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.     

White Organic Light‐Emitting Diodes with Evenly Separated Red,Green, and Blue Colors for Efficiency/Color‐Rendition Trade‐Off Optimization

A novel yellowish‐green triplet emitter, bis(5‐(trifluoromethyl)‐2‐p‐tolylpyridine) (acetylacetonate)iridium(III) (1), was conveniently synthesized and used in the fabrication of both monochromatic and white organic light‐emitting diodes (WOLEDs). At the optimal doping concentration, monochromatic devices based on 1 exhibit a high efficiency of 63 cd A^?1 (16.3% and 36.6 lm W^?1) at a luminance of 100 cd m^?2. By combining 1 with a phosphorescent sky‐blue emitter, bis(3,5‐difluoro‐2‐(2‐pyridyl)phenyl)‐(2‐carboxypyridyl)iridium(III) (FIrPic), and a red emitter, bis(2‐benzo[b]thiophen‐2‐yl‐pyridine)(acetylacetonate)iridium(III) (Ir(btp)₂(acac)), the resulting electrophosphorescent WOLEDs show three evenly separated main peaks and give a high efficiency of 34.2 cd A^?1 (13.2% and 18.5 lm W^?1) at a luminance of 100 cd m^?2. When 1 is mixed with a deep‐blue fluorescent emitter, 4,4′‐bis(9‐ethyl‐3‐carbazovinylene)‐1,1′‐biphenyl (BCzVBi), and Ir(btp)₂(acac), the resulting hybrid WOLEDs demonstrate a high color‐rendering index of 91.2 and CIE coordinates of (0.32, 0.34). The efficient and highly color‐pure WOLEDs based on 1 with evenly separated red, green, blue peaks and a high color‐rendering index outperform those of the state‐of‐the‐art emitter, fac‐tris(2‐phenylpyridine)iridium(III) (Ir(ppy)₃), and are ideal candidates for display and lighting applications.     

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.     

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.     

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.     

A Bipolar Host Material Containing Triphenylamine and Diphenylphosphoryl‐Substituted Fluorene Units for Highly Efficient Blue Electrophosphorescence

Highly efficient blue electrophosphorescent organic light‐emitting diodes incorporating a bipolar host, 2,7‐bis(diphenylphosphoryl)‐9‐[4‐(N,N‐diphenylamino)phenyl]‐9‐phenylfluorene (POAPF), doped with a conventional blue triplet emitter, iridium(III) bis[(4,6‐difluoro‐phenyl)pyridinato‐N,C^2´]picolinate (FIrpic) are fabricated. The molecular architecture of POAPF features an electron‐donating (p‐type) triphenylamine group and an electron‐accepting (n‐type) 2,7‐bis(diphenyl‐phosphoryl)fluorene segment linked through the sp³‐hybridized C9 position of the fluorene unit. The lack of conjugation between these p‐ and n‐type groups endows POAPF with a triplet energy gap (E_T) of 2.75 eV, which is sufficiently high to confine the triplet excitons on the blue‐emitting guest. In addition, the built‐in bipolar functionality facilitates both electron and hole injection. As a result, a POAPF‐based device doped with 7 wt% FIrpic exhibits a very low turn‐on voltage (2.5 V) and high electroluminescence efficiencies (20.6% and 36.7 lm W^?1). Even at the practical brightnesses of 100 and 1000 cd m^?2, the efficiencies remain high (20.2%/33.8 lm W^?1 and 18.8%/24.3 lm W^?1, respectively), making POAPF a promising material for use in low‐power‐consumption devices for next‐generation flat‐panel displays and light sources.     

