A DCM‐Type Red‐Fluorescent Dopant for High‐Performance Organic Electroluminescent Devices

2‐(2‐tert‐Butyl‐6‐((E)‐2‐(2,6,6‐trimethyl‐2,4,5,6‐tetrahydro‐1H‐pyrrolo[3,2,1‐ij]quinolin‐8‐yl)vinyl)‐4H‐pyran‐4‐ylidene)malononitrile (DCQTB) is designed and synthesized in high yield for application as the red‐light‐emitting dopant in organic light‐emitting diodes (OLEDs). Compared with 4‐(dicyanomethylene)‐2‐tert‐butyl‐6‐(1,1,7,7,‐tetramethyljulolidyl‐9‐enyl)‐4H‐pyran (DCJTB), one of the most efficient red‐emitting dopants, DCQTB exhibits red‐shifted fluorescence but blue‐shifted absorption. The unique characteristics of DCQTB with respect to DCJTB are utilized to achieve a red OLED with improved color purity and luminous efficiency. As a result, the device that uses DCQTB as dopant, with the configuration: indium tin oxide (ITO)/N,N′‐bis(1‐naphthyl)‐N,N′‐diphenyl‐1,1′‐biphenyl‐4,4′‐diamine (NPB; 60 nm)/tris(8‐quinolinolato) aluminum (Alq₃):dopant (2.3 wt %) (7 nm)/2,9‐dimethyl‐4,7‐diphenyl‐1,10‐phenanthroline (BCP; 12 nm)/Alq₃(45 nm)/LiF(0.3 nm):Al (300 nm), shows a larger maximum luminance (L_max = 6021 cd m^–2 at 17 V), higher maximum efficiency (η_max = 4.41 cd A^–1 at 11.5 V (235.5 cd m^–2)), and better chromaticity coordinates (Commission Internationale de l'Eclairage, CIE, (x,y) = (0.65,0.35)) than a DCJTB‐based device with the same structure (L_max = 3453 cd m^–2 at 15.5 V, η_max = 3.01 cd A^–1 at 10 V (17.69 cd m^–2), and CIE (x,y) = (0.62,0.38)). The possible reasons for the red‐shifted emission but blue‐shifted absorption of DCQTB relative to DCJTB are also discussed.     

Monodisperse Starburst Oligofluorene‐Functionalized 4,4′,4″‐Tris(carbazol‐9‐yl)‐triphenylamines: Their Synthesis and Deep‐Blue Fluorescent Properties for Organic Light‐Emitting Diode Applications

Four monodisperse starburst oligomers bearing a 4,4′,4″‐tris(carbazol‐9‐yl)‐triphenylamine (TCTA) core and six oligofluorene arms are synthesized and characterized. The lengths of oligofluorene arms vary from one to four fluorene units, giving the starburst oligomers molecular weights ranging from 3072 to 10 068 Da (1 Da = 1.66 × 10^–27 kg). All of the starburst oligomers have good film‐forming capabilities, and display bright, deep‐blue fluorescence (λ_max = 395–416 nm) both in solution and in the solid state, with the quantum efficiencies of the films (Φ_PL) varying between 27 and 88 %. Electrochemical studies demonstrate that these materials have large energy gaps, and are stable for both p‐doping and n‐doping processes. Electroluminescent devices are successfully fabricated using these materials as hole‐transporting emitters, and emit deep‐blue light. Devices with luminance values up to 1025 cd m^–2 at 11 V and luminous efficiencies of 0.47 cd A^–1 at 100 cd m^–2 have been produced, which translates to an external quantum efficiency of 1.4 %. In addition, these large‐energy‐gap starburst oligomers are good host materials for red electrophosphorescence. The luminance of the red electrophosphorescent devices is as high as 4452 cd m^–2, with a luminous efficiency of 4.31 cd A^–1 at 15 mA cm^–2: This value is much higher than those obtained from the commonly used hole‐transporting materials, such as poly(vinyl carbazole) (PVK) (1.10 cd A^–1 at 16 mA cm^–2).     

