A Highly Efficient Host/Dopant Combination for Blue Organic Electrophosphorescence Devices

We have synthesized a new blue‐emitting iridium complex, FIrpytz (iridium(III) bis(4,6‐difluorophenylpyridinato)‐4‐(pyridin‐2‐yl)‐1,2,3‐triazolate), and two new bis(triphenylsilyl) derivatives, BSB (4,4'‐bis‐triphenylsilanyl‐biphenyl) and BST (4,4″‐bis(triphenylsilanyl)‐(1,1′,4′,1″)‐terphenyl) as hosts for blue phosphorescence devices. The photoluminescence (PL) and electroluminescence (EL) properties of different host/dopant combinations were studied in details. These two arylsilanes showed glass transition temperatures (T_gs) ≥ 100 °C higher than those of UGH1 (diphenyl‐di(o‐tolyl)silane) and UGH2 (1,4‐bis(triphenylsilyl)benzene), the common arylsilane‐based hosts. The band gaps for BSB and BST are 4.16 and 3.78 eV, respectively, lower than that of UGH2 of 4.40 eV. The FIrpytz‐doped UGH2, BSB and BST films exhibit PL quantum yields of 0.58, 0.83 and 0.48, respectively. The EL devices using FIrpytz or FIrpic (iridium(III) bis(4,6‐difluorophenylpyridinato)‐picolinate) as the blue phosphorescence dopants and UGH2, BSB and BST as the hosts also showed that BSB‐based devices gave the best device efficiencies. Both PL and EL studies show that BSB is better than UGH2 and BST as the host material for FIrpytz and FIrpic. In particular, the use of FIrpytz as dopant, BSB as host and LiF/Al as cathode provides a remarkably efficient combination for blue electrophosphorescence device reaching a very high external quantum efficiency of 19.3% at 8.5 V and a high luminance level of 20500 cd m⁻² at 19.3 V after electroluminescence started at 5.1 V.     

Highly Efficient and Robust Blue Phosphorescent Pt(II) Compounds with a Phenyl‐1,2,3‐triazolyl and a Pyridyl‐1,2,4‐triazolyl Chelate Core

A new class of brightly phosphorescent Pt(II) compounds that contain an N^∧C‐chelate phenyl‐1,2,3‐triazolyl ligand (ptrz) and an N^∧C‐chelate pyridyl‐1,2,4‐triazolyl ligand (pytrz) in the central core is achieved. The impact of various substituent groups on phosphorescence of this class of molecules is examined. Crystal structural analyses revealed that this class of compounds has a great tendency to form stacked dimers—one of which is persistent even in the gas phase—leading to excimer emission. The introduction of bulky substituents, such as diphenyl amino (NPh₂) or trityl (CPh₃), is found to greatly diminish the excimer emission. Using this approach, several highly efficient blue and green phosphorescent Pt(II) compounds with λ_em at ≈450–460 nm and Φ_p ≈ 0.70 to 1.00 are obtained. These molecules are highly robust with exceptionally high thermal stability. Bright bluish‐green electrophosphorescent devices with external quantum efficiencies as high as 16.7% are fabricated.     

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.     

Effect of Electric Field on Coulomb‐Stabilized Excitons in Host/Guest Systems for Deep‐Blue Electrophosphorescence

Here, a study of the electric field induced quenching on the phosphorescence intensity of a deep‐blue triplet emitter dispersed in different host materials is presented. The hosts are characterized by a higher triplet excitonic level with respect to the emitter, ensuring efficient energy transfer and exciton confinement, whereas they differ in the highest occupied molecular orbital (HOMO) alignment, forming type I and type II host/guest heterostructures. While the type I structure shows negligible electric field induced quenching, a quenching up to 25% for the type II at a field of 2 MV/cm is reported. A similar quenching behaviour is also reported for thin films of the pure emitter, revealing an important luminescence loss mechanism for aggregated emitter molecules. These results are interpreted by considering Coulomb stabilized excitons in the type II heterostructure and in the pure emitter, that become very sensitive to dissociation upon application of the field. These results clarify the role of external electric field quenching on the phosphorescence of triplet emitters and provide useful insights for the design of deep‐blue electrophosphorescent devices with a reduced efficiency roll‐off.     

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.     

