Solution‐Processed,Alkali Metal‐Salt‐Doped,Electron‐Transport Layers for High‐Performance Phosphorescent Organic Light‐Emitting Diodes

High‐performance, blue, phosphorescent organic light‐emitting diodes (PhOLEDs) are achieved by orthogonal solution‐processing of small‐molecule electron‐transport material doped with an alkali metal salt, including cesium carbonate (Cs₂CO₃) or lithium carbonate (Li₂CO₃). Blue PhOLEDs with solution‐processed 4,7‐diphenyl‐1,10‐phenanthroline (BPhen) electron‐transport layer (ETL) doped with Cs₂CO₃ show a luminous efficiency (LE) of 35.1 cd A^?1 with an external quantum efficiency (EQE) of 17.9%, which are two‐fold higher efficiency than a BPhen ETL without a dopant. These solution‐processed blue PhOLEDs are much superior compared to devices with vacuum‐deposited BPhen ETL/alkali metal salt cathode interfacial layer. Blue PhOLEDs with solution‐processed 1,3,5‐tris(m‐pyrid‐3‐yl‐phenyl)benzene (TmPyPB) ETL doped with Cs₂CO₃ have a luminous efficiency of 37.7 cd A^?1 with an EQE of 19.0%, which is the best performance observed to date in all‐solution‐processed blue PhOLEDs. The results show that a small‐molecule ETL doped with alkali metal salt can be realized by solution‐processing to enhance overall device performance. The solution‐processed metal salt‐doped ETLs exhibit a unique rough surface morphology that facilitates enhanced charge‐injection and transport in the devices. These results demonstrate that orthogonal solution‐processing of metal salt‐doped electron‐transport materials is a promising strategy for applications in various solution‐processed multilayered organic electronic devices.     

Pyridine‐Containing Electron‐Transport Materials for Highly Efficient Blue Phosphorescent OLEDs with Ultralow Operating Voltage and Reduced Efficiency Roll‐Off

A series of pyridine‐containing electron‐transport materials are developed as an electron‐transport layer for the FIrpic‐based blue phosphorescent organic light‐emitting diodes. Their energy levels can be tuned by the introduction of pyridine rings in the framework and on the periphery of the molecules. Significantly reduced operating voltage is achieved without compromising external quantum efficiency by solely tuning the nitrogen atom orientations of those pyidine rings. Unprecedented low operating voltages of 2.61 and 3.03 V are realized at 1 and 100 cd m^?2, giving ever highest power efficiency values of 65.8 and 59.7 lm W^?1, respectively. In addition, the operating voltages at 100 cd m^?2 can be further reduced to 2.70 V by using a host material with a small singlet‐triplet exchange energy, and the threshold voltage for electroluminescence can even be 0.2–0.3 V lower than the theoretical minimum value of the photon energy divided by electron charge. Aside from the reduced operating voltage, a further reduced roll‐off in efficiency is also achieved by the combination of an appropriate host material.     

Structure–Property Relationship of Pyridine‐Containing Triphenyl Benzene Electron‐Transport Materials for Highly Efficient Blue Phosphorescent OLEDs

Three triphenyl benzene derivatives of 1,3,5‐tri(m‐pyrid‐2‐yl‐phenyl)benzene (Tm2PyPB), 1,3,5‐tri(m‐pyrid‐3‐yl‐phenyl)benzene (Tm3PyPB) and 1,3,5‐tri(m‐pyrid‐4‐yl‐phenyl)benzene (Tm4PyPB), containing pyridine rings at the periphery, are developed as electron‐transport and hole/exciton‐blocking materials for iridium(III) bis(4,6‐(di‐fluorophenyl)pyridinato‐N,C^2′)picolinate (FIrpic)‐based blue phosphorescent organic light‐emitting devices. Their highest occupied molecular orbital and lowest unoccupied molecular orbital (LUMO) energy levels decrease as the nitrogen atom of the pyridine ring moves from position 2 to 3 and 4; this is supported by both experimental results and density functional theory calculations, and gives improved electron‐injection and hole‐blocking properties. They exhibit a high electron mobility of 10^?4–10^?3 cm² V^?1 s^?1 and a high triplet energy level of 2.75 eV. Confinement of FIrpic triplet excitons is strongly dependent on the nitrogen atom position of the pyridine ring. The second exponential decay component in the transient photoluminescence decays of Firpic‐doped films also decreases when the position of the nitrogen atom in the pyridine ring changes. Reduced driving voltages are obtained when the nitrogen atom position changes because of improved electron injection as a result of the reduced LUMO level, but a better carrier balance is achieved for the Tm3PyPB‐based device. An external quantum efficiency (EQE) over 93% of maximum EQE was achieved for the Tm4PyPB‐based device at an illumination‐relevant luminance of 1000 cd m^?2, indicating reduced efficiency roll‐off due to better confinement of FIrpic triplet excitons by Tm4PyPB in contrast to Tm2PyPB and Tm3PyPB.     