Efficient Bipolar Blue AIEgens for High‐Performance Nondoped Blue OLEDs and Hybrid White OLEDs

Blue organic luminescent materials play a crucial role in full‐color display and white lighting but efficient ones meeting commercial demands are very rare. Herein, the design and synthesis of tailor‐made bipolar blue luminogens with an anthracene core and various functional groups are reported. The thermal stabilities, photophysical properties, electronic structures, electrochemical behaviors, carrier transport abilities, and electroluminescence performances are systematically investigated. The luminogen TPE‐TAPBI containing a tetraphenylethene moiety shows aggregation‐induced emission, while another luminogen TriPE‐TAPBI bearing a triphenylethene unit exhibits light aggregation‐caused quenching. In comparison with TriPE‐TAPBI, TPE‐TAPBI has stronger blue emission in neat film and functions more efficiently in nondoped organic light‐emitting diodes (OLEDs). High maxima current, power, and external quantum efficiencies of 7.21 cd A^?1, 6.78 lm W^?1, and 5.73%, respectively, are attained by the nondoped blue OLED of TPE‐TAPBI (CIE_x,y = 0.15, 0.16). Moreover, efficient two‐color hybrid warm white OLEDs (CIE_x,y = 0.457, 0.470) are achieved using TPE‐TAPBI neat film as the blue‐emitting component, which provide total current, power, external quantum efficiencies of up to 70.5 lm W^?1, 76.0 cd A^?1, and 28% at 1000 cd m^?2, respectively. These blue and white OLEDs are among the most efficient devices with similar colors in the literature.     

High Efficiency White Organic Light‐Emitting Devices Incorporating Yellow Phosphorescent Platinum(II) Complex and Composite Blue Host

A new class of charge neutral, strongly luminescent cyclometalated platinum(II) complexes supported by dianionic tetradentate ligand are synthesized. One of these platinum(II) complexes, Y‐Pt , displays a high photoluminescence quantum yield of 86% and electroluminescence efficacy (η_power) of up to 52 lm W^?1, and is utilized as a yellow phosphorescent dopant in the fabrication of white organic light‐emitting devices (WOLEDs). WOLEDs based on conventional structures with yellow emission from Y‐Pt in combination with blue emission from bis(4,6‐difluorophenyl‐pyridinato‐N,C²′) (picolinate) iridium(III) (FIrpic) show a total η_power of up to 31 lm W^?1. A two‐fold increase in η_power by utilizing a modified WOLED structure comprising of a composite blue host is realized. With this modified device structure, the total η_power and driving voltage at a luminance of 1000 cd m^?2 can be improved to 61 lm W^?1 and 7.5 V (i.e., 10 V for control devices). The performance improvement is attributed to an effectively broaden exciton formation‐recombination zone and alleviation of localized exciton accumulation within the FIrpic‐doped composite host for reduced triplet‐triplet annihilation, yielding blue light‐emission with enhanced intensity. The modified device structure can also adopt a higher concentration of Y‐Pt towards its optimal value, leading to WOLEDs with high efficiency.     

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.     

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.     

High‐Efficiency Deep‐Blue Light‐Emitting Diodes Based on Phenylquinoline/Carbazole‐Based Compounds

Highly efficient deep‐blue fluorescent materials based on phenylquinoline–carbazole derivatives (PhQ‐CVz, MeO‐PhQ‐CVz, and CN‐PhQ‐CVz) are synthesized for organic light‐emitting diodes (OLEDs). The materials form high‐quality amorphous thin films by thermal evaporation and the energy levels can be easily adjusted by the introduction of different electron‐donating and electron‐withdrawing groups on carbazoylphenylquinoline. Non‐doped deep‐blue OLEDs that use PhQ‐CVz as the emitter show bright emission (Commission Internationale de L'Éclairage (CIE) coordinates, x = 0.156, y = 0.093) with an external quantum efficiency of 2.45%. Furthermore, the material works as an excellent host material for 4,4′‐bis(9‐ethyl‐3‐carbazovinylene)‐1,1′‐biphenyl dopant to get high‐performance OLEDs with excellent deep‐blue CIE coordinates (x = 0.155, y = 0.157), high power efficiency (5.98 lm W^?1), and high external quantum efficiency (5.22%).     