Optimization of Orange‐Emitting Electrophosphorescent Copolymers for Organic Light‐Emitting Diodes

Orange‐emitting phosphorescent copolymers containing iridium complexes and bis(carbazolyl)fluorene groups in their side chains are employed as the emissive layer in multilayer organic light‐emitting diodes (OLEDs). The efficiency of the OLED devices is optimized by varying characteristics of the copolymers: the molecular weight, the iridium loading level, and the nature and length of the linker between the side chains and the polymer backbone. A maximum efficiency of 4.9 ± 0.4%, 8.8 ± 0.7 cd A⁻¹ at 100 cd m⁻² is achieved with an optimized copolymer.     

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

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

Highly Efficient Solid‐State Near‐Infrared Emitting Material Based on Triphenylamine and Diphenylfumaronitrile with an EQE of 2.58% in Nondoped Organic Light‐Emitting Diode

The development of efficient near‐infrared (NIR) emitting material is of current focus. Donor–acceptor (D–A) architecture has been proved to be an effective strategy to obtain narrow energy gap. Herein, a D–A‐type NIR fluorescent compound 2,3‐bis(4′‐(diphenylamino)‐[1,1′‐biphenyl]‐4‐yl)fumaronitrile (TPATCN) is synthesized and fully characterized. As revealed by theoretical calculations and photophysical experiments, TPATCN exerts the advantages of the relatively large dipole moment of the charge transfer state and a certain degree of orbital overlap of the local excited state. A highly mixed or hybrid local and charge transfer excited state might occur to simultaneously achieve both a large fraction of singlet formation and a high quantum efficiency in D–A system. TPATCN exhibits strong NIR fluorescence with the corresponding thin film quantum efficiency of 33% and the crystal efficiency of 72%. Remarkably, the external quantum efficiency of nondoped NIR organic light‐emitting diode (OLED) reaches 2.58% and remains fairly constant over a range of 100–300 mA cm^?2, which is among the best results for NIR OLEDs reported so far.     

Multifunctional Triphenylamine/Oxadiazole Hybrid as Host and Exciton‐Blocking Material: High Efficiency Green Phosphorescent OLEDs Using Easily Available and Common Materials

A new triphenylamine/oxadiazole hybrid, namely m‐TPA‐o‐OXD, formed by connecting the meta‐position of a phenyl ring in triphenylamine with the ortho‐position of 2,5‐biphenyl‐1,3,4‐oxadiazole, is designed and synthesized. The new bipolar compound is applicable in the phosphorescent organic light‐emitting diodes (PHOLEDs) as both host and exciton‐blocking material. By using the new material and the optimization of the device structures, very high efficiency green and yellow electrophosphorescence are achieved. For example, by introducing 1,3,5‐tris(N‐phenylbenzimidazol‐2‐yl)benzene (TPBI) to replace 2, 9‐dimethyl‐4,7‐diphenyl‐1, 10‐phenanthroline (BCP)/tris(8‐hydroxyquinoline)aluminium (Alq₃) as hole blocking/electron transporting layer, followed by tuning the thicknesses of hole‐transport 1, 4‐bis[(1‐naphthylphenyl)amino]biphenyl (NPB) layer to manipulate the charge balance, a maximum external quantum efficiency (η_EQE,max) of 23.0% and a maximum power efficiency (η_p,max) of 94.3 lm W⁻¹ are attained for (ppy)₂Ir(acac) based green electrophosphorescence. Subsequently, by inserting a thin layer of m‐TPA‐o‐OXD as self triplet exciton block layer between hole‐transport and emissive layer to confine triplet excitons, a η_EQE,max of 23.7% and η_p,max of 105 lm W⁻¹ are achieved. This is the highest efficiency ever reported for (ppy)₂Ir(acac) based green PHOLEDs. Furthermore, the new host m‐TPA‐o‐OXD is also applicable for other phosphorescent emitters, such as green‐emissive Ir(ppy)₃ and yellow‐emissive (fbi)₂Ir(acac). A yellow electrophosphorescent device with η_EQE,max of 20.6%, η_c,max of 62.1 cd A⁻¹, and η_p,max of 61.7 lm W⁻¹, is fabricated. To the author’s knowledge, this is also the highest efficiency ever reported for yellow PHOLEDs.     