Dependence of Light‐Emitting Characteristics of Blue Phosphorescent Organic Light‐Emitting Diodes on Electron Injection and Transport Materials

We investigate the light‐emitting performances of blue phosphorescent organic light‐emitting diodes (PHOLEDs) with three different electron injection and transport materials, that is, bathocuproine(2,9‐dimethyl‐4,7‐diphenyl‐1,10‐phenanthroline) (Bphen), 1,3,5‐tri(m‐pyrid‐3‐yl‐phenyl)benzene (Tm3PyPB), and 2,6‐bis(3‐(carbazol‐9‐yl)phenyl)pyridine (26DCzPPy), which are partially doped with cesium metal. We find that the device characteristics are very dependent on the nature of the introduced electron injection layer (EIL) and electron transporting layer (ETL). When the appropriate EIL and ETL are combined, the peak external quantum efficiency and peak power efficiency improve up to 20.7% and 45.6 lm/W, respectively. Moreover, this blue PHOLED even maintains high external quantum efficiency of 19.6% and 16.9% at a luminance of 1,000 cd/m² and 10,000 cd/m², respectively.     

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.     

A Light‐Blue Phosphorescent Dendrimer for Efficient Solution‐Processed Light‐Emitting Diodes

We describe the preparation of a dendrimer that is solution‐processible and contains 2‐ethylhexyloxy surface groups, biphenyl‐based dendrons, and a fac‐tris[2‐(2,4‐difluorophenyl)pyridyl]iridium(III ) core. The homoleptic complex is highly luminescent and the color of emission is similar to the heteroleptic iridium(III ) complex, bis[2‐(2,4‐difluorophenyl)pyridyl]picolinate iridium(III ) (FIrpic). To avoid the change in emission color that would arise from attaching a conjugated dendron to the ligand, the conjugation between the dendron and the ligand is decoupled by separating them with an ethane linkage. Bilayer devices containing a light‐emitting layer comprised of a 30 wt.‐% blend of the dendrimer in 1,3‐bis(N‐carbazolyl)benzene (mCP) and a 1,3,5‐tris(2‐N‐phenylbenzimidazolyl)benzene electron‐transport layer have external quantum and power efficiencies, respectively, of 10.4 % and 11 lm W^–1 at 100 cd m^–2 and 6.4 V. These efficiencies are higher than those reported for more complex device structures prepared via evaporation that contain FIrpic blended with mCP as the emitting layer, showing the advantage of using a dendritic structure to control processing and intermolecular interactions. The external quantum efficiency of 10.4 % corresponds to the maximum achievable efficiency based on the photoluminescence quantum yield of the emissive film and the standard out‐coupling of light from the device.     

