m‐Indolocarbazole Derivative as a Universal Host Material for RGB and White Phosphorescent OLEDs

The host materials designed for highly efficient white phosphorescent organic light‐emitting diodes (PhOLEDs) with power efficiency (PE) >50 lm W^‐1 and low efficiency roll‐off are very rare. In this work, three new indolocarbazole‐based materials (ICDP, 4ICPPy, and 4ICDPy) are presented composed of 6,7‐dimethylindolo[3,2‐a]carbazole and phenyl or 4‐pyridyl group for hosting blue, green, and red phosphors. Among this three host materials, 4ICDPy‐based devices reveal the best electroluminescent performance with maximum external quantum efficiencies (EQEs) of 22.1%, 27.0%, and 25.3% for blue (FIrpic), green (fac‐Ir(ppy)₃), and red ((piq)₂Ir(acac)) PhOLEDs. A two‐color and single‐emitting‐layer white organic light‐emitting diode hosted by 4ICDPy with FIrpic and Ir(pq)₃ as dopants achieves high EQE of 20.3% and PE of 50.9 lm W^?1 with good color stability; this performance is among the best for a single‐emitting‐layer white PhOLEDs. All 4ICDPy‐based devices show low efficiency roll‐off probably due to the excellent balanced carrier transport arisen from the bipolar character of 4ICDPy.     

New Solution‐Processable Electron Transport Materials for Highly Efficient Blue Phosphorescent OLEDs

Several new solution‐processable organic semiconductors based on dendritic oligoquinolines were synthesized and were used as electron‐transport and hole‐blocking materials to realize highly efficient blue phosphorescent organic light‐emitting diodes (PhOLEDs). Various substitutions on the quinoline rings while keeping the central meta‐linked tris(quinolin‐2‐yl)benzene gave electron transport materials that combined wide energy gap (>3.3 eV), moderate electron affinity (2.55‐2.8 eV), and deep HOMO energy level (<‐6.08 eV) with electron mobility as high as 3.3 × 10^?3 cm² V^?1 s^?1. Polymer‐based PhOLEDs with iridium (III) bis(4,6‐(di‐fluorophenyl)pyridinato‐N,C^2′)picolinate (FIrpic) blue triplet emitter and solution‐processed oligoquinolines as the electron‐transport layers (ETLs) gave luminous efficiency of 30.5 cd A^?1 at a brightness of 4130 cd m^?2 with an external quantum efficiency (EQE) of 16.0%. Blue PhOLEDs incorporating solution‐deposited ETLs were over two‐fold more efficient than those containing vacuum‐deposited ETLs. Atomic force microscopy imaging shows that the solution‐deposited oligoquinoline ETLs formed vertically oriented nanopillars and rough surfaces that enable good ETL/cathode contacts, eliminating the need for cathode interfacial materials (LiF, CsF). These solution‐processed blue PhOLEDs have the highest performance observed to date in polymer‐based blue PhOLEDs.     

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.     

Bipolar Tetraarylsilanes as Universal Hosts for Blue,Green, Orange,and White Electrophosphorescence with High Efficiency and Low Efficiency Roll‐Off

