose a simple method toward the development of promising Ir(III) phosphors for high-efficiency WOLEDs.

Air-Stable Ultrabright Inverted Organic Light-Emitting Devices with Metal Ion-Chelated Polymer Injection Layer.

Here, this work presents an air-stable ultrabright inverted organic light-emitting device (OLED) by using zinc ion-chelated polyethylenimine (PEI) as electron injection layer. The zinc chelation is demonstrated to increase the conductivity of the PEI by three orders of magnitude and passivate the polar amine groups. With these physicochemical properties, the inverted OLED shows a record-high external quantum efficiency of 10.0% at a high brightness of 45,610 cd m-2 and can deliver a maximum brightness of 121,865 cd m-2. Besides, the inverted OLED is also demonstrated to possess an excellent air stability (humidity, 35%) with a half-brightness operating time of 541 h @ 1000 cd m-2 without any protection nor encapsulation.

Top-emitting thermally activated delayed fluorescence organic light-emitting devices with weak light-matter coupling.

Resonance interaction between a molecular transition and a confined electromagnetic field can lead to weak or strong light-matter coupling. Considering the substantial exciton-phonon coupling in thermally activated delayed fluorescence (TADF) materials, it is thus interesting to explore whether weak light-matter coupling can be used to redistribute optical density of states and to change the rate of radiative decay. Here, we demonstrate that the emission distribution of TADF emitters can be reshaped and narrowed in a top-emitting organic light-emitting device (OLED) with a weakly coupled microcavity. The Purcell effect of weak microcavity is found to be different for TADF emitters with different molecular orientations. We demonstrate that radiative rates of the TADF emitters with vertical orientation can be substantial increased in weakly coupled organic microcavity. These observations can enhance external quantum efficiencies, reduce efficiency roll-off, and improve color-purities of TADF OLEDs, especially for emitters without highly horizontal orientation.

Retraction: Sublimable cationic Ir(iii) phosphor using chlorine as a counterion for high-performance monochromatic and white OLEDs.

Retraction of 'Sublimable cationic Ir(iii) phosphor using chlorine as a counterion for high-performance monochromatic and white OLEDs' by Lei Ding et al., Chem. Commun., 2018, 54, 11761-11764.

Sublimable cationic Ir(iii) phosphor using chlorine as a counterion for high-performance monochromatic and white OLEDs.

Different from the previous design strategy, herein, a cationic Ir(iii) complex ([(ptbi)2Ir(bisq)]Cl) with a small chlorine as the counterion was synthesized, which realized the formation of a solid film via a vacuum-deposition process. The white OLED, employing it as an orange-emitting layer, achieved excellent performances with a brightness of 50 122 cd m-2, a CE of 25.5 cd A-1, an EQE of 13.1%, accompanied by a low CE efficiency roll-off of 4.7%. These are the best results among evaporated cationic Ir(iii)-based white OLEDs reported so far.

Molecular Engineering of Phenylbenzimidazole-Based Orange Ir(III) Phosphors toward High-Performance White OLEDs.

To develop B-O complementary-color white organic light-emitting diodes (WOLEDs) exhibiting high efficiency and low roll-off as well as color stability simultaneously, we have designed two orange iridium(III) complexes by simply controlling the position of the methoxyl group on the cyclometalated ligand. The obtained emitters mOMe-Ir-BQ and pOMe-Ir-BQ show good photophysical and electrochemical stabilities with a broadened full width at half-maximum close to 100 nm. The corresponding devices realize highly efficient electrophosphorescence with a maximum current efficiency (CE) and power efficiency (PE) of 24.4 cd A-1 and 15.3 lm W-1 at a high doping concentration of 15 wt %. Furthermore, the complementary-color all-phosphor WOLEDs based on these phosphors exhibit good performance with a maximum CE of 31.8 cd A-1, PE of 25.0 lm W-1, and external quantum efficiency of 15.5%. Particularly, the efficiency of this device is still as high as 29.3 cd A-1 and 14.2% at the practical brightness level of 1000 cd m-2, giving a small roll-off. Meanwhile, extremely high color stability is achieved by these devices with insignificant chromaticity variation.

Achieving High Performances of Nondoped OLEDs Using Carbazole and Diphenylphosphoryl-Functionalized Ir(III) Complexes as Active Components.

Nondoped electroluminescent devices offer advantages over their doped counterparts such as good reproducibility, reduced phase separation between host and guest materials, and potential of lower-cost devices. However, low luminance efficiencies and significant roll-off values are longstanding issues for nondoped devices, and a rational design strategy for the preparation of efficient phosphors is highly desired. In this work, cyclometalated Ir(III) complexes 3CzIr(mtpy), 4CzIr(mtpy), 3POIr(mtpy), and 4POIr(mtpy) bearing carbazole (Cz) or diphenylphosphoryl (Ph2PO) groups substituted at different positions of 1,2-diphenyl-H-benzimidazole (HPBI) were designed and synthesized. Owing to the steric effects induced by these groups, a significant intermolecular interaction was avoided, thereby reducing self-quenching and triplet-triplet annihilation (TTA) at high brightness. Simultaneously, attached functional moieties manipulate the charge-carrier character and enhance the EL performance of the complexes. Device N3-10, based on 3POIr(mtpy), successfully realized excellent performance and improved efficiency stability, rendering a turn-on voltage of 2.5 V, a maximum current efficiency of 29.7 cd A-1, and a maximum power efficiency of 31.1 lm W-1, which are all almost 3-fold higher than that of the control device N-10 based on parent complex. Inspiringly, all of the devices showed reduced efficiency roll-off as luminance increased. To the best of our knowledge, these are good results for green-emitting PHOLEDs using vacuum evaporation techniques, and they provide fundamental insights into the future realization of efficient phosphorescent Ir(III) complexes and corresponding nondoped devices.