Deep‐Blue Phosphorescent Ir(III) Complexes with Light‐Harvesting Functional Moieties for Efficient Blue and White PhOLEDs in Solution‐Process

The photoluminescence (PL) efficiency of emitters is a key parameter to accomplish high electroluminescent performance in phosphorescent organic light‐emitting diodes (PhOLEDs). With the aim of enhancing the PL efficiency, this study designs deep‐blue emitting heteroleptic Ir(III) complexes (tBuCN‐FIrpic, tBuCN‐FIrpic‐OXD, and tBuCN‐FIrpic‐mCP) for solution‐processed PhOLEDs by covalently attaching the light‐harvesting functional moieties (mCP‐Me or OXD‐Me) to the control Ir(III) complex, tBuCN‐FIrpic. These Ir(III) complexes show similar deep‐blue emission peaks around 453, 480 nm (298 K) and 447, 477 nm (77 K) in chloroform. tBuCN‐FIrpic‐mCP demonstrates higher light‐harvesting efficiency (142%) than tBuCN‐FIrpic‐OXD (112%), relative to that of tBuCN‐FIrpic (100%), due to an efficient intramolecular energy transfer from the mCP group to the Ir(III) complex. Accordingly, the monochromatic PhOLEDs of tBuCN‐FIrpic‐mCP show higher external quantum efficiency (EQE) of 18.2% with one of the best blue coordinates (0.14, 0.18) in solution‐processing technology. Additionally, the two‐component (deep‐blue:yellow‐orange), single emitting layer, white PhOLED of tBuCN‐FIrpic‐mCP shows a maximum EQE of 20.6% and superior color quality (color rendering index (CRI) = 78, Commission Internationale de L'Eclairage (CIE) coordinates of (0.353, 0.352)) compared with the control device containing sky‐blue:yellow‐orange emitters (CRI = 60, CIE coordinates of (0.293, 0.395)) due to the good spectral coverage by the deep‐blue emitter.     

Synthesis and Characterization of Red‐Emitting Iridium(III) Complexes for Solution‐Processable Phosphorescent Organic Light‐Emitting Diodes

A new series of highly efficient red‐emitting phosphorescent Ir(III) complexes, (Et‐CVz‐PhQ)₂Ir(pic‐N‐O), (Et‐CVz‐PhQ)₂Ir(pic), (Et‐CVz‐PhQ)₂Ir(acac), (EO‐CVz‐PhQ)₂Ir(pic‐N‐O), (EO‐CVz‐PhQ)₂Ir(pic), and (EO‐CVz‐PhQ)₂Ir(acac), based on carbazole (CVz)‐phenylquinoline (PhQ) main ligands and picolinic acid N‐oxide (pic‐N‐O), picolinic acid (pic), and acetylacetone (acac) ancillary ligands, are synthesized for phosphorescent organic light‐emitting diodes (PhOLEDs), and their photophysical, electrochemical, and electroluminescent (EL) properties are investigated. All of the Ir(III) complexes have high thermal stability and emit an intense red light with an excellent color purity at CIE coordinates of (0.65,0.34). Remarkably, high‐performance solution‐processable PhOLEDs were fabricated using Ir(III) complexes with a pic‐N‐O ancillary ligand with a maximum external quantum efficiency (5.53%) and luminance efficiency (8.89 cd A^?1). The novel use of pic‐N‐O ancillary ligand in the synthesis of phosphorescent materials is reported. The performance of PhOLEDs using these Ir(III) complexes correlates well with the results of density functional theory calculations.     

Multifunctional Crosslinkable Iridium Complexes as Hole Transporting/Electron Blocking and Emitting Materials for Solution‐Processed Multilayer Organic Light‐Emitting Diodes

Here, a new series of crosslinkable heteroleptic iridium (III) complexes for use in solution processed phosphorescent organic light emitting diodes (OLEDs) is reported. These iridium compounds have the general formula of (PPZ‐VB)₂Ir(CˆN), where PPZ‐VB is phenylpyrazole (PPZ) vinyl benzyl (VB) ether; and the CˆN ligands represent a family of four different cyclometallating ligands including 1‐phenylpyrazolyl (PPZ) (1), 2‐(4,6‐difluorophenyl)pyridyl (DFPPY) (2), 2‐(p‐tolyl)pyridyl (TPY) (3), and 2‐phenylquinolyl (PQ) (4). With the incorporation of two crosslinkable VB ether groups, these compounds can be fully crosslinked after heating at 180 °C for 30 min. The crosslinked films exhibit excellent solvent resistance and film smoothness which enables fabrication of high‐performance multilayer OLEDs by sequential solution processing of multiple layers. Furthermore, the photophysical properties of these compounds can be easily controlled by simply changing the cyclometallating CˆN ligand in order to tune the triplet energy within the range of 3.0–2.2 eV. This diversity makes these materials not only suitable for use in hole transporting and electron blocking but also as emissive layers of several colors. Therefore, these compounds are applied as effective materials for all‐solution processed OLEDs with (PPZ‐VB)₂IrPPZ (1) acting as hole transporting and electron blocking layer and host material, as well as three other compounds, (PPZ‐VB)₂IrDFPPY ( 2 ), (PPZ‐VB)₂IrTPY(3), and (PPZ‐VB)₂IrPQ( 4 ), used as crosslinkable phosphorescent emitters.     