A series of tetraarylsilane compounds, namely p‐BISiTPA ( 1 ), m‐BISiTPA ( 2 ), p‐OXDSiTPA ( 3 ), m‐OXDSiTPA ( 4 ), are designed and synthesized by incorporating electron‐donating arylamine and electron‐accepting benzimidazole or oxadiazole into one molecule via a silicon‐bridge linkage mode. Their thermal, photophysical and electrochemical properties can be finely tuned through the different groups and linking topologies. The para‐disposition compounds 1 and 3 display higher glass transition temperatures, slightly lower HOMO levels and triplet energies than their meta‐disposition isomers 2 and 4 , respectively. The silicon‐interrupted conjugation of the electron‐donating and electron‐accepting segments gives these materials the following advantages: i) relative high triplet energies in the range of 2.69–2.73 eV; ii) HOMO/LUMO levels of the compounds mainly depend on the electron‐donating and electron‐accepting groups, respectively; iii) bipolar transporting feature as indicated by hole‐only and electron‐only devices. These advantages make these materials ideal universal hosts for multicolor phosphorescent OLEDs. 1 and 3 have been demonstrated as universal hosts for blue, green, orange and white electrophosphorescence, exhibiting high efficiencies and low efficiency roll‐off. For example, the devices hosted by 1 achieve maximum external quantum efficiencies of 16.1% for blue, 22.7% for green, 20.5% for orange, and 19.1% for white electrophosphorescence. Furthermore, the external quantum efficiencies are still as high as 14.2% for blue, 22.4% for green, 18.9% for orange, and 17.4% for white electrophosphorescence at a high luminance of 1000 cd m^?2. The two‐color, all‐phosphor white device hosted by 3 acquires a maximum current efficiency of 51.4 cd A^?1, and a maximum power efficiency of 51.9 lm W^?1. These values are among the highest for single emitting layer white PhOLEDs reported till now.     

An Exciplex Forming Host for Highly Efficient Blue Organic Light Emitting Diodes with Low Driving Voltage

The exciplex forming co‐host with phosphorescent dopant system has potential to realize highly efficient phosphorescent organic light emitting didoes (PhOLEDs). However, the exciplex forming co‐host for blue phosphorescent OLEDs has been rarely introduced because of higher triplet level of the blue dopant than green and red dopants. In this work, a novel exciplex forming co‐host with high triplet energy level is developed by mixing a phosphine oxide based electron transporting material, PO‐T2T, and a hole transporting material, N,N′‐dicarbazolyl‐3,5‐benzene (mCP). Photo‐physical analysis shows that the exciplexes are formed efficiently in the host and the energy transfer from the exciplex to blue phosphorescent dopant (iridium(III)bis[(4,6‐difluorophenyl)‐pyridinato‐N,C2′]picolinate; FIrpic) is also efficient, enabling the triplet harvest without energy loss. As a result, an unprecedented high performance blue PhOLED with the exciplex forming co‐host is demonstrated, showing a maximum external quantum efficiency (EQE) of 30.3%, a maximum power efficiency of 66 lm W^?1, and low driving voltage of 2.75 at 100 cd m^?2, 3.29 V at 1000 cd m^?2, and 4.65 V at 10 000 cd m^?2, respectively. The importance of the exciton confinement in the exciplex forming co‐host is further investigated which is directly related to the performance of PhOLEDs.     

Solution‐Processible 2,2′‐Dimethyl‐biphenyl Cored Carbazole Dendrimers as Universal Hosts for Efficient Blue,Green, and Red Phosphorescent OLEDs

A series of solution‐processible 2,2′‐dimethyl‐biphenyl cored dendrimers, namely G1MP, G2MP, and G3MP, is designed and synthesized by tuning the generation of periphery carbazole dendron. The resulting dendrimers all show excellent solubility in common organic solvents, and their high‐quality thin films can be formed via spin‐coating with a root‐mean‐square roughness in the range of 0.38–0.54 nm. G3MP, which contains the third‐generation carbazole dendron, has the greatest potential among those made here as an ideal universal host for multicolored triplet emitters. G3MP exhibits good thermal stability, with a glass transition temperature of 368 °C, a triplet energy as high as 2.85 eV enough to prevent the loss of triplet excitons, and suitable HOMO/LUMO levels of –5.30/–2.11 eV to facilitate both hole and electron injection and transport. When using G3MP as the host, highly efficient deep‐blue, blue, green, and red phosphorescent organic light‐emitting diodes (PhOLEDs) are successfully demonstrated, revealing a maximum luminous efficiency up to 18.2, 28.2, 54.0, and 12.7 cd A^–1 with the corresponding Commission Internationale de L'Eclairage (CIE) coordinates of (0.15, 0.23), (0.15, 0.35), (0.38, 0.59), and (0.64, 0.34), respectively. The state‐of‐art performance indicates that dendritic hosts have a favorable prospect of applications in solution‐processed white PhOLEDs and full‐color displays.     

