Phosphorescent Organic Light-emitting Diodes Research Articles

Dimesitylborane as Electron Accepting Unit in High Performance Yellow Single-Layer Phosphorescent Organic Light Emitting Diode.

A new host material for Single-Layer Phosphorescent Organic Light-Emitting Diodes (SL-PhOLED) is reported, namely SPA-2-FDMB, using the dimesitylborane (DMB) fragment as an acceptor unit. The molecular design is constructed on the general donor-spiro-acceptor architecture, which consists of connecting, via a spiro bridge, a donor and an acceptor units in order to avoid strong interaction between them. The DMB fragment is known for many electronic applications (notably Aggregation-Induced Emission) but has not been used yet for SL-PhOLED applications. This appears particularly interesting, as the development of this simplified technology has shown that only a few electron-accepting fragments such as diphenylphosphine oxide can provide high-performance devices. Herein, the yellow-emitting SL-PhOLED using SPA-2-FDMB as host presents an External Quantum Efficiency of 8.1% (Current Efficiency of 24.9cd.A-1) with a low threshold voltage of 2.6V. As SPA-2-FDMB presents a sharp HOMO/LUMO difference, the good matching of HOMO and LUMO energy levels with the Fermi level of the electrodes is responsible for these performances. The low LUMO level of -2.61eV also appears particularly important. These performances are, to date, the highest reported for a yellow/orange-emitting SL-PhOLED and show the potential of DMB unit in the single-layer technology.

1,5‐Diazocine‐Based Diaryl Ketones: Design, Synthesis, and Optoelectronic Properties

ABSTRACTThree novel heterocyclic host based on diaryl ketone‐tethered 1,5‐diazocines were designed and synthesized for applications in phosphorescent organic light‐emitting diodes (PhOLEDs). The hosts were derived by anchoring the naphthyl ketone (TBN), anthryl ketone (TBA), and phenanthryl ketone (TBP) to the 1,5‐diazocine core. The materials were successfully characterized using spectroscopic techniques. TBN and TBP exhibited low external quantum efficiency of 1.5% and 1.9% when explored as hosts in PhOLED devices. Among the series, TBP exhibited the highest luminance of 4160 cd/m2, maximum luminance efficiency of 6.3 cd/A, and power efficiency of 3.21 lm/w, when doped with Ir(ppy)3 in PhOLED. Nevertheless to our surprise, TBA manifested the lowest device performance than other TBs as a host due to low carrier mobility caused by a highly twisted structure as deciphered from the comparative analysis of single‐crystal structure that could impede carrier transport crucial for efficient electroluminescence. The outcomes of electroluminescence were validated and explained with analysis of single‐crystal structure, and also with the aid of density functional theory.

Unveiling the ligand effects on Pt(Ⅱ) carbene complexes for rapid, efficient and narrow-spectra blue phosphorescence

Tetradentate Pt(II) complexes, comprising of benzoimidazolyl N-heterocyclic carbene (BI-NHC) coordination, have shown superior performance in blue phosphorescent organic light-emitting diodes (PhOLEDs). Here, four frame-structured complexes were synthesized to explore the intrinsic ligand effect for rapid, efficient and narrow-spectra blue phosphorescence through experimental analyses and theoretical calculations. We found carbazolylpridine (CzPy) chelating part in Pt(II) BI-NHC complexes dominates the phosphorescence with the suppression of metal-centered transition and electron-vibration coupling. Consequently, the CzPy chelated complexes (PtN-dip and PtN-dtb) achieved high luminescent efficiency, rapid radiative decay rate (kr) and narrow emission spectra. The peripheral substituent 2,6-di-iso-propylphenyl (dip) on NHC of PtN-dip constrains the molecule, significantly reducing the non-radiative decay rate (knr) and enhancing the efficiency. The 3,5-di-tert-butylphenyl (dtb) in PtN-dtb could enhances low-frequency vibration coupling that could expedite the excitons decay, resulting in higher kr and knr. This work unveils the intrinsic factors behind the ligand effects of Pt(II) BI-NHC based complexes, leading to a rapid, efficient and narrow-spectra phosphorescence.