Solution‐Processible Carbazole Dendrimers as Host Materials for Highly Efficient Phosphorescent Organic Light‐Emitting Diodes

A group of dendrimers with oligo‐carbazole dendrons appended at 4,4′‐ positions of biphenyl core are synthesized for use as host materials for solution‐processible phosphorescent organic light‐emitting diodes (PHOLEDs). In comparison with the traditional small molecular host 4,4′‐N,N′‐dicarbazolebiphenyl (CBP), the dendritic conformation affords these materials extra merits including amorphous nature with extremely high glass transition temperatures (ca. 376 °C) and solution‐processibility, but inherent the identical triplet energies (2.60–2.62 eV). In comparison with the widely‐used polymeric host polyvinylcarbazole (PVK), these dendrimers possess much higher HOMO levels (–5.61 to –5.42 eV) that facilitate efficient hole injection and are favorable for high power efficiency in OLEDs. The agreeable properties and the solution‐processibility of these dendrimers makes it possible to fabricate highly efficient PHOLEDs by spin coating with the dendimers as phosphorescent hosts. The green PHOLED containing Ir(ppy)₃ (Hppy = 2‐phenyl‐pyridine) dopant exhibits high peak efficiencies of 38.71 cd A^?1 and 15.69 lm W^?1, which far exceed those of the control device with the PVK host (27.70 cd A^?1 and 9.6 lm W^?1) and are among the best results for solution‐processed green PHOLEDs ever reported. The versatility of these dendrimer hosts can be spread to orange PHOLEDs and high efficiencies of 32.22 cd A^?1 and 20.23 lm W^?1 are obtained, among the best ever reported for solution‐processed orange PHOLEDs.     

Versatile,Benzimidazole/Amine‐Based Ambipolar Compounds for Electroluminescent Applications: Single‐Layer,Blue, Fluorescent OLEDs,Hosts for Single‐Layer,Phosphorescent OLEDs

A series of compounds containing arylamine and 1,2‐diphenyl‐1H‐benz[d]imidazole moieties are developed as ambipolar, blue‐emitting materials with tunable blue‐emitting wavelengths, tunable ambipolar carrier‐transport properties and tunable triplet energy gaps. These compounds possess several novel properties: (1) they emit in the blue region with high quantum yields; (2) they have high morphological stability and thermal stability; (3) they are capable of ambipolar carrier transport; (4) they possess tunable triplet energy gaps, suitable as hosts for yellow‐orange to green phosphors. The electron and hole mobilities of these compounds lie in the range of 0.68–144 × 10^?6 and 0.34–147 × 10^?6 cm² V^?1 s^?1, respectively. High‐performance, single‐layer, blue‐emitting, fluorescent organic light‐emitting diodes (OLEDs) are achieved with these ambipolar materials. High‐performance, single‐layer, phosphorescent OLEDs with yellow‐orange to green emission are also been demonstrated using these ambipolar materials, which have different triplet energy gaps as the host for yellow‐orange‐emitting to green‐emitting iridium complexes. When these ambipolar, blue‐emitting materials are lightly doped with a yellow‐orange‐emitting iridium complex, white organic light‐emitting diodes (WOLEDs) can be achieved, as well by the use of the incomplete energy transfer between the host and the dopant.     