Binaphthyl‐Containing Green‐ and Red‐Emitting Molecules for Solution‐Processable Organic Light‐Emitting Diodes

Strong intermolecular interactions usually result in decreases in solubility and fluorescence efficiency of organic molecules. Therefore, amorphous materials are highly pursued when designing solution‐processable, electroluminescent organic molecules. In this paper, a non‐planar binaphthyl moiety is presented as a way of reducing intermolecular interactions and four binaphthyl‐containing molecules ( BNCM s): green‐emitting BBB and TBT as well as red‐emitting BTBTB and TBBBT , are designed and synthesized. The photophysical and electrochemical properties of the molecules are systematically investigated and it is found that TBT , TBBBT , and BTBTB solutions show high photoluminescence (PL) quantum efficiencies of 0.41, 0.54, and 0.48, respectively. Based on the good solubility and amorphous film‐forming ability of the synthesized BNCM s, double‐layer structured organic light‐emitting diodes (OLEDs) with BNCM s as emitting layer and poly(N‐vinylcarbazole) (PVK) or a blend of poly[N,N′‐bis(4‐butylphenyl)‐N,N′‐bis(phenyl)benzidine] and PVK as hole‐transporting layer are fabricated by a simple solution spin‐coating procedure. Amongst those, the BTBTB based OLED, for example, reaches a high maximum luminance of 8315 cd · m⁻² and a maximum luminous efficiency of 1.95 cd · A⁻¹ at a low turn‐on voltage of 2.2 V. This is one of the best performances of a spin‐coated OLED reported so far. In addition, by doping the green and red BNCM s into a blue‐emitting host material poly(9,9‐dioctylfluorene‐2,7‐diyl) high performance white light‐emitting diodes with pure white light emission and a maximum luminance of 4000 cd · m⁻² are realized.     

Tetraphenylimidazole‐Based Excited‐State Intramolecular Proton‐Transfer Molecules for Highly Efficient Blue Electroluminescence

Aiming for highly efficient blue electroluminescence, we have designed and synthesized a novel class of tetraphenylimidazole‐ based excited‐state intramolecular proton‐transfer (ESIPT) molecules with covalently linked charge‐transporting functional groups (carbazole‐ and oxadiazole‐functionalized hydroxyl‐substituted tetraphenylimidazole (HPI), i.e., HPI‐Cbz and HPI‐Oxd, respectively). High T_g (ca. 130 °C) amorphous films of HPI‐Cbz and HPI‐Oxd showed intense and ideal blue‐light emission (λ_max = 462 and 468 nm, Φ_PL = 0.44 and 0.38) with a large Stokes shift of over 160 nm and a narrow full width at half‐maximum of less than 65 nm. Organic light‐emitting devices using HPI‐Cbz and HPI‐Oxd as the emitting layer generated an efficient blue electroluminescence (EL) emission peaking at around 460 nm with excellent CIE coordinates of (x, y) = (0.15, 0.11). A maximum external quantum efficiency of 2.94%, and a maximum brightness of 1 229 cd m⁻² at 100 mA cm⁻², as well as a low turn‐on voltage of 4.8 V were achieved in this work.     

Starburst DCM‐Type Red‐Light‐Emitting Materials for Electroluminescence Applications