Enhanced Emitting Dipole Orientation Based on Asymmetric Iridium(III) Complexes for Efficient Saturated-Blue Phosphorescent OLEDs.

Three novel asymmetric Ir(III) complexes have been rationally designed to optimize their emitting dipole orientations (EDO) and enhance light outcoupling in blue phosphorescent organic light-emitting diodes (OLEDs), thereby boosting their external quantum efficiency (EQE). Bulky electron-donating groups (EDGs), namely: carbazole (Cz), di-tert-butyl carbazole (tBuCz), and phenoxazine (Pxz) are incorporated into the tridentate dicarbene pincer chelate to induce high degree of packing anisotropy, simultaneously enhancing their photophysical properties. Angle-dependent photoluminescence (ADPL) measurements indicate increased horizontal transition dipole ratios of 0.89 and 0.90 for the Ir(III) complexes Cz-dfppy-CN and tBuCz-dfppy-CN, respectively. Analysis of the single crystal structure and density functional theory (DFT) calculation results revealed an inherent correlation between molecular aspect ratio and EDO. Utilizing the newly obtained emitters, the blue OLED devices demonstrated exceptional performance, achieving a maximum EQE of 30.7% at a Commission International de l'Eclairage (CIE) coordinate of (0.140, 0.148). Optical transfer matrix-based simulations confirmed a maximum outcoupling efficiency of 35% due to improved EDO. Finally, the tandem OLED and hyper-OLED devices exhibited a maximumEQE of 44.2% and 31.6%, respectively, together with good device stability. This rational molecular design provides straightforward guidelines to reach highly efficient and stable saturated blue emission.

Superbly Efficient and Stable Ultrapure Blue Phosphorescent Organic Light-Emitting Diodes with Tetradentate Pt(II) Complex with Vibration Suppression Effect.

Blue phosphorescent organic light-emitting diodes (PHOLEDs) are on the brink of commercialization for decades. However, the external quantum efficiency (EQE) and operational lifetime of PHOLEDs are not yet reached industrial standards. Here, a novel tetradentate Pt(II) emitter with a spirofluorene onto the carbazole unit that minimizes the vibration modes, corresponding to the structural relaxation during the de-excitation, called the vibration suppression effect is reported. This modification reduces the intensity of the second peak in the spectrum and Shockley-Read-Hall recombination by blocking direct hole injection into the emitter while enhancing Förster resonance energy transfer, resulting in 451h of LT50 (the time until a 50% decrease in initial luminance at 1000cdm-2) and 25.1% of the maximum EQE (EQEmax). Thanks to the vibration suppression effect, an extremely narrow full width at half a maximum of 22nm is obtained. In phosphor-sensitized thermally activated delayed fluorescent OLED, ultra-pure blue emission with Commission internationale de l'Eclairage (CIE) coordinates of (0.136, 0.096) is obtained with 28.1% of EQEmax. Furthermore, 50.3% of the EQEmax and 589h of LT70 are simultaneously recorded with the two-stack tandem PHOLED, which is the highest EQEmax among 2-tandem and bottom-emission PHOLEDs with CIEy<0.15.

Chemical reactions as a means of installing adlayers on electron transport layers

Adlayers are often placed at metal-on-organic interfaces as a common strategy to alleviate damage during metal deposition by thermal evaporation. Methods of chemically installing adlayers have been recently demonstrated on organic semiconductors that address these interfacial issues while providing many secondary benefits. Chemical installation has yet to be attempted at the cathode-electron transport layer (ETL) interface within organic light-emitting devices (OLEDs), offering a powerful option to optimize electron injection, improve surface wetting, and reduce metal penetration. Here, a reaction between TPBi (2,2′,2′’-(1,2,5-benzinetriyl)-tris(1-phenyl-1-H-benzimidazole) and propylene oxide results in a controllable 1–3 nm thick layer of propylene oxide as shown by high-resolution X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDX). The reactive addition of the adlayer at temperatures below 40℃ does not affect the morphology of the thin film and reaches a high degree of coverage within 3 h. Integration of this layer into a phosphorescent OLED does not introduce any significant negative impact on device function. This result opens up the possibility of introducing further specific functionality into the adlayer to engineer OLED performance.