Tilted Spiro‐Type Thermally Activated Delayed Fluorescence Host for ≈100% Exciton Harvesting in Red Phosphorescent Electronics with Ultralow Doping Ratio

Despite promising efficiency, the high fabrication cost due to the required high concentrations of noble metal based phosphors is still problematic for phosphorescent organic light‐emitting diodes (PhOLEDs). This situation becomes even serious considering some practical applications need high luminance, which in turn requires a higher concentration of emitters. A paradigm shift to circumvent these issues can be development of materials that are able to operate efficiently in very low concentrations ( < 1 wt%). Here, two thermally activated delayed fluorescence hosts ( OSTFPCN and OSTFPB ) with tilted spiro geometry, small singlet‐triplet splitting ( Δ E _st), and effective resonance energy transfer are developed. Within expectation, record performances with a power efficiency of 63.6 lm W^?1 and an external quantum efficiency (EQE) of 31.2% for the red phosphor Ir(MDQ)₂(acac) (2.0 wt%) are achieved with OSTFPCN as host. Additionally, a high power efficiency around 58 lm W^?1 is also gained even at an ultralow dopant concentration of 0.5 wt% for a OSTFPB based device. Mechanism studies demonstrate that efficiency roll‐off can be effectively suppressed in such low concentrations. These findings pave a new way to exploit low cost and high efficiency PhOLEDs.     

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.     

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.     

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.     

Spin‐Coated Highly Efficient Phosphorescent Organic Light‐Emitting Diodes Based on Bipolar Triphenylamine‐Benzimidazole Derivatives

A new series of star‐shaped bipolar host molecules, tris(4′‐(1‐phenyl‐1H‐benzimidazol‐2‐yl)biphen‐yl‐4‐yl) amine (TIBN), tris(2′‐methyl‐4′‐(1‐phenyl‐1H‐benzimida zol‐2‐yl)biphenyl‐4‐yl)amine (Me‐TIBN), and tris(2,2′‐dimethyl‐4′‐(1‐phenyl‐1H‐benzimidazol‐2‐yl)biphenyl‐4‐yl)amine (DM‐TIBN), that contain hole‐transporting triphenylamine and electron‐transporting benzimidazole moieties are designed based on calculations using density functional theory and successfully prepared. The theoretical calculation of energy levels of TIBN derivatives affords helpful ideas to design molecules with a favorable localization of highest occupied/lowest unoccupied molecular orbital (HOMO/LUMO) levels and a predefined enhancement of the triplet energy gap. The TIBN derivatives are employed as hosts to fabricate phosphorescent organic light‐emitting diodes (OLEDs) by the two methods of spin‐coating and vacuum deposition. Notably, the spin‐coated Me‐TIBN and DM‐TIBN devices exhibit a much better performance than the vacuum‐deposited ones, in which the spin‐coated DM‐TIBN device (47 500 cd m^?2, 27.3 cd A^?1, 7.3 lm W^?1) is outstanding with respect to other seminal work for solution‐processed OLEDs. More importantly, the new concept of localizing HOMO and LUMO levels for bipolar molecules is illustrated, and a facile strategy to tailor the energy levels by breaking the conjugation of hole‐ and electron‐transporting moieties is demonstrated.     

Color Tuning and Highly Efficient Blue Emitters of Finite Diphenylamino‐Containing Oligo(arylenevinylene) Derivatives Using Fluoro Substituents