High‐Performance Organic Light‐Emitting Diodes Based on Intramolecular Charge‐Transfer Emission from Donor–Acceptor Molecules: Significance of Electron‐ Donor Strength and Molecular Geometry

Organic light‐emitting diodes based on intramolecular‐charge‐transfer emission from two related donor–acceptor (D–A) molecules, 3,7‐[bis(4‐phenyl‐2‐quinolyl)]‐10‐methylphenothiazine (BPQ‐MPT) and 3,6‐[bis(4‐phenyl‐2‐quinolyl)]‐9‐methylcarbazole (BPQ‐MCZ), were found to have electroluminescence (EL) efficiencies and device brightnesses that differ by orders of magnitude. High brightness (> 40 000 cd m^–2) and high efficiency (21.9 cd A^–1, 10.8 lm W^–1, 5.78 % external quantum efficiency (EQE) at 1140 cd m^–2) green EL was achieved from the BPQ‐MPT emitter, which has its highest occupied molecular orbital (HOMO) level at 5.09 eV and a nonplanar geometry. In contrast, diodes with much lower brightness (2290 cd m^–2) and efficiency (1.4 cd A^–1, 0.66 lm W^–1, 1.7 % EQE at 405 cd m^–2) were obtained from the BPQ‐MCZ emitter, which has its HOMO level at 5.75 eV and exhibits a planar geometry. Compared to BPQ‐MCZ, the higher‐lying HOMO level of BPQ‐MPT facilitates more efficient hole injection/transport and a higher charge‐recombination rate, while its nonplanar geometry ensures diode color purity. White EL was observed from BPQ‐MCZ diodes owing to a blue intramolecular charge‐transfer emission and a yellow–orange intermolecular excimer emission, enabled by the planar molecular geometry. These results demonstrate that high‐performance light‐emitting devices can be achieved from intramolecular charge‐transfer emission, while highlighting the critical roles of the electron‐donor strength and the molecular geometry of D–A molecules.     

Thermally Activated Delayed Fluorescence Material as Host with Novel Spiro‐Based Skeleton for High Power Efficiency and Low Roll‐Off Blue and White Phosphorescent Devices

Efficiency roll‐off in blue organic light‐emitting diodes especially at high brightness still remains a vital issue for which the excitons density‐dependent mechanism of host materials takes most responsibility. Additionally, the efficiency roll‐off leads to high power consumption and reduces the operating lifetime because higher driving voltage and current are required. Here, by subtly modifying the triphenylamine to oxygen‐bridged quasi‐planar structure, a novel thermally activated delayed fluorescence type blue host Tri‐o‐2PO is successfully developed. Efficiency roll‐off based on Tri‐o‐2PO is ultralow with external quantum efficiency (EQE) just dropping by around 2% in the high luminance range from 1000 cd m^?2 to 10 000 cd m^?2. As expected, low turn‐on voltage (≈2.9 V) of device is also achieved, which is close to the theory limit value (≈2.62 V). Super‐high power efficiency (≈60 lm W^?1) and EQE (>22%) are also achieved when utilizing Tri‐o‐2PO as host. Furthermore, two‐color warm‐white light with CIE of (0.45, 0.43) and correlated color temperature of 2921 K is also fabricated and a champion EQE of 21% is delivered. These excellent performances prove the strategy of bridging the triphenylamine to reduce ΔE_st is validated and suggest the great potential of this novel skeleton.     

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.     