Carbon Quantum Dots with Highly Efficient Bandgap Emission for Electroluminescent Light-Emitting Diodes

Carbon quantum dots (CQDs) feature bright and tunable photoluminescence, solution processability, and low toxicity, showing great potential in optoelectronics. The multicolor fluorescent CQDs were first fabricated as active layers in our lab, and then the high-performance electroluminescent warm white light-emitting diodes (LEDs) were obtained with the synthesized bright red CQDs. More significantly, through designing the triangular structure of the carbon core, fluorescent CQDs first achieved the narrow-bandwidth (∼30 nm) electroluminescent LEDs with appreciable stability, high color purity, and high luminescence performance. These results lay the foundation for the development of next-generation high performance displays based on CQDs. Here, we will report the large-scale synthesis of CQDs with near-unity photoluminescence quantum yield and the synthesis of red (625 nm) phosphorescent carbon quantum dot organic frameworks (CDOFs) with a quantum yield of up to 42.3% and realization of high-efficiency red phosphorescent electroluminescent LEDs. The LEDs based on the CDOFs exhibited a red emission with a maximum luminance of 1818 cd m−2 and an EQE of 5.6%. This work explores the possibility of a new perspective for developing high-performance CQD-based electroluminescent LEDs.References Yuxin Shi, Louzhen Fan, et al., Red Phosphorescent Carbon Quantum Dot Organic Framework-Based Electroluminescent Light-Emitting Diodes Exceeding 5% External Quantum Efficiency, Am. Chem. Soc. 2021, 143, 45, 18941–18951Ting Yuan, Louzhen Fan, et al., Carbon Quantum Dots with Near-Unity Quantum Yield Bandgap Emission for Electroluminescent Light-Emitting Diodes, Angew. Chem. Int. Ed. 2023, e202218568.Fanglong Yuan，Louzhen Fan, et al., Engineering triangular carbon quantum dots with unprecedented narrow bandwidth emission for multicolored LEDs, Nat. Commun., 2018, 9, 2249. Figure 1

A Mononuclear [PtCl(tpy)]PF6 Complex for a Yellow Emitting Solution-Processable Organic Light Emitting Diode.

We report square planar mononuclear Pt(II)-complexes of terpyridines in the form of [PtCl(L1/L2)]PF6 as phosphorescent emitters (where L1 = 4-(3-pyridine)2,2':6',2''-terpyridine and L2 = 4'-(3-pyridinyl)-4,4''-di(tert-butyl)-2,2':6'2''-terpyridine). Complex 2 showed emission at 534 nm in the DCM solution with photoluminescence quantum efficiency (ΦPL) = 14%, while in the mCBP host (5-wt % doped), the emission shifted to 584 nm with ΦPL = 37.8% and a phosphorescence lifetime (τphos) of 37.8 μs. Complex 2 in mCBP was used to fabricate a solution-processed phosphorescent organic light-emitting diode (PhOLED) which showed maximum external quantum efficiency (EQEmax) = 7.4% with yellow emission at λEL = 570 nm and exhibited a low efficiency roll-off with an EQE drop to 7.0% at 1000 cd/m2.