An Alternative Approach to Constructing Solution Processable Multifunctional Materials: Their Structure,Properties, and Application in High‐Performance Organic Light‐Emitting Diodes

A new series of full hydrocarbons, namely 4,4′‐(9,9′‐(1,3‐phenylene)bis(9H‐fluorene‐9,9‐diyl))bis(N,N‐diphenylaniline) (DTPAFB), N,N′‐(4,4′‐(9,9′‐(1,3‐phenylene)bis(9H‐fluorene‐9,9‐diyl))bis(4,1‐phenylene))bis(N‐phenylnaphthalen‐1‐amine) (DNPAFB), 1,3‐bis(9‐(4‐(9H‐carbazol‐9‐yl)phenyl)‐9H‐fluoren‐9‐yl)benzene, and 1,3‐bis(9‐(4‐(3,6‐di‐tert‐butyl‐9H‐carbazol‐9‐yl)phenyl)‐9H‐fluoren‐9‐yl)benzene, featuring a highly twisted tetrahedral conformation, are designed and synthesized. Organic light‐emitting diodes (OLEDs) comprising DNPAFB and DTPAFB as hole transporting layers and tris(quinolin‐8‐yloxy)aluminum as an emitter are made either by vacuum deposition or by solution processing, and show much higher maximum efficiencies than the commonly used N,N′‐di(naphthalen‐1‐yl)‐N,N′‐diphenylbiphenyl‐4,4′‐diamine device (3.6 cd A^?1) of 7.0 cd A^?1 and 6.9 cd A^?1, respectively. In addition, the solution processed blue phosphorescent OLEDs employing the synthesized materials as hosts and iridium (III) bis[(4,6‐di‐fluorophenyl)‐pyridinato‐N, C²] picolinate (FIrpic) phosphor as an emitter present exciting results. For example, the DTPAFB device exhibits a brightness of 47 902 cd m^?2, a maximum luminescent efficiency of 24.3 cd A^?1, and a power efficiency of 13.0 lm W^?1. These results show that the devices are among the best solution processable blue phosphorescent OLEDs based on small molecules. Moreover, a new approach to constructing solution processable small molecules is proposed based on rigid and bulky fluorene and carbazole moieties combined in a highly twisted configuration, resulting in excellent solubility as well as chemical miscibility, without the need to introduce any solubilizing group such as an alkyl or alkoxy chain.     

Phosphorescent Cationic Au4Ag2 Alkynyl Cluster Complexes for Efficient Solution‐Processed Organic Light‐Emitting Diodes

Cationic Au₄Ag₂ heterohexanuclear aromatic acetylides cluster complexes supported by bis(2‐diphenylphosphinoethyl)phenylphosphine (dpep) are prepared. The Au₄Ag₂ cluster structure originating from the combination of one anionic [Au(C≡CR)₂]^? with one cationic [Au₃Ag₂(dpep)₂(C≡CR)₂]³⁺ through the formation of Ag?acetylide η²‐bonds is highly stabilized by Au–Ag and Au–Au contacts. The Au₄Ag₂ alkynyl cluster complexes are moderately phosphorescent in the fluid CH₂Cl₂ solution, but exhibit highly intense phosphorescent emission in solid state and film. As revealed by theoretical computational studies, the phosphorescence is ascribable to significant ³[π (aromatic acetylide) → s/p (Au)] ³LMCT parentage with a noticeable Au₄Ag₂ cluster centered ³[d → s/p] triplet state. Taking advantage of mCP and OXD‐7 as a mixed host with 20 wt% dopant of phosphorescent Au₄Ag₂ cluster complex in the emitting layer, solution‐processed organic light‐emitting diodes (OLEDs) exhibit highly efficient electrophosphorescence with the maximum current, power, and external quantum efficiencies of 24.1 cd A^?1, 11.6 lm W^?1, and 7.0%, respectively. Introducing copper(I) thiocyanate (CuSCN) as a hole‐transporting layer onto the PEDOT:PSS hole‐injecting layer through the orthogonal solution process induces an obvious improvement of the device performance with lower turn‐on voltage and higher electroluminescent efficiency.     