Three new starburst DCM (4‐(dicyanomethylene)‐2‐methyl‐6‐[4‐(dimethylaminostyryl)‐4H‐pyran]) derivatives, 4,4′,4′′‐tris[2‐(4‐dicyanomethylene‐6‐t‐butyl‐4H‐pyran‐2‐yl)‐ethylene]triphenylamine (TDCM), 4,4′,′′‐tris[2‐(4‐(1′,3′‐indandione)‐6‐t‐butyl‐4H‐pyran‐2‐yl)‐ethylene]triphenylamine (TIN), and 4‐methoxy‐4′,4′′‐bis[2‐(4‐(1′,3′‐indandione)‐6‐t‐butyl‐4H‐pyran‐2‐yl)‐ethylene]triphenylamine (MBIN), have been designed and synthesized for application as red‐light emitters in organic light‐emitting diodes (OLEDs). Differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) reveal their extremely high glass‐transition temperatures and decomposition temperatures, as well as their low tendency to crystallize. Photoluminescence and electroluminescence measurements show that they exhibit a greatly restricted concentration‐quenching effect compared to DCM1 (4‐(dicyanomethylene)‐2‐methyl‐6‐[p‐(N,N‐dimethylamino)‐styryl]‐4H‐pyran), a simple but typical DCM‐type dye, as a result of their non‐planar, three‐dimensional structures that result from their unique propeller‐like triphenylamine electron‐donating cores. The peripheral electron‐withdrawing moieties also play a key role in the restriction of concentration quenching. That is, TIN and MBIN, bearing 1,3‐indandione acceptors, emit more efficiently than TDCM and DCM1, which have dicyanomethylene as acceptors at a high doping concentration of 10 wt.‐% in poly(9‐vinylcarbazole) (PVK) film, irrespective of whether they are photoexcited or electroexcited, though their fluorescence quantum yields in dilute solutions are much lower than that of DCM1. By way of the co‐doping approach, the electroluminescence device with the configuration indium tin oxide (ITO)/PVK:MBIN(10 wt.‐%):tris(4‐(2‐phenylethynyl)‐phenyl)amine (TPA; 30 wt.‐%) (70 nm)/2,9‐dimethyl‐4,7‐diphenyl‐1,10‐phenanthroline (BCP; 20 nm)/tris(8‐quinolinolato) aluminum (Alq₃;15 nm)/LiF (0.3 nm)/Al (150 nm) exhibits a turn‐on voltage of 5.1 V, a maximum luminance of 6971 cd m^–2, a maximum efficiency of 6.14 cd A^–1 (405 cd m^–2), and chromaticity coordinates of (0.66,0.33). The encouraging electroluminescence performance suggests potential applications of the starburst DCM red‐light emitters in OLEDs.     

High‐Purity‐Blue and High‐Efficiency Electroluminescent Devices Based on Anthracene

Novel blue‐light‐emitting materials, 9,10‐bis(1,2‐diphenyl styryl)anthracene (BDSA) and 9,10‐bis(4′‐triphenylsilylphenyl)anthracene (BTSA), which are composed of an anthracene molecule as the main unit and a rigid and bulky 1,2‐diphenylstyryl or triphenylsilylphenyl side unit, have been designed and synthesized. Theoretical calculations on the three‐dimensional structures of BDSA and BTSA show that they have a non‐coplanar structure and inhibited intermolecular interactions, resulting in a high luminescence efficiency and good color purity. By incorporating these new, non‐doped, blue‐light‐emitting materials into a multilayer device structure, it is possible to achieve luminance efficiencies of 1.43 lm W^–1 (3.0 cd A^–1 at 6.6 V) for BDSA and 0.61 lm W^–1 (1.3 cd A^–1 at 6.7 V) for BTSA at 10 mA cm^–2. The electroluminescence spectrum of the indium tin oxide (ITO)/copper phthalocyanine (CuPc)/1,4‐bis[(1‐naphthylphenyl)‐amino]biphenyl (α‐NPD)/BDSA/tris(9‐hydroxyquinolinato)aluminum (Alq₃)/LiF/Al device shows a narrow emission band with a full width at half maximum (FWHM) of 55 nm and a λ_max = 453 nm. The FWHM of the ITO/CuPc/α‐NPD/BTSA/Alq₃/LiF/Al device is 53 nm, with a λ_max = 436 nm. Regarding color, the devices showed highly pure blue emission ((x,y) = (0.15,0.09) for BTSA, (x,y) = (0.14,0.10) for BDSA) at 10 mA cm^–2 in Commission Internationale de l'Eclairage (CIE) chromaticity coordinates.     

