Nonfullerene Polymer Solar Cells based on a Perylene Monoimide Acceptor with a High Open‐Circuit Voltage of 1.3 V

Nonfullerene polymer solar cells (PSCs) are fabricated with a perylene monoimide‐based n‐type wide‐bandgap organic semiconductor PMI‐F‐PMI as an acceptor and a bithienyl‐benzodithiophene‐based wide‐bandgap copolymer PTZ1 as a donor. The PSCs based on PTZ1:PMI‐F‐PMI (2:1, w/w) with the treatment of a mixed solvent additive of 0.5% N ‐methyl pyrrolidone and 0.5% diphenyl ether demonstrate a very high open‐circuit voltage (V _oc) of 1.3 V with a higher power conversion efficiency (PCE) of 6%. The high V _oc of the PSCs is a result of