Stable,Glassy, and Versatile Binaphthalene Derivatives Capable of Efficient Hole Transport,Hosting, and Deep‐Blue Light Emission

Organic light‐emitting diodes (OLEDs) have great potential applications in display and solid‐state lighting. Stability, cost, and blue emission are key issues governing the future of OLEDs. The synthesis and photoelectronics of a series of three kinds of binaphthyl (BN) derivatives are reported. BN_1–3 are “melting‐point‐less” and highly stable materials, forming very good, amorphous, glass‐like films. They decompose at temperatures as high as 485–545 °C. At a constant current density of 25 mA cm^?2, an ITO/BN₃/Al single‐layer device has a much‐longer lifetime (>80 h) than that of an ITO/NPB/Al single‐layer device (8 h). Also, the lifetime of a multilayer device based on BN₁ is longer than a similar device based on NPB. BNs are efficient and versatile OLED materials: they can be used as a hole‐transport layer (HTL), a host, and a deep‐blue‐light‐emitting material. This versatility may cut the cost of large‐scale material manufacture. More importantly, the deep‐blue electroluminescence (emission peak at 444 nm with CIE coordinates (0.16, 0.11), 3.23 cd A^?1 at 0.21 mA cm^?2, and 25200 cd m^?2 at 9 V) remains very stable at very high current densities up to 1000 mA cm^?2.     

Interlayer Engineering with Different Host Material Properties in Blue Phosphorescent Organic Light‐Emitting Diodes

We investigated the light‐emitting performances of blue phosphorescent organic light‐emitting diodes, known as PHOLEDs, by incorporating an N,N’‐dicarbazolyl‐3,5‐benzen interlayer between the hole transporting layer and emitting layer (EML). We found that the effects of the introduced interlayer for triplet exciton confinement and hole/electron balance in the EML were exceptionally dependent on the host materials: 9‐(4‐tert‐butylphenyl)‐3.6‐bis(triphenylsilyl)‐9H‐carbazole, 9‐(4‐tert‐butylphenyl)‐3.6‐ditrityl‐9H‐carbazole, and 4,4’‐bis‐triphenylsilanyl‐biphenyl. When an appropriate interlayer and host material were combined, the peak external quantum efficiency was greatly enhanced by over 21 times from 0.79% to 17.1%. Studies on the recombination zone using a series of host materials were also conducted.     

Highly Efficient Greenish‐Yellow Phosphorescent Organic Light‐Emitting Diodes Based on Interzone Exciton Transfer

Phosphorescent organic light emitting diodes (PHOLEDs) have undergone tremendous growth over the past two decades. Indeed, they are already prevalent in the form of mobile displays, and are expected to be used in large‐area flat panels recently. To become a viable technology for next generation solid‐state light source however, PHOLEDs face the challenge of achieving concurrently a high color rendering index (CRI) and a high efficiency at high luminance. To improve the CRI of a standard three color white PHOLED, one can use a greenish‐yellow emitter to replace the green emitter such that the gap in emission wavelength between standard green and red emitters is eliminated. However, there are relatively few studies on greenish‐yellow emitters for PHOLEDs, and as a result, the performance of greenish‐yellow PHOLEDs is significantly inferior to those emitting in the three primary colors, which are driven strongly by the display industry. Herein, a newly synthesized greenish‐yellow emitter is synthesized and a novel device concept is introduced featuring interzone exciton transfer to considerably enhance the device efficiency. In particular, high external quantum efficiencies (current efficiencies) of 21.5% (77.4 cd/A) and 20.2% (72.8 cd/A) at a luminance of 1000 cd/m² and 5000 cd/m², respectively, have been achieved. These efficiencies are the highest reported to date for greenish‐yellow emitting PHOLEDs. A model for this unique design is also proposed. This design could potentially be applied to enhance the efficiency of even longer wavelength yellow and red emitters, thereby paving the way for a new avenue of tandem white PHOLEDs for solid‐state lighting.     