New fluoro derivatives of Ph₂N‐containing (Ph: phenyl) oligo(arylenevinylene) derivatives are prepared by using double Heck‐coupling reactions or Horner–Wadsworth–Emmons reactions. These oligomers are highly fluorescent (fluorescence quantum yields Φ = 0.93–0.68) with emissions in a broad wavelength region (448–579 nm), depending on the position of the fluoro substituents. The highest occupied and lowest unoccupied molecular orbital (HOMO–LUMO) energy levels of these oligomers are characterized by electrochemistry and UV spectroscopy. The effects of the fluoro substituents on the energy levels are rationalized with HOMO–LUMO simulations. In a classical organic light emitting diode (OLED), one representative ( 5a ) shows a remarkable external quantum efficiency value (η_ext = 4.87 %) at J = 20 mA cm^–2; the maximum brightness at 10.2 V is 22 506 cd m^–2 (λ = 458 nm; Commission Internationale de l'Eclairage (CIE) coordinates x = 0.14, y = 0.14) with a full width at half‐maximum of 54 nm, demonstrating the superiority of these fluoro‐containing oligomers in OLED devices.     

Highly Efficient Non‐Doped Blue Organic Light‐Emitting Diodes Based on Fluorene Derivatives with High Thermal Stability

A new series of blue‐light‐emitting fluorene derivatives have been synthesized and characterized. The fluorene derivatives have high fluorescence yields, good thermal stability, and high glass‐transition temperatures in the range 145–193 °C. Organic light‐emitting diodes (OLEDs) fabricated using the fluorene derivatives as the host emitter show high efficiency (up to 5.3 cd A^–1 and 3.0 lm W^–1) and bright blue‐light emission (Commission Internationale de L'Eclairage (CIE) coordinates of x = 0.16, y = 0.22). The performance of the non‐doped fluorene‐based devices is among the best fluorescent blue‐light‐emitting OLEDs. The good performance of the present blue OLEDs is considered to derive from: 1) appropriate energy levels of the fluorene derivatives for good carrier injection; 2) good carrier‐transporting properties; and 3) high fluorescence efficiency of the fluorene derivatives. These merits are discussed in terms of the molecular structures.     

White Electroluminescence from a Single‐Polymer System with Simultaneous Two‐Color Emission: Polyfluorene as the Blue Host and a 2,1,3‐Benzothiadiazole Derivative as the Orange Dopant

New single‐polymer electroluminescent systems containing two individual emission species—polyfluorenes as a blue host and 2,1,3‐benzothiadiazole derivative units as an orange dopant on the main chain—have been designed and synthesized. The resulting single polymers are found to have highly efficient white electroluminescence with simultaneous blue (λ_max = 421 nm/445 nm) and orange emission (λ_max = 564 nm) from the corresponding emitting species. The influence of the photoluminescence (PL) efficiencies of both the blue and orange species on the electroluminescence (EL) efficiencies of white polymer light‐emitting diodes (PLEDs) based on the single‐polymer systems has been investigated. The introduction of the highly efficient 4,7‐bis(4‐(N‐phenyl‐N‐(4‐methylphenyl)amino)phenyl)‐2,1,3‐benzothiadiazole unit to the main chain of polyfluorene provides significant improvement in EL efficiency. For a single‐layer device fabricated in air (indium tin oxide/poly(3,4‐ethylenedioxythiophene): poly(styrene sulfonic acid/polymer/Ca/Al), pure‐white electroluminescence with Commission Internationale de l'Eclairage (CIE) coordinates of (0.35,0.32), maximum brightness of 12 300 cd m^–2, luminance efficiency of 7.30 cd A^–1, and power efficiency of 3.34 lm W^–1 can be obtained. This device is approximately two times more efficient than that utilizing a single polyfluorene containing 1,8‐naphthalimide moieties, and shows remarkable improvement over the corresponding blend systems in terms of efficiency and color stability. Thermal treatment of the single‐layer device before cathode deposition leads to the further improvement of the device performance, with CIE coordinates of (0.35,0.34), turn‐on voltage of 3.5 V, luminance efficiency of 8.99 cd A^–1, power efficiency of 5.75 lm W^–1, external quantum efficiency of 3.8 %, and maximum brightness of 12 680 cd m^–2. This performance is roughly comparable to that of white organic light‐emitting diodes (WOLEDs) with multilayer device structures and complicated fabrication processes.     

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.