A Hole‐Transporting Material with Controllable Morphology Containing Binaphthyl and Triphenylamine Chromophores

An organic compound with two triphenylamine moieties linked with binaphthyl at the 3,3′‐positions (2,2′‐dimethoxyl‐3,3′‐ di(phenyl‐4‐yl‐diphenyl‐amine)‐[1,1′]‐binaphthyl, TPA–BN–TPA) can be synthesized by Suzuki coupling. Amorphous and homogeneous films are obtained by either vacuum deposition or spin‐coating from solution in good solvents, while single crystals are grown in an appropriate polar solvent. X‐ray crystallography showed that a TPA–BN–TPA crystal is a multichannel structure containing solvent molecules in the channels. The intramolecular charge‐transfer state resulting from amino conjugation effects is observed by solvatochromic experiments. The high glass‐transition temperature (130 °C) and decomposition temperature (439 °C) of this material, in combination with its reversible oxidation property, make it a promising candidate as a hole‐transport material for light‐emitting diodes. With TPA–BN–TPA as the hole‐transporting layer in an indium tin oxide/TPA–BN–TPA/aluminum tris(8‐hydroxyquinoline)/Mg:Ag device, a brightness of about 10 100 cd m^–2 at 15.6 V with a maximum efficiency of 3.85 cd A^–1 is achieved, which is superior to a device with N,N′‐di(1‐naphthyl)‐N,N′‐diphenyl‐[1,1′‐biphenyl]‐4,4′‐diamine as the hole‐transporting layer under the same conditions. Other devices with TPA–BN–TPA as the blue‐light‐emitting layer or host for a blue dye emitter are also studied.     

Highly Efficient,Solution‐Processed,Single‐Layer,Electrophosphorescent Diodes and the Effect of Molecular Dipole Moment

A new family of highly soluble electrophosphorescent dopants based on a series of tris‐cyclometalated iridium(III) complexes (1–4) of 2‐(carbazol‐3‐yl)‐4/5‐R‐pyridine ligands with varying molecular dipole strengths have been synthesized. Highly efficient, solution‐processed, single‐layer, electrophosphorescent diodes utilizing these complexes have been prepared and characterized. The high triplet energy poly(9‐vinylcarbazole) PVK is used as a host polymer doped with 2‐(4‐biphenylyl)‐5‐(4‐tert‐butyl‐phenyl)‐1,3,4‐oxadiazole (PBD) for electron transport. Devices with a current efficiency of 40 cd A^?1 corresponding to an EQE of 12% can thus be achieved. The effect of the type and position of the substituent (electron‐withdrawing group (CF₃) and electron‐donating group (OMe)) on the molecular dipole moment of the complexes has been investigated. A correlation between the absorption strength of the singlet metal‐to‐ligand charge‐transfer (¹MLCT) transition and the luminance spectral red shift as a function of solvent polarity is observed. The strength of the transition dipole moments for complexes 1–4 has also been obtained from TD‐DFT computations, and is found to be consistent with the observed molecular dipole moments of these complexes. The relatively long lifetime of the excitons of the phosphorescence (microseconds) compared to the charge‐carrier scattering time (less than nanoseconds), allows the transition dipole moment to be considered as a “quasi permanent dipole”. Therefore, the carrier mobility is sufficiently affected by the long‐lived transition dipole moments of the phosphorescent molecules, which are randomly oriented in the medium. The dopant dipoles cause positional and energetic disorder because of the locally modified polarization energy. Furthermore, the electron‐withdrawing group CF₃ induces strong carrier dispersion that enhances the electron mobility. Therefore, the strong transition dipole moment in complexes 3 and 4 perturbs both electron and hole mobilities, yielding a reduction in exciton formation and an increase in the device dark current, thereby decreasing the device efficiency.     

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.     

DPVBi高效、高亮度非掺杂蓝色有机电致发光器件

以典型蓝色发光材料—联苯乙烯衍生物(4,4′-bis(2,2′-diphenylvinyl)-1,1′-biphenyl,DPVBi)为发光层,采用MoO3为阳极缓冲层制备了结构简单的非掺杂型蓝色有机电致发光器件,得到了低压启动,效率、亮度和色度俱佳的蓝色发光器件。器件启亮电压为3.4V,最高外量子效率为3.2%,最高亮度达到15 840cd/m2,器件色坐标为(0.15,0.15)。高性能器件的获得归因于MoO3缓冲层的插入在阳极/有机层间形成了良好的欧姆接触。     

