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.     

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.     

High‐Performance Red,Green, and Blue Electroluminescent Devices Based on Blue Emitters with Small Singlet–Triplet Splitting and Ambipolar Transport Property

Two coordination complex emitters as well as host materials Be(PPI)₂ and Zn(PPI)₂ (PPI = 2‐(1‐phenyl‐1H‐phenanthro[9,10‐d]imidazol‐2‐yl)phenol) are designed, synthesized, and characterized. The incorporation of the metal atom leads to a twisted conformation and rigid molecular structure, which improve the thermal stability of Be(PPI)₂ and Zn(PPI)₂ with high T_d and T_g at around 475 and 217 °C, respectively. The introduction of the electron‐donating phenol group results in the emission color shifting to the deep‐blue region and the emission maximum appears at around 429 nm. This molecular design strategy ensures that the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) HOMO and LUMO of Be(PPI)₂ and Zn(PPI)₂ localize on the different moieties of the molecules. Therefore, the two complexes have an ambipolar transport property and a small singlet–triplet splitting of 0.35 eV for Be(PPI)₂ and 0.21 eV for Zn(PPI)₂. An undoped deep‐blue fluorescent organic light‐emitting device (OLED) that uses Be(PPI)₂ as emitter exhibits a maximum power efficiency of 2.5 lm W^?1 with the CIE coordinates of (0.15, 0.09), which are very close to the National Television Standards Committee (NTSC) blue standard (CIE: 0.14, 0.08). Green and red phosphorescent OLEDs (PhOLEDs) that use Be(PPI)₂ and Zn(PPI)₂ as host materials show high performance. Highest power efficiencies of 67.5 lm W^?1 for green PhOLEDs and 21.7 lm W^?1 for red PhOLEDs are achieved. In addition, the Be(PPI)₂‐based devices show low‐efficiency roll‐off behavior, which is attributed to the more balanced carrier‐transport property of Be(PPI)₂.     

A Novel Fluorene‐Triphenylamine Hybrid That is a Highly Efficient Host Material for Blue‐, Green‐, and Red‐Light‐Emitting Electrophosphorescent Devices

TFTPA (tris[4‐(9‐phenylfluoren‐9‐yl)phenyl]amine), a novel host material that contains a triphenylamine core and three 9‐phenyl‐9‐fluorenyl peripheries, was effectively synthesized through a Friedel‐Crafts‐type substitution reaction. Owing to the presence of its sterically bulky 9‐phenyl‐9‐fluorenyl groups, TFTPA exhibits a high glass transition temperature (186 °C) and is morphologically and electrochemically stable. In addition, as demonstrated from atomic force microscopy measurements, the aggregation of the triplet iridium dopant is significantly diminished in the TFTPA host, resulting in a highly efficient full‐color phosphorescence. The performance of TFTPA ‐based devices is far superior to those of the corresponding mCP‐ or CBP‐based devices, particularly in blue‐ and red‐emitting electrophosphorescent device systems. The efficiency of the FIrpic‐based blue‐emitting device reached 12 % (26 cd A^–1) and 18 lm W^–1 at a practical brightness of 100 cd m^–2; the Ir(piq)₂acac‐based red‐emitting device exhibited an extremely low turn‐on voltage (2.6 V) and a threefold enhancement in device efficiency (9.0 lm W^–1) relative to those of reference devices based on the CBP host material.     

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.     

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.     

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.     

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.     

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.     

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.     

Carbazole-bridged triphenylamine-bipyridine bipolar hosts for high-efficiency low roll-off multi-color PhOLEDs

Three new bipolar molecules composed of carbazole, triarylamine, and bipyridine were synthesized and utilized as host materials in multi-color phosphorescent OLEDs (PhOLEDs). These carbazole-based materials comprise a hole-transport triarylamine at C3 and an electron-transport 2,4′- or 4,4′-bipyridine at N9. The different bipyridine isomers and linking topology of the bipyridine with respect to carbazole N9 not only allows fine-tuning of physical properties but also imparts conformational change which subsequently affects molecular packing and carrier transport properties in the solid state. PhOLEDs were fabricated using green [(ppy)₂Ir(acac)], yellow [(bt)₂Ir(acac)], and red [(mpq)₂Ir(acac)] as doped emitters, which showed low driving voltage, high external quantum efficiency (EQE), and extremely low efficiency roll-off. Among these new bipolar materials, the 2Cz-44Bpy-hosted device doping with 10% (ppy)₂Ir(acac) as green emitting layer showed a high EQE of 22% (79.8 cd A⁻¹) and power efficiency (PE) of 102.5 lm W⁻¹ at a practical brightness of 100 cd m⁻². In addition, the device showed limited efficiency roll-off (21.6% EQE) and low driving voltage (2.8 V) at a practical brightness of 1000 cd m⁻².     

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.     

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.     

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.     