Monothiatruxene‐Based,Solution‐Processed Green,Sky‐Blue,and Deep‐Blue Organic Light‐Emitting Diodes with Efficiencies Beyond 5% Limit

The development of blue materials with good efficiency, even at high brightness, with excellent color purity, simple processing, and high thermal stability assuring adequate device lifetime is an important remaining challenge for organic light‐emitting didoes (OLEDs) in displays and lightning applications. Furthermore, these various features are typically mutually exclusive in practice. Herein, four novel green and blue light‐emitting materials based on a monothiatruxene core are reported together with their photophysical and thermal properties, and performance in solution‐processed OLEDs. The materials show excellent thermal properties with high glass transition temperatures ranging from 171 to 336 °C and decomposition temperatures from 352 to 442 °C. High external quantum efficiencies of 3.7% for a deep‐blue emitter with CIE color co‐ordinates (0.16, 0.09) and 7% for green emitter with color co‐ordinates (0.22, 0.40) are achieved at 100 cd m^?2. The efficiencies observed are exceptionally high for fluorescent materials with photoluminescence quantum yields of 24% and 62%, respectively. The performance at higher brightness is very good with only 38% and 17% efficiency roll‐offs at 1000 cd m^?2. The results indicate that utilization of this unique molecular design is promising for efficient deep‐blue highly stable and soluble light‐emitting materials.     

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).     

Manipulation of Charge and Exciton Distribution Based on Blue Aggregation‐Induced Emission Fluorophors: A Novel Concept to Achieve High‐Performance Hybrid White Organic Light‐Emitting Diodes

The aggregation‐induced emission (AIE) phenomenon is important in organic light‐emitting diodes (OLEDs), for it can potentially solve the aggregation‐caused quenching problem. However, the performance of AIE fluorophor‐based OLEDs (AIE OLEDs) is unsatisfactory, particularly for deep‐blue devices (CIEy < 0.15). Here, by enhancing the device engineering, a deep‐blue AIE OLED exhibits low voltage (i.e., 2.75 V at 1 cd m^?2), high luminance (17 721 cd m^?2), high efficiency (4.3 lm W^?1), and low efficiency roll‐off (3.6 lm W^?1 at 1000 cd m^?2), which is the best deep‐blue AIE OLED. Then, blue AIE fluorophors, for the first time, have been demonstrated to achieve high‐performance hybrid white OLEDs (WOLEDs). The two‐color WOLEDs exhibit i) stable colors and the highest efficiency among pure‐white hybrid WOLEDs (32.0 lm W^?1); ii) stable colors, high efficiency, and very low efficiency roll‐off; or iii) unprecedented efficiencies at high luminances (i.e., 70.2 cd A^?1, 43.4 lm W^?1 at 10 000 cd m^?2). Moreover, a three‐color WOLED exhibits wide correlated color temperatures (10 690–2328 K), which is the first hybrid WOLED showing sunlight‐style emission. These findings will open a novel concept that blue AIE fluorophors are promising candidates to develop high‐performance hybrid WOLEDs, which have a bright prospect for the future displays and lightings.     

Great improvement of operation-lifetime for all-solution OLEDs with mixed hosts by blade coating

We investigated some effective device designs and fabrication methods for long operation-lifetime all-solution-processed Phosphorescent OLEDs (PhOLEDs) and fluorescent OLEDs with mixed-hosts system and thin Poly [(9, 9-dioctylfluorenyl-2, 7-diyl)-co-(4, 4′-(N-(4-sec-butylphenyl) diphenylamine)] (TFB). The all-solution-processed green PhOLEDs had high current efficiency (30.3 cd/A) and long operation-lifetime. The best half-lifetime of green PhOLEDs with thin HTL, MH-hosts EML and optimized deposition was 310 h at an initial luminance 1000 cd/m², 250 h at an initial luminance 500 cd/m² for green PhOLEDs with thin HTL, and MH-hosts EML, and the lifetime of triple layer PhOLEDs device was only 0.5 h for the same materials. The red PhOLEDs exhibited a high current efficiency (10.93 cd/A) and half-lifetime with 157.9 h at an initial luminance 500 cd/m². For the blue fluorescent OLEDs, the thin polymer TFB, mixed-hosts EML, double EMLs and optimization deposition yield a high current efficiency (5.68 cd/A) and long operation-lifetime with 117.7 h at an initial luminance 500 cd/m². Single host fluorescent device had half-lifetime of 73.5 h only at an initial luminance 100 cd/m². Finally, by doping red emitter Rubrene into stable blue device, we achieved soft yellow OLEDs with high efficiency (10.87 cd/A) and 8 fold improvement operation-lifetime (1200 h). We believe that such all-solution-processed OLEDs which showed greatly improved operational lifetimes would be suitable for the indoor supportive lighting with natural colors.     