Synthesis,Photophysical, and Electroluminescent Device Properties of Zn(II)‐Chelated Complexes Based on Functionalized Benzothiazole Derivatives

New Zn(II)‐chelated complexes based on benzothiazole derivatives, including substituted functional groups such as methyl ( MeZn ), methoxy ( MeOZn ), or fluorenyl unit ( FuZn ), are investigated to produce white‐light emission. 2‐(2‐Hydroxyphenyl)benzothiazole derivatives in toluene and DMSO exhibit excited‐state intramolecular proton transfer (ESIPT), leading to a large Stokes shift of the fluorescence emission. However, in methanol they exhibit no ESIPT due to the intermolecular hydrogen bonding between the 2‐(2‐hydroxyphenyl)benzothiazole derivative and methanol. Their Zn(II)‐chelated complexes exhibit the absorption band red‐shifted at 500 nm in nonpolar solvent and the absorption band blue‐shifted at about 420 nm in protic solvent. In multilayer electroluminescent devices, methyl‐substituted Zn(II)‐chelated complex ( MeZn ) exhibits excellent power efficiency and fluorene‐substituted Zn(II)‐chelated complex ( FuZn ) has a high luminance efficiency (1 cd m^?2 at 3.5 V, 10 400 cd m^?2 at 14 V). The EL spectra of Zn(II)‐chelated complexes based on benzothiazole derivatives exhibit broad emission bands. In addition, their electron‐transport property for red–green–blue (RGB) organic light‐emitting diodes (OLEDs) is systematically studied, in comparison with that of Alq₃. The results demonstrate the promising potential of MeZn as an electron‐transporting layer (ETL) material in preference to Alq₃, which is widely used as an ETL material.     

Improved Efficiency of Single‐Layer Polymer Light‐Emitting Devices with Poly(vinylcarbazole) Doubly Doped with Phosphorescent and Fluorescent Dyes as the Emitting Layer

We demonstrate novel organic light‐emitting diode (LED) materials that contain a green phosphorescent dye (dmbpy)Re(CO)₃Cl (dmbpy = 4,4′‐dimethyl‐2,2′‐bipyridine), and a red fluorescent dye 4‐dicyanomethylene‐6‐(p‐dimethylaminostyryl)‐2‐methyl‐4H‐pyran (DCM) as dopants and polyvinylcarbazole (PVK) as the host. The photoluminescence (PL) and electroluminescence (EL) properties of these complex materials were studied. The energy transfer efficiency from PVK host to DCM is increased by the (dmbpy)Re(CO)₃Cl co‐dopant, which has an emission energy between that of PVK and DCM. The (dmbpy)Re(CO)₃Cl, which emits a long‐lived phosphorescence, is used as an energy coupler, providing the possibility to harvest both singlet and triplet energy in the devices. The pure red emission from DCM was observed from PL and EL spectra of (dmbpy)Re(CO)₃‐Cl(> 2.0 wt.‐%):DCM(> 0.5 wt. %) doped PVK films, demonstrating an efficient energy transfer from PVK and (dmbpy)Re(CO)₃‐Cl to DCM. By optimizing the concentration of DCM and (dmbpy)Re(CO)₃Cl in PVK, a maximum EL quantum efficiency of 0.42 cd A^–1 at a current density of 9.5 mA cm^–2 was obtained. The EL quantum efficiency of the doubly doped device is significantly enhanced in comparison with both a DCM‐only doped PVK device and a DCM‐doped PVK device with the green fluorescent dye Alq₃ as co‐dopant. The improvement in the operating characteristics of the phosphorescent and fluorescent dye doubly doped device is attributed to efficient energy transfer in the system, in which both triplet and singlet excitons are used for resultant emission in the polymer device.     