Novel bipolar host materials based on benzimidazole-hybridized phenanthridine for efficient red PhOLEDs

In this work, two innovative bipolar host materials, TPA-BIP and Cz-BIP, were designed and synthesized based on benzimidazole-hybridized phenanthridine (BIP) moiety as the electron transport unit. Compared to the widely used electronic transport unit benzimidazole, the BIP unit possesses a large planar rigid structure that can effectively enhance the thermal stability and the electron transfer capability of materials. Both materials exhibit good thermal stability respectively with Tg of 113 °C and 141 °C, proper HOMO/LUMO energy levels, and balance carrier transport capabilities. The red phosphorescent organic light-emitting diode prepared based on both materials achieve relatively high luminescence efficiency and relatively low efficiency roll-off. In particular, the EQEmax of the R1 device using TPA-BIP as the host material reaches 21.5 %, which is more superior than that of the conventional host material CBP (EQEmax of 9.84 %). Even at 1000 cd/m2, the device still achieves an EQE of 21.3 % with virtually no decrease. In conclusion, the results demonstrate the broad development potential of these BIP-based host materials for red PhOLEDs applications.

Spirobifluorene Trimers: High Triplet Pure Hydrocarbon Hosts for Highly Efficient Blue Phosphorescent Organic Light‐Emitting Diodes

AbstractPure aromatic hydrocarbon materials (PHCs) represent a new generation of host materials for phosphorescent OLEDs (PhOLEDs), free of heteroatoms. They reduce the molecular complexity, can be easily synthesized and are an important direction towards robust devices. As heteroatoms can be involved in bonds dissociations in operating OLEDs through exciton induced degradation processes, developing novel PHCs appear particularly relevant for the future of this technology. In the present work, we report a series of extended PHCs constructed by the assembly of three spirobifluorene fragments. The resulting positional isomers present a high triplet energy level, a wide HOMO/LUMO difference and improved thermal and morphological properties compared to previously reported PHCs. These characteristics are beneficial for the next generation of host materials for PhOLEDs and provide relevant design guidelines. When used as a host in blue‐emitting PhOLEDs, which are still the weakest link of the field, a very high EQE of 24 % and low threshold voltage of 3.56 V were obtained with a low‐efficiency roll‐off. This high performance strengthens the position of PHC strategy as an efficient alternative for OLED technology and opens the way to a more simple electronic.

Spirobifluorene Trimers: High Triplet Pure Hydrocarbon Hosts for Highly Efficient Blue Phosphorescent Organic Light-Emitting Diodes.

Pure aromatic hydrocarbon materials (PHCs) represent a new generation of host materials for phosphorescent OLEDs (PhOLEDs), free of heteroatoms. They reduce the molecular complexity, can be easily synthesized and are an important direction towards robust devices. As heteroatoms can be involved in bonds dissociations in operating OLEDs through exciton induced degradation processes, developing novel PHCs appear particularly relevant for the future of this technology. In the present work, we report a series of extended PHCs constructed by the assembly of three spirobifluorene fragments. The resulting positional isomers present a high triplet energy level, a wide HOMO/LUMO difference and improved thermal and morphological properties compared to previously reported PHCs. These characteristics are beneficial for the next generation of host materials for PhOLEDs and provide relevant design guidelines. When used as a host in blue-emitting PhOLEDs, which are still the weakest link of the field, a very high EQE of 24 % and low threshold voltage of 3.56 V were obtained with a low-efficiency roll-off. This high performance strengthens the position of PHC strategy as an efficient alternative for OLED technology and opens the way to a more simple electronic.

Improving efficiency in RGB phosphorescent and white organic light emitting diodes via donor-spiro-boron acceptor host materials