Highly Branched Phosphorescent Dendrimers for Efficient Solution‐Processed Organic Light‐Emitting Diodes

Intermolecular interactions play a crucial role in the performance of organic light‐emitting diodes (OLEDs). Here we report the photophysical and electroluminescence properties of a fac‐tris(2‐phenylpyridyl)iridium(III ) cored dendrimer in which highly branched biphenyl dendrons are used to control the intermolecular interactions. The presence of fluorene surface groups improves the solubility and enhances the efficiency of photoluminescence, especially in the solid state. The emission peak of the dendrimer is around 530 nm with a PL quantum yield of 76 % in solution and 25 % in a film. The photophysical properties of this dendrimer are compared with a similar dendrimer with the same structure but without the fluorene surface groups. Dendrimer LEDs (DLEDs) are prepared using each dendrimer as a phosphorescent emitter blended in a 4,4′‐bis(N‐carbazolyl)biphenyl host. Device performance is improved significantly by the incorporation of an electron‐transporting layer of 1,3,5‐tris(2‐N‐phenylbenzimidazolyl)benzene. A peak external quantum efficiency of 10 % (38 Cd A^–1) for the dendrimer without surface groups and 13 % (49.8 Cd A^–1) for the dendrimer with fluorene surface groups is achieved in the bilayer LEDs.     

n‐Doping of a Low‐Electron‐Affinity Polymer Used as an Electron‐Transport Layer in Organic Light‐Emitting Diodes

n‐Doping electron‐transport layers (ETLs) increases their conductivity and improves electron injection into organic light‐emitting diodes (OLEDs). Because of the low electron affinity and large bandgaps of ETLs used in green and blue OLEDs, n‐doping has been notoriously more difficult for these materials. In this work, n‐doping of the polymer poly[(9,9‐dioctylfluorene‐2,7‐diyl)‐alt‐(benzo[2,1,3]thiadiazol‐4,7‐diyl)] (F8BT) is demonstrated via solution processing, using the air‐stable n‐dopant (pentamethylcyclopentadienyl)(1,3,5‐trimethylbenzene)ruthenium dimer [RuCp*Mes]₂. Undoped and doped F8BT films are characterized using ultraviolet and inverse photoelectron spectroscopy. The ionization energy and electron affinity of the undoped F8BT are found to be 5.8 and 2.8 eV, respectively. Upon doping F8BT with [RuCp*Mes]₂, the Fermi level shifts to within 0.25 eV of the F8BT lowest unoccupied molecular orbital, which is indicative of n‐doping. Conductivity measurements reveal a four orders of magnitude increase in the conductivity upon doping and irradiation with ultraviolet light. The [RuCp*Mes]₂‐doped F8BT films are incorporated as an ETL into phosphorescent green OLEDs, and the luminance is improved by three orders of magnitude when compared to identical devices with an undoped F8BT ETL.     

Study of Configuration Differentia and Highly Efficient,Deep‐Blue,Organic Light‐Emitting Diodes Based on Novel Naphtho[1,2‐d]imidazole Derivatives

Two novel naphtho[1,2‐d]imidazole derivatives are developed as deep‐blue, light‐emitting materials for organic light‐emitting diodes (OLEDs). The 1H‐naphtho[1,2‐d]imidazole based compounds exhibit a significantly superior performance than the 3H‐naphtho[1,2‐d]imidazole analogues in the single‐layer devices. This is because they have a much higher capacity for direct electron‐injection from the cathode compared to their isomeric counterparts resulting in a ground‐breaking EQE (external quantum efficiency) of 4.37% and a low turn‐on voltage of 2.7 V, and this is hitherto the best performance for a non‐doped single‐layer fluorescent OLED. Multi‐layer devices consisting of both hole‐ and electron‐transporting layers, result in identically excellent performances with EQE values of 4.12–6.08% and deep‐blue light emission (Commission Internationale de l'Eclairage (CIE) y values of 0.077–0.115) is obtained for both isomers due to the improved carrier injection and confinement within the emissive layer. In addition, they showed a significantly better blue‐color purity than analogous molecules based on benzimidazole or phenanthro[9,10‐d]imidazole segments.