功能层界面制备方法对OLED性能的影响

在功能层界面处采用各功能材料共蒸的方法,制备了典型的绿光有机发光器件(OLED)。器件的结构为ITO/NPB(37nm)/(NPB:Alq3)(3nm)/Alq3(27nm):C545T(3%)/Alq3(20nm)/LiF(1nm)/Al(100nm),并与传统的制备方法进行了比较。结果发现,起亮电压从4.5V降低到2.5V,最高耐压从16V提高到21V,最大亮度从13 940cd/m2提高到24 630cd/m2,发光效率由7.0cd/A提高到11.4cd/A。结果表明,本文方法有利于载流子传输,可以有效提高激子形成概率,提高了OLED发光效率。     

Highly Efficient Electroluminescence from Green‐Light‐Emitting Electrochemical Cells Based on CuI Complexes

The complexes [Cu(dnbp)(DPEphos)]⁺(X^–) (dnbp and DPEphos are 2,9‐di‐n‐butyl‐1,10‐phenanthroline and bis[2‐(diphenylphosphino)phenyl]ether, respectively, and X^– is BF₄^–, ClO₄^–, or PF₆^–) can form high‐quality films with photoluminescence quantum yields of up to 71 ± 7 %. Their electroluminescent properties are studied using the device structure indium tin oxide (ITO)/complex/metal cathode. The devices emit green light efficiently, with an emission maximum of 523 nm, and work in the mode of light‐emitting electrochemical cells. The response time of the devices greatly depends on the driving voltage, the counterions, and the thickness of the complex film. After pre‐biasing at 25 V for 40 s, the devices turn on instantly, with a turn‐on voltage of ca. 2.9 V. A current efficiency of 56 cd A^–1 and an external quantum efficiency of 16 % are realized with Al as the cathode. Using a low‐work‐function metal as the cathode can significantly enhance the brightness of the device almost without affecting the turn‐on voltage and current efficiency. With a Ca cathode, a brightness of 150 cd m^–2 at 6 V and 4100 cd m^–2 at 25 V is demonstrated. The electroluminescent performance of these types of complexes is among the best so far for transition metal complexes with counterions.     

Improved property in organic light-emitting diode utilizing two Al/Alq3 layers

We reported on the fabrication of organic light-emitting devices (OLEDs) utilizing the two Al/Alq₃ layers and two electrodes. This novel green device with structure of Al(110 nm)/tris(8-hydroxyquinoline) aluminum (Alq₃)(65 nm)/Al(110 nm)/Alq₃(50 nm)/N,N′-dipheny1-N, N′-bis-(3-methy1phyeny1)-1, 1′-bipheny1-4, 4′-diamine (TPD)(60 nm)/ITO(60 nm)/Glass. TPD were used as holes transporting layer (HTL), and Alq₃ was used as electron transporting layer (ETL), at the same time, Alq₃ was also used as emitting layer (EL), Al and ITO were used as cathode and anode, respectively. The results showed that the device containing the two Al/Alq₃ layers and two electrodes had a higher brightness and electroluminescent efficiency than the device without this layer. At current density of 14 mA/cm², the brightness of the device with the two Al/Alq₃ layers reach 3693 cd/m², which is higher than the 2537 cd/m² of the Al/Alq₃/TPD:Alq₃/ITO/Glass device and the 1504.0 cd/m² of the Al/Alq₃/TPD/ITO/Glass. Turn-on voltage of the device with two Al/Alq₃ layers was 7 V, which is lower than the others.     