The universal host material with boron acceptor core structure is exceptionally sparse to be designed for red, green, and blue in efficient phosphorescent organic light emitting diodes (PhOLEDs) accompanying white OLEDs, possessing indistinguishable device feature. Herein, two boron acceptors spiro-host materials namely 1'-(4-(dimesitylboranyl)phenyl)-10-phenyl-10H-spiro[acridine-9,9′-fluorene] (TPA-PBM) and 1-(4-(dimesitylboranyl)phenyl)-3′,6′-dimethylspiro[fluorene-9,8′-indolo[3,2,1-de]acridine] (2MeCz-PBM) were designed and synthesized. The designed rigid donor strategy exhibited good device performance among the reported boron donor-spiro-acceptor (D-spiro-A) skeleton for organic light emitting diodes (OLEDs). In particular, we fabricate RGB three-color phosphorescent OLEDs based on TPA-PBM and 2MeCz-PBM. The red devices exhibit a maximum external quantum efficiency (EQE) of nearly 28 % (26.8 % for TPA-PBM and 27.5 % for 2MeCz-PBM), with an electroluminescence spectrum at 608 nm. The green/blue devices obtain maximum EQEs of 21.2 %/15.3 % and 21.8 % 17.3 %, for TPA-PBM and 2MeCz-PBM, respectively. Furthermore, green devices display an extremely low efficiency roll-off with decreasing 1 % and 3 % at luminance of 5000 cd m−2. Additionally, the two-color white OLED using 2MeCz-PBM exhibits EQEmax and PEmax are 24.5 % and 62.9 lm W−1 respectively, the EQE remain 23.8 % at commercial lighting brightness of 1000 cd m−2. The WOLED also shows a stable white spectrum with CIE varying range of (0.41, 0.47) to (0.39, 0.46) at 100 cd m−2 to 15000 cd m−2. All obtained results confirmed that our targeted molecules have advantage of carrier balance and efficient charge recombination, which might replace many other commercial host materials.

Effect of molecular permanent dipole moment on guest aggregation and exciton quenching in phosphorescent organic light emitting diodes.

This study explores the effect of molecular permanent dipole moment (PDM) on aggregation of guest molecules in phosphorescent host-guest organic light-emitting diodes (OLEDs). Through a combination of photoluminescence measurements, high-angle annular dark-field scanning transmission electron microscopy analysis, and an Ising model based physical vapor-deposition simulation, we show that higher PDM of tris[2-phenylpyridinato-C2,N]iridium(III) guest can actually lead to a reduced aggregation relative to tris[bis[2-(2-pyridinyl-N)phenyl-C] (acetylacetonato)iridium(III) when doped into a non-polar host 1,3,5-tris(carbazol-9-yl)benzene. This study further explores the effect of host polarity by using a polar host 3',5'-di(carbazol-9-yl)-[1,1'-biphenyl]-3,5-dicarbonitrile, and it is shown that the polar host leads to reduced guest aggregation. This study provides a comprehensive understanding of the impact of molecular PDM on OLED material efficiency and stability, providing insights for optimizing phosphorescent OLED materials.

π‐Conjugated Nanohoops: A New Generation of Curved Materials for Organic Electronics

AbstractNanohoops, cyclic association of π‐conjugated systems to form a hoop‐shaped molecule, have been widely developed in the last 15 years. Beyond the synthetic challenge, the strong interest towards these molecules arises from their radially oriented π‐orbitals, which provide singular properties to these fascinating structures. Thanks to their particular cylindrical arrangement, this new generation of curved molecules have been already used in many applications such as host–guest complexation, biosensing, bioimaging, solid‐state emission and catalysis. However, their potential in organic electronics has only started to be explored. From the first incorporation as an emitter in a fluorescent organic light emitting diode (OLED), to the recent first incorporation as a host in phosphorescent OLEDs or as charge transporter in organic field‐effect transistors and in organic photovoltaics, this field has shown important breakthroughs in recent years. These findings have revealed that curved materials can play a key role in the future and can even be more efficient than their linear counterparts. This can have important repercussions for the future of electronics. Time has now come to overview the different nanohoops used to date in electronic devices in order to stimulate the future molecular designs of functional materials based on these macrocycles.

π-Conjugated Nanohoops: A New Generation of Curved Materials for Organic Electronics.