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

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

Dopant‐Free Spiro‐Triphenylamine/Fluorene as Hole‐Transporting Material for Perovskite Solar Cells with Enhanced Efficiency and Stability

Chemical doping is often used to enhance electric conductivity of the conjugated molecule as hole‐transporting material (HTM) for the application in optoelectronics. However, chemical dopants can promote ion migration at the electrical field, which deteriorates the device efficiency as well as increases the fabrication cost. Here, two star HTMs, namely 2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenyl‐amine) 9,9′‐spirobifluorene (Spiro‐OMeTAD) and poly(triarylamine) are subjeted to chemical combination to yield dopant‐free N2,N2,N2′,N2′,N7,N7,N7′,N7′‐octakis(4‐methoxyphenyl)‐10‐phenyl‐10H‐spiro[acridine‐9,9′‐fluorene]‐2,2′,7,7′‐tetraamine (SAF‐OMe). The power conversion efficiencies (PCEs) of 12.39% achieved by solar cells based on pristine, dopant‐free SAF‐OMe are among the highest reported for perovskite solar cells and are even comparable to devices based on chemically doped Spiro‐OMeTAD (14.84%). Moreover, using a HTM comprised of SAF‐OMe with an additional dopant results in a record PCE of 16.73%. Compared to Spiro‐OMeTAD‐based devices, SAF‐OMe significantly improves stability.     

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.     

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

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

A Versatile Fluoro‐Containing Low‐Bandgap Polymer for Efficient Semitransparent and Tandem Polymer Solar Cells

The versatility of a fluoro‐containing low band‐gap polymer, poly[2,6‐(4,4‐bis(2‐ethylhexyl)‐4H‐cyclopenta[2,1‐b;3,4‐b’]dithiophene)‐alt‐4,7‐(5‐fluoro‐2,1,3‐benzothia‐diazole)] (PCPDTFBT) in organic photovoltaics (OPVs) applications is demonstrated. High boiling point 1,3,5‐trichlorobenzene (TCB) is used as a solvent to manipulate PCPDTFBT:[6,6]‐phenyl‐C₇₁‐butyric acid methyl ester (PC₇₁BM) active layer morphology to obtain high‐performance single‐junction devices. It promotes the crystallization of PCPDTFBT polymer, thus improving the charge‐transport properties of the active layer. By combining the morphological manipulation with interfacial optimization and device engineering, the single‐junction device exhibits both good air stability and high power‐conversion efficiency (PCE, of 6.6%). This represents one of the highest PCE values for cyclopenta[2,1‐b;3,4‐b’]dithiophene (CPDT)‐based OPVs. This polymer is also utilized for constructing semitransparent solar cells and double‐junction tandem solar cells to demonstrate high PCEs of 5.0% and 8.2%, respectively.     

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.     

Highly Efficient Inverted Organic Solar Cells Through Material and Interfacial Engineering of Indacenodithieno[3,2‐b]thiophene‐Based Polymers and Devices

A synergistic approach combining new material design and interfacial engineering of devices is adopted to produce high efficiency inverted solar cells. Two new polymers, based on an indacenodithieno[3,2‐b]thiophene‐difluorobenzothiadiazole (PIDTT‐DFBT) donor–acceptor (D–A) polymer, are produced by incorporating either an alkyl thiophene (PIDTT‐DFBT‐T) or alkyl thieno[3,2‐b]thiophene (PIDTT‐DFBT‐TT) π‐bridge as spacer. Although the PIDTT‐DFBT‐TT polymer exhibits decreased absorption at longer wavelengths and increased absorption at higher energy wavelengths, it shows higher power conversion efficiencies in devices. In contrast, the thiophene bridged PIDTT‐DFBT‐T shows a similar change in its absorption spectrum, but its low molecular weight leads to reduced hole mobilities and performance in photovoltaic cells. Inverted solar cells based on PIDTT‐DFBT‐TT are explored by modifying the electron‐transporting ZnO layer with a fullerene self‐assembled monolayer and the MoO₃ hole‐transporting layer with graphene oxide. This leads to power conversion efficiencies as high as 7.3% in inverted cells. PIDTT‐DFBT‐TT's characteristic strong short wavelength absorption and high efficiency suggests it is a good candidate as a wide band gap material for tandem solar cells.