1‐Methyl‐2‐(anthryl)‐imidazo[4,5‐f][1,10]‐phenanthroline: A Highly Efficient Electron‐Transport Compound and a Bright Blue‐Light Emitter for Electroluminescent Devices

A new organic blue‐light emitter 1‐methyl‐2‐(anthryl)‐imidazo[4,5‐f][1,10]‐phenanthroline ( 1 ) has been synthesized and fully characterized. The utility of compound 1 as a blue‐light emitter in electroluminescent (EL) devices has been evaluated by fabricating a series of EL devices A where compound 1 functions as an emitter. The EL spectrum of device series A has the emission maximum at 481 nm with the CIE (Commission Internationale de l'Eclairage) color coordinates 0.198 and 0.284. The maximum luminance of devices in series A is 4000 cd m^–2 and the best external quantum efficiency of device series A is 1.82 %. The utility of compound 1 as an electron injection–electron transport material has been evaluated by constructing a set of EL devices B where 1 is used as either the electron‐injection layer or the electron injection–electron transport layer. The performance of device series B is compared to the standard device in which Alq₃ (tris(8‐hydroxyquinoline) aluminum) is used as the electron injection–electron transport layer. The experimental results show that the performance of 1 as an electron injection–electron transport material is considerably better than Alq₃. The stability of device series B is comparable to that of the standard Alq₃ device. The excellent performance of 1 as an electron injection/transport material may be attributed to the strong intermolecular interactions of 1 in the solid state as revealed by single‐crystal X‐ray diffraction analysis. In addition, compound 1 is a colorless material with a much larger highest occupied molecular orbital–lowest unoccupied molecular (HOMO–LUMO) gap than Alq₃, which renders it potentially useful for a wide range of applications in EL devices.     

High‐Performance Quantum‐Dot Light‐Emitting Diodes Using NiOx Hole‐Injection Layers with a High and Stable Work Function

Solution‐processed oxide thin films are actively pursued as hole‐injection layers (HILs) in quantum‐dot light‐emitting diodes (QLEDs), aiming to improve operational stability. However, device performance is largely limited by inefficient hole injection at the interfaces of the oxide HILs and high‐ionization‐potential organic hole‐transporting layers. Solution‐processed NiO_x films with a high and stable work function of ≈5.7 eV achieved by a simple and facile surface‐modification strategy are presented. QLEDs based on the surface‐modified NiO_x HILs show driving voltages of 2.1 and 3.3 V to reach 1000 and 10 000 cd m^?2, respectively, both of which are the lowest among all solution‐processed LEDs and vacuum‐deposited OLEDs. The device exhibits a T₉₅ operational lifetime of ≈2500 h at an initial brightness of 1000 cd m^?2, meeting the commercialization requirements for display applications. The results highlight the potential of solution‐processed oxide HILs for achieving efficient‐driven and long‐lifetime QLEDs.     

Molecular Engineering of Blue Fluorescent Molecules Based on Silicon End‐Capped Diphenylaminofluorene Derivatives for Efficient Organic Light‐Emitting Materials

Blue fluorescent materials based on silicone end‐capped 2‐diphenylaminofluorene derivatives are synthesized and characterized. These materials are doped into a 2‐methyl‐9,10‐di‐[2‐naphthyl]anthracene host as blue dopant materials in the emitting layer of organic light‐emitting diode devices bearing a structure of ITO/DNTPD (60 nm)/NPB (30 nm)/emitting layer (30 nm)/Alq₃ (20 nm)/LiF (1.0 nm)/Al (200 nm). All devices exhibit highly efficient blue electroluminescence with high external quantum efficiencies (3.47%–7.34% at 20 mA cm^?2). The best luminous efficiency of 11.2 cd A^?1 and highest quantum efficiency of 7.34% at 20 mA cm^?2 are obtained in a device with CIE coordinates (0.15, 0.25). A deep‐blue OLED with CIE coordinates (0.15, 0.14) exhibits a luminous efficiency of 3.70 cd A^?1 and quantum efficiency of 3.47% at 20 mA cm^?2.     