Nanohoops, cyclic association of π-conjugated systems to form a hoop-shaped molecule, have been widely developed in the last 15 years. Beyond the synthetic challenge, the strong interest towards these molecules arises from their radially oriented π-orbitals, which provide singular properties to these fascinating structures. Thanks to their particular cylindrical arrangement, this new generation of curved molecules have been already used in many applications such as host-guest complexation, biosensing, bioimaging, solid-state emission and catalysis. However, their potential in organic electronics has only started to be explored. From the first incorporation as an emitter in a fluorescent organic light emitting diode (OLED), to the recent first incorporation as a host in phosphorescent OLEDs or as charge transporter in organic field-effect transistors and in organic photovoltaics, this field has shown important breakthroughs in recent years. These findings have revealed that curved materials can play a key role in the future and can even be more efficient than their linear counterparts. This can have important repercussions for the future of electronics. Time has now come to overview the different nanohoops used to date in electronic devices in order to stimulate the future molecular designs of functional materials based on these macrocycles.

Blue Phosphorescent Pt(II) Compound Based on Tetradentate Carbazole/2,3'-Bipyridine Ligand and Its Application in Organic Light-Emitting Diodes.

The tetradentate ligand, merging a carbazole unit with high triplet energy and dimethoxy bipyridine, renowned for its exceptional quantum efficiency in coordination with metals like Pt, is expected to demonstrate remarkable luminescent properties. However, instances of tetradentate ligands such as bipyridine-based pyridylcarbazole derivatives remain exceptionally scarce in the current literature. In this study, we developed a tetradentate ligand based on carbazole and 2,3'-bipyridine and successfully complexed it with Pt(II) ions. This novel compound (1) serves as a sky-blue phosphorescent material for use in light-emitting diodes. Based on single-crystal X-ray analysis, compound 1 has a distorted square-planar geometry with a 5/6/6 backbone around the Pt(II) core. Bright sky-blue emissions were observed at 488 and 516 nm with photoluminescent quantum yields of 34% and a luminescent lifetime of 2.6 μs. TD-DFT calculations for 1 revealed that the electronic transition was mostly attributed to the ligand-centered (LC) charge transfer transition with a small contribution from the metal-to-ligand charge transfer transition (MLCT, ~14%). A phosphorescent organic light-emitting device was successfully fabricated using this material as a dopant, along with 3'-di(9H-carbazol-9-yl)-1,1'-biphenyl (mCBP) and 9-(3'-carbazol-9-yl-5-cyano-biphenyl-3-yl)-9H-carbazole-3-carbonitrile (CNmCBPCN) as mixed hosts. A maximum quantum efficiency of 5.2% and a current efficiency of 15.5 cd/A were obtained at a doping level of 5%.

P‐206: Key factor of Device Lifetime in Exciplex Host Based Blue Phosphorescent Organic Light Emitting Diodes

In this study, we investigated the key factor of device lifetime in blue phosphorescent organic light emitting diodes (PhOLEDs) by managing hosts and dopants in the emitting layer. We manufactured four phosphorescent devices using the exciplex type mixed host and single bipolar host doped with either Pt type and Ir type phosphors. The mixed host was better than single host in the Pt emitter doped device, while it was similar to the single host in the Ir emitter doped device. Investigation of the light‐emission mechanism of the PhOLEDs revealed that the mixed host is essential in the device showing strong hole trapping behavior. The strong p‐type host in the mixed host relieves the hole trapping by the Pt phosphor, resulting in less polaron formation and polaron accumulation. As a result, the mixed host reduces triplet‐polaron annihilation and extends the device lifetime of the Pt emitter doped PhOLEDs.

Narrow-emitting pyridoimidazole functionalized N-heterocyclic carbene based tetradentate Pt(II) complexes for blue phosphorescent organic light-emitting diodes