Doping‐Free Organic Light‐Emitting Diodes with Very High Power Efficiency,Simple Device Structure,and Superior Spectral Performance

Today's state‐of‐the‐art phosphorescent organic light‐emitting diodes (PhOLEDs) must rely on the host‐guest doping technique to decrease triplet quenching and increase device efficiency. However, doping is a sophisticated device fabrication process. Here, a Pt(II)‐based complex with a near unity photoluminescence quantum yield and excellent electron transporting properties in the form of neat film is reported. Simplified doping‐free white PhOLED and yellow‐orange PhOLED based on this emitter achieve rather low operating voltages (2.2–2.4 V) and very high power efficiencies of approximately 80 lm W^?1 (yellow‐orange) and 50 lm W^?1 (white), respectively, without any light extraction enhancement. Furthermore, the efficient white device also exhibits high color stability. No color shift is observed during the entire operation of the device. Analysis of the device's operational mechanism has been postulated in terms of exciton and polaron formation and fate. It is found that using the efficient neat Pt(II)‐complex as a homogeneous emitting and electron transporting layer and an ambipolar blue emitter are determining factors for achieving such a high efficiency.     

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.     

A Multifunctional Bipolar Luminogen with Delayed Fluorescence for High‐Performance Monochromatic and Color‐Stable Warm‐White OLEDs

Increasing exciton utilization and reducing exciton annihilation are crucial to achieve high performance of organic light‐emitting diodes (OLEDs), which greatly depend on molecular engineering of emitters and hosts. A novel luminogen (SBF‐BP‐DMAC) is synthesized and characterized. Its crystal and electronic structures, thermal stability, electrochemical behavior, carrier transport, photoluminescence, and electroluminescence are investigated. SBF‐BP‐DMAC exhibits enhanced photoluminescence and promotes delayed fluorescence in solid state and bipolar carrier transport ability, and thus holds multifunctionality of emitter and host for OLEDs. Using SBF‐BP‐DMAC as an emitter, the nondoped OLEDs exhibit maximum electroluminescence (EL) efficiencies of 67.2 cd A^?1, 65.9 lm W^?1, and 20.1%, and the doped OLEDs provide maximum EL efficiencies of 79.1 cd A^?1, 70.7 lm W^?1, and 24.5%. A representative orange phosphor, Ir(tptpy)₂acac, is doped into SBF‐BP‐DMAC for OLED fabrication, giving rise to superior EL efficiencies of 88.0 cd A^?1, 108.0 lm W^?1, and 26.8% for orange phosphorescent OLEDs, and forward‐viewing EL efficiencies of 69.3 cd A^?1, 45.8 lm W^?1, and 21.0% for two‐color hybrid warm‐white OLEDs. All of these OLEDs can retain high EL efficiencies at high luminance, with very small efficiency roll‐offs. The outstanding EL performance demonstrates the great potentials of SBF‐BP‐DMAC in practical display and lighting devices.     

Harvesting Excitons Via Two Parallel Channels for Efficient White Organic LEDs with Nearly 100% Internal Quantum Efficiency: Fabrication and Emission‐Mechanism Analysis

By incorporating two phosphorescent dyes, namely, iridium(III)[bis(4,6‐difluorophenyl)‐pyridinato‐N,C²′]picolinate (FIrpic) for blue emission and bis(2‐(9,9‐diethyl‐9H‐fluoren‐2‐yl)‐1‐phenyl‐1H‐benzoimidazol‐N,C³)iridium(acetylacetonate) ((fbi)₂Ir(acac)) for orange emission, into a single‐energy well‐like emissive layer, an extremely high‐efficiency white organic light‐emitting diode (WOLED) with excellent color stability is demonstrated. This device can achieve a peak forward‐viewing power efficiency of 42.5 lm W^?1, corresponding to an external quantum efficiency (EQE) of 19.3% and a current efficiency of 52.8 cd A^?1. Systematic studies of the dopants, host and dopant‐doped host films in terms of photophysical properties (including absorption, photoluminescence, and excitation spectra), transient photoluminescence, current density–voltage characteristics, and temperature‐dependent electroluminescence spectra are subsequently performed, from which it is concluded that the emission natures of FIrpic and (fbi)₂Ir(acac) are, respectively, host–guest energy transfer and a direct exciton formation process. These two parallel pathways serve to channel the overall excitons to both dopants, greatly reducing unfavorable energy losses. It is noteworthy that the introduction of the multifunctional orange dopant (fbi)₂Ir(acac) (serving as either hole‐trapping site or electron‐transporting channel) is essential to this concept as it can make an improved charge balance and broaden the recombination zone. Based on this unique working model, detailed studies of the slight color‐shift in this WOLED are performed. It is quantitatively proven that the competition between hole trapping on orange‐dopant sites and undisturbed hole transport across the emissive layer is the actual reason. Furthermore, a calculation of the fraction of trapped holes on (fbi)₂Ir(acac) sites with voltage shows that the hole‐trapping effect of the orange dopant is decreased with increasing drive voltage, leading to a reduction of orange emission.     

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.     

Cover Picture: 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 (Adv. Funct. Mater. 7/2006)

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 by Wang and co‐workers on p. 957. The resulting single polymers are found to have highly efficient white electroluminescence with simultaneous blue and orange emission from the corresponding emitting species. A single‐layer device has been fabricated that has performance characteristics roughly comparable to those of organic white‐light‐emitting diodes with multilayer device structures. 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.