Efficient Light‐Emitting Electrochemical Cells (LECs) Based on Ionic Iridium(III) Complexes with 1,3,4‐Oxadiazole Ligands

Eight new iridium(III) complexes 1‐8 , with 1,3,4‐oxadiazole (OXD) derivatives as the cyclometalated C^N ligand and/or the ancillary N^N ligands are synthesized and their electrochemical, photophysical, and solid‐state light‐emitting electrochemical cell (LEC) properties are investigated. Complexes 1 , 2 , 7 and 8 are additionally characterized by single crystal X‐ray diffraction. LECs based on complexes 1‐8 are fabricated with a structure indium tin oxide (ITO)/poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)/cationic iridium complex:ionic liquid/Al. LECs of complexes 1 – 6 with OXD derivatives as the cyclometalated ligands and as the ancillary ligand show yellow luminescence (λ_max = 552–564 nm). LECs of complexes 7 and 8 with cyclometalated C^N phenylpyridine ligands and an ancillary N^N OXD ligand show red emission (λ_max 616–624 nm). Using complex 7 external quantum efficiency (EQE) values of >10% are obtained for devices (210 nm emission layer) at 3.5 V. For thinner devices (70 nm) high brightness is achieved: red emission for 7 (8528 cd m^?2 at 10 V) and yellow emission for 1 (3125 cd m^?2 at 14 V).     

White organic light-emitting diodes based on emission from DPVBi-doped 4,48-bis (2,28-diphenylvinyl)-1, 18-biphenyl

Organiclight-emitting diodes (OLEDs) have beenin-vestigated for many years on account of their highlumi-nance,low driven voltages ,wide visual range,flexiblesubstratesinflat-panel ,full color displays and backlightapplications .For high brightness and eff…     

Manipulating Charge‐Transfer Character with Electron‐Withdrawing Main‐Group Moieties for the Color Tuning of Iridium Electrophosphors

A new and synthetically versatile strategy has been developed for the phosphorescence color tuning of cyclometalated iridium phosphors by simple tailoring of the phenyl ring of ppy (Hppy = 2‐phenylpyridine) with various main‐group moieties in [Ir(ppy‐X)₂(acac)] (X = B(Mes)₂, SiPh₃, GePh₃, NPh₂, POPh₂, OPh, SPh, SO₂Ph). This can be achieved by shifting the charge‐transfer character from the pyridyl groups in some traditional iridium ppy‐type complexes to the electron‐withdrawing main‐group moieties and these assignments were supported by theoretical calculations. This new color tuning strategy in Ir^III‐based triplet emitters using electron‐withdrawing main‐group moieties provides access to Ir^III phosphors with improved electron injection/electron transporting features essential for highly efficient, color‐switchable organic light‐emitting diodes (OLEDs). The present work furnished OLED colors spanning from bluish‐green to red (505–609 nm) with high electroluminescence efficiencies which have great potential for application in multicolor displays. The maximum external quantum efficiency of 9.4%, luminance efficiency of 10.3 cd A⁻¹ and power efficiency of 5.0 lm W⁻¹ for the red OLED (X = B(Mes)₂), 11.1%, 35.0 cd A⁻¹, and 26.8 lm W⁻¹ for the bluish‐green device (X = OPh), 10.3%, 36.9 cd A⁻¹, and 28.6 lm W⁻¹ for the bright green device (X = NPh₂) as well as 10.7%, 35.1 cd A⁻¹, and 23.1 lm W⁻¹ for the yellow‐emitting device (X = SO₂Ph) can be obtained.     

Extremely Low Operating Voltage Green Phosphorescent Organic Light‐Emitting Devices

Organic light‐emitting devices (OLEDs) are expected to be adopted as the next generation of general lighting because they are more efficient than fluorescent tubes and are mercury‐free. The theoretical limit of operating voltage is generally believed to be equal to the energy gap, which corresponds to the energy difference between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) for the emitter molecule divided by the electron charge (e). Here, green OLEDs operating below a theoretical limit of the energy gap (E_g) voltage with high external quantum efficiency over 20% are demonstrated using fac‐tris(2‐phenylpyridine)iridium(III) with a peak emission wavelength of 523 nm, which is equivalent to a photon energy of 2.38 eV. An optimized OLED operates clearly below the theoretical limit of the E_g voltage at 2.38 V showing 100 cd m^?2 at 2.25 V and 5000 cd m^?2 at 2.95 V without any light outcoupling enhancement techniques.     