Two novel classes of N-heterocyclic carbene (NHC) based tetradentate Pt(II) complexes possessing bulky benzyl groups and pyridoimidazole ligands were designed and synthesized to produce efficient blue phosphorescent organic light-emitting diodes (PHOLEDs). Two blue Pt(II) complexes are reported, namely, platinum (II) [2-(3-(1-(4-(tert-butyl)benzyl)-1H-imidazo [4,5-b]pyridin-3(2H)-yl)phenoxy)-9-(pyridin-2-yl)-9H-carbazole] (Pt(t-BuBnOCzPy)) and platinum (II) [3-(3-(1-benzyl-1H-imidazo [4,5-b]pyridin-3(2H)-yl)phenoxy)-9-(4-(tert-butyl)pyridin-2-yl)-9H-carbazole] (Pt(BnOCz4t-BuPy)), respectively. Notably, pyridoimidazole and bulky benzyl groups efficiently reduced steric hindrance, vibrational peaks, and intermolecular interactions. The photophysical and electrochemical properties of the two Pt(II) complexes were analytically examined experimentally and theoretically. The complexes exhibited blue electroluminescence (EL) emission at 466 nm with a small full-width half maximum (FWHM) of 26 nm and completely suppressed vibrational emission peaks. Blue PHOLEDs, at 5 wt% Pt(t-BuBnOCzPy) and Pt(BnOCz4t-BuPy) doping ratios exhibited maximum external quantum efficiencies (EQEmax) of 19 and 18.6 %, maximum power efficiencies (PEmax) of 25.5 and 24.9 cd m−2, and maximum current efficiencies (CEmax) of 24.3 and 24.3 cd m−2 with Commission International de I'Eclairage (CIEx,y) color coordinates of (0.13, 0.17) and (0.13, 0.17), respectively. These superior results suggest that the designed benzylated NHC pyridoimidazole tetradentate Pt(II) complexes provide a novel means of reducing steric hindrance and intermolecular interactions.

Unraveling the Degradation Pathways in Deep Blue Phosphorescent OLEDs Depending on Charge Dynamics: Insights from Numerical Analysis and Magneto-Electroluminescence Characterization.

To analyze the lifetime difference based on the charge dynamics in the emitting layer (EML), we applied two electron transport layers (ETLs) with significantly different electron transporting characteristics to the same EML. Even with the same EML configuration, the device lifetime increased by approximately 4-fold, from 291 h to over 1000 h of LT50 (the time taken for the luminance to decrease to 50% of its initial value of 1000 cd/m2). Although trap/detrap of holes in the dopant molecules was observed through impedance spectroscopy, we found that the most significant difference in lifetime was caused by the quantity of electron current. Surprisingly, depending on the electron transporting layer, the primary bimolecular interaction in the EML (i.e., exciton-exciton, exciton-polaron interaction) dramatically changes even in the same EML configuration, which is theoretically analyzed by the numerical fitting of transient electroluminescence data and experimentally confirmed by magneto-electroluminescence (MEL) measurements. To the best of our knowledge, for the first time, the MEL measurements are demonstrated as a tool that can be utilized to intuitively discern the dominance of bimolecular interaction with respect to the operational stability of phosphorescent organic light-emitting diodes (PhOLEDs).

Novel indolocarbazole-based bipolar host materials for fabricating green phosphorescent organic light-emitting diodes with high efficiency and low roll-off

Herein we report two novel host materials, viz., 2-(dibenzo [b,d]furan-2-yl)indolo [3,2,1-jk]carbazole (ICz-DBF) and 3-(indolo [3,2,1-jk]carbazol-2-yl)furo [2,3-b:5,4-b']dipyridine (ICz-PFP), for fabricating highly stable and efficient organic light-emitting diodes (OLEDs). Green phosphorescent OLEDs (PhOLEDs) based on ICz-DBF and ICz-PFP exhibited less efficiency roll-off than those based on 4,4′-bis(N-carbazolyl)-1,1′-biphenyl (CBP) host, and especially, the ICz-DBF-based device achieved a high external quantum efficiency (EQE) of 20.5 %. Bipolar hosts composed of indolocarbazole (ICz) exhibit strong molecular rigidity, high triplet energy, and fast electron transport properties; therefore, they act as acceptors, but dibenzofuran (DBF) and dipyridofuran (PFP) substitutions endow them with controlled electron-donating characteristics. The bipolar properties of the new host materials were demonstrated by single-carrier device analysis, confirming the effectiveness of our research strategy for developing hosts for high-quality OLEDs.