Fluorene‐Based Asymmetric Bipolar Universal Hosts for White Organic Light Emitting Devices

Two new bipolar host molecules composed of hole‐transporting carbazole and electron‐transporting cyano ( CzFCN ) or oxadiazole ( CzFOxa )‐substituted fluorenes are synthesized and characterized. The non‐conjugated connections, via an sp³‐hybridized carbon, effectively block the electronic interactions between electron‐donating and ‐accepting moieties, giving CzFCN and CzFOxa bipolar charge transport features with balanced mobilities (10^?5 to 10^?6 cm² V^?1 s^?1). The meta–meta configuration of the fluorene‐based acceptors allows the bipolar hosts to retain relatively high triplet energies [E_T = 2.70 eV ( CzFOxa ) and 2. 86 eV ( CzFCN )], which are sufficiently high for hosting blue phosphor. Using a common device structure – ITO/PEDOT:PSS/DTAF/TCTA/host:10% dopants (from blue to red)/DPPS/LiF/Al – highly efficient electrophosphorescent devices are successfully achieved. CzFCN ‐based devices demonstrate better performance characteristics, with maximum η_ext of 15.1%, 17.9%, 17.4%, 18%, and 20% for blue (FIrpic), green [(PPy)₂Ir(acac)], yellowish‐green [m‐(Tpm)₂Ir(acac)], yellow [(Bt)₂Ir(acac)], and red [Os(bpftz)₂(PPhMe₂)₂, OS1], respectively. In addition, combining yellowish‐green m‐(Tpm)₂Ir(acac) with a blue emitter (FIrpic) and a red emitter (OS1) within a single emitting layer hosted by bipolar CzFCN , three‐color electrophosphorescent WOLEDs with high efficiencies (17.3%, 33.4 cd A^?1, 30 lm W ^?1), high color stability, and high color‐rendering index (CRI) of 89.7 can also be realized.     

Multifunctional Fluorene‐Based Oligomers with Novel Spiro‐Annulated Triarylamine: Efficient,Stable Deep‐Blue Electroluminescence,Good Hole Injection,and Transporting Materials with Very High Tg

A series of fluorene‐based oligomers with novel spiro‐annulated triarylamine structures, namely DFSTPA, TFSTPA, and TFSDTC, are synthesized by a Suzuki cross‐coupling reaction. The spiro‐configuration molecular structures lead to very high glass transition temperatures (197–253 °C) and weak intermolecular interactions, and consequently the structures retain good morphological stability and high fluorescence quantum efficiencies(0.69–0.98). This molecular design simultaneously solves the spectral stability problems and hole‐injection and transport issues for fluorene‐based blue‐light‐emitting materials. Simple double‐layer electroluminescence (EL) devices with a configuration of ITO/TFSTPA (device A) or TFSDTC (device B)/ TPBI/LiF/Al, where TFSTPA and TFSDTC serve as hole‐transporting blue‐light‐emitting materials, show a deep‐blue emission with a peak around 432 nm, and CIE coordinates of (0.17, 0.12) for TFSTPA and (0.16, 0.07) for TFSDTC, respectively, which are very close to the National Television System Committee (NTSC) standard for blue (0.15, 0.07). The maximum current efficiency/external quantum efficiencies are 1.63 cd A^?1/1.6% for device A and 1.91 cd A^?1/2.7% for device B, respectively. In addition, a device with the structure ITO/DFSTPA/Alq₃/LiF/Al, where DFSTPA acts as both the hole‐injection and ‐transporting material, is shown to achieve a good performance, with a maximum luminance of 14 047 cd m^?2, and a maximum current efficiency of 5.56 cd A^?1. These values are significantly higher than those of devices based on commonly usedN,N′‐di(1‐naphthyl)‐N,N′‐diphenyl‐[1,1′‐biphenyl]‐4,4′‐diamine (NPB) as the hole‐transporting layer (11 738 cd m^?2 and 3.97 cd A^?1) under identical device conditions.     