MoO3 as p-type dopant for Alq3-based p–i–n homojunction organic light-emitting diodes

Using high-work-function material MoO₃ as a p-type dopant, efficient single-layer hybrid organic light-emitting diodes (OLEDs) with the p–i–n homojunction structure are investigated. When MoO₃ and Cs₂CO₃ are doped into the conventional emitting/electron-transport material tris-(8-hydroxyquinoline) aluminum (Alq₃), respectively, a significant increase in p- and n-type conductivities is observed compared to that of intrinsic Alq₃ thin films. With optimal doping, the hole and electron mobilities in Alq₃:MoO₃ and Alq₃:Cs₂CO₃ films was estimated to be 9.76 × 10⁻⁶ and 1.26 × 10⁻⁴ cm²/V s, respectively, which is about one order of magnitude higher than that of the undoped device. The p–i–n OLEDs outperform undoped (i–i–i) and single-dopant (p–i–i and i–i–n) OLEDs; they have the lowest turn-on voltage (4.3 V at 1 cd/m²), highest maximum luminance (5860 cd/m² at 11.4 V), and highest luminous efficiency (2.53 cd/A at 100 mA/cm²). These values are better than those for bilayer heterojunction OLEDs using the same emitting layer. The increase in conductivity can be attributed to the charge transfer process between the Alq₃ host and the dopant. Due to the change of carrier concentration in the Alq₃ films, the Fermi level of Alq₃ is close to the highest occupied molecular orbital (HOMO) or lowest unoccupied molecular orbital (LUMO) energy levels upon p- and n-type doping, respectively, and the carrier injection efficiency can thus be enhanced because of the lower carrier injection barrier. The carriers move closer to the center energy levels of the HOMO or LUMO distributions, which increases the hopping rate for charge transport and results in an increase of charge carrier mobility. The electrons are the majority charge carriers, and both the holes and electrons can be dramatically injected in high numbers and then efficiently recombined in the p–i–n OLEDs. As a result, the improved conductivity characteristics as well as the appropriate energy levels of the doped layers result in improved electroluminescent performance of the p–i–n homojunction OLEDs.     

A Pyridine‐Containing Anthracene Derivative with High Electron and Hole Mobilities for Highly Efficient and Stable Fluorescent Organic Light‐Emitting Diodes

A pyridine‐containing anthracene derivative, 9,10‐bis(3‐(pyridin‐3‐yl)phenyl)anthracene (DPyPA), which comprehensively outperforms the widely used electron‐transport material (ETM), tris(8‐quinolinolato) aluminum (Alq₃), is synthesized. DPyPA exhibits ambipolar transport properties, with both electron and hole mobilities of around 10^?3 cm^?2 V^?1 s^?1; about two orders of magnitude higher than that of Alq₃. The nitrogen atom in the pyridine ring of DPyPA coordinates to lithium cations, which leads to efficient electron injection when LiF/Al is used as the cathode. Electrochemical measurements demonstrate that both the cations and anions of DPyPA are stable, which may improve the stability of devices based on DPyPA. Red‐emitting, green‐emitting, and blue‐emitting fluorescent organic light emitting diodes with DPyPA as the ETM display lower turn‐on voltages, higher efficiencies, and stronger luminance than the devices with Alq₃ as the ETM. The power efficiencies of the devices based on DPyPA are greater by 80–140% relative to those of the Alq₃‐based devices. The improved performance of these devices is attributed to the increased carrier balance. In addition, the device employing DPyPA as the ETM possesses excellent stability: the half‐life of the DPyPA‐based device is 67 000 h—seven times longer than that of the Alq₃‐based device—for an initial luminance of 5000 cd m^?2.