Utilizing a Spiro TADF Moiety as a Functional Electron Donor in TADF Molecular Design toward Efficient “Multichannel” Reverse Intersystem Crossing

Designing thermally activated delayed fluorescence (TADF) materials with an efficient reverse intersystem crossing (RISC) process is regarded as the key to actualize efficient organic light‐emitting diodes (OLEDs) with low efficiency roll‐off. Herein, a novel molecular design strategy is reported where a typical TADF material 10‐phenyl‐10H, 10′H‐spiro[acridine‐9, 9′‐anthracen]‐10′‐one (ACRSA) is utilized as a functional electron donor to design TADF materials of 2,4,6‐triphenyl‐1,3,5‐triazine(TRZ)‐p‐ACRSA and TRZ‐m‐ACRSA. It is unique that the intramolecular charge transfer of the ACRSA moiety and the intramolecular and through‐space intermolecular charge transfer between the TRZ and ACRSA moieties, provide a “multichannel” effect to enhance the rate of the reverse intersystem crossing process (k_risc) exceeding 10^?6 s^?1. TADF OLEDs based on TRZ‐p‐ACRSA as an emitter show a maximum external quantum efficiency (EQE) of 28% with reduced efficiency roll‐off (EQEs of 27.5% and 22.1% at 100 and 1000 cd m^?2, respectively). Yellow phosphorescent OLEDs utilizing TRZ‐p‐ACRSA as a host material show record‐high EQE of 25.5% and power efficiency of 115 lm W^?1, while phosphorescent OLEDs based on TRZ‐m‐ACRSA show further lower efficiency roll‐off with EQEs of 25.2%, 24.3%, and 21.5% at 100, 1000, and 10 000 cd m^?2, respectively.     

Efficiency Roll‐Off in Blue Emitting Phosphorescent Organic Light Emitting Diodes with Carbazole Host Materials

The efficiency roll‐off in blue phosphorescent organic light emitting diodes (OLEDs) using different carbazole compounds as the host is systematically studied. While there is no significant difference in device efficiency, OLEDs using ter‐carbazole as the host show a reduction in efficiency roll‐off at high luminance. Data from transient photoluminescence and electroluminescence measurements show that the lower triplet–triplet annihilation (TTA) and triplet–polaron quenching (TPQ) rates in devices with the ter‐carbazole host compared with other carbazole hosts are the reasons for this reduced efficiency roll‐off. It is also found that the host materials with low glass transition temperatures are more susceptible to the efficiency roll‐off problem.     

Efficient Nondoped Blue Fluorescent Organic Light‐Emitting Diodes (OLEDs) with a High External Quantum Efficiency of 9.4% @ 1000 cd m−2 Based on Phenanthroimidazole−Anthracene Derivative

Organic light‐emitting diodes (OLEDs) can promise flexible, light weight, energy conservation, and many other advantages for next‐generation display and lighting applications. However, achieving efficient blue electroluminescence still remains a challenge. Though both phosphorescent and thermally activated delayed fluorescence materials can realize high‐efficiency via effective triplet utilization, they need to be doped into appropriate host materials and often suffer from certain degree of efficiency roll‐off. Therefore, developing efficient blue‐emitting materials suitable for nondoped device with little efficiency roll‐off is of great significance in terms of practical applications. Herein, a phenanthroimidazole?anthracene blue‐emitting material is reported that can attain high efficiency at high luminescence in nondoped OLEDs. The maximum external quantum efficiency (EQE) of nondoped device is 9.44% which is acquired at the luminescence of 1000 cd m^?2. The EQE is still as high as 8.09% even the luminescence reaches 10 000 cd m^?2. The maximum luminescence is ≈57 000 cd m^?2. The electroluminescence (EL) spectrum shows an emission peak of 470 nm and the Commission International de L'Eclairage (CIE) coordinates is (0.14, 0.19) at the voltage of 7 V. To the best of the knowledge, this is among the best results of nondoped blue EL devices.     

Thermally Activated Delayed Fluorescence Conjugated Polymers with Backbone‐Donor/Pendant‐Acceptor Architecture for Nondoped OLEDs with High External Quantum Efficiency and Low Roll‐Off

Most thermally activated delayed fluorescence (TADF) emitters have to be doped in the host for fabricating efficient organic light‐emitting diodes (OLEDs) and always suffer from quick efficiency roll‐off at high brightness, which severely affect their commercial application in display and lighting fields. In the work, a series of the polymers are synthesized by copolymerization of two carbazole monomers and one acridine derivative monomer containing benzophenone acceptor group. The obtained polymers therefore possess a conjugated backbone with carbazole/acridine moieties and benzophenone pendant to form the twisted donor/acceptor structure. Consequently, the TADF features inherited from the acridine derivative are maintained and improved by managing the content of acridine derivative monomer in the polymers. Solution‐processed OLEDs obtained from using neat polymer films exhibit comparable performance with organic TADF small molecules, achieving a maximum external quantum efficiency (EQE) of 18.1% and a very slow roll‐off with EQE of 17.8% at the luminance of 1000 cd m⁻².     

Highly Efficient Simple‐Structure Blue and All‐Phosphor Warm‐White Phosphorescent Organic Light‐Emitting Diodes Enabled by Wide‐Bandgap Tetraarylsilane‐Based Functional Materials

Two host materials of {4‐[diphenyl(4‐pyridin‐3‐ylphenyl)silyl]phenyl}diphenylamine (p‐PySiTPA) and {4‐[[4‐(diphenylphosphoryl)phenyl](diphenyl)silyl]phenyl}diphenylamine (p‐POSiTPA), and an electron‐transporting material of [(diphenylsilanediyl)bis(4,1‐phenylene)]bis(diphenylphosphine) dioxide (SiDPO) are developed by incorporating appropriate charge transporting units into the tetraarylsilane skeleton. The host materials feature both high triplet energies (ca. 2.93 eV) and ambipolar charge transporting nature; the electron‐transporting material comprising diphenylphosphine oxide units and tetraphenylsilane skeleton exhibits a high triplet energy (3.21 eV) and a deep highest occupied molecular orbital (HOMO) level (‐6.47 eV). Using these tetraarylsilane‐based functional materials results in a high‐efficiency blue phosphorescent device with a three‐organic‐layer structure of 1,1‐bis[4‐[N,N‐di(p‐tolyl)‐amino]phenyl]cyclohexane (TAPC)/p‐POSiTPA: iridium(III) bis(4′,6′‐difluorophenylpyridinato)tetrakis(1‐pyrazolyl)borate (FIr6)/SiDPO that exhibits a forward‐viewing maximum external quantum efficiency (EQE) up to 22.2%. This is the first report of three‐organic‐layer FIr6‐based blue PhOLEDs with the forward‐viewing EQE over 20%, and the device performance is among the highest for FIr6‐based blue PhOLEDs even compared with the four or more than four organic‐layer devices. Furthermore, with the introduction of bis(2‐(9,9‐diethyl‐9H‐fluoren‐2‐yl)‐1‐phenyl‐1H‐benzoimidazol‐N,C³)iridium acetylacetonate [(fbi)₂Ir(acac)] as an orange emitter, an all‐phosphor warm‐white PhOLED achieves a peak power efficiency of 47.2 lm W^?1, which is close to the highest values ever reported for two‐color white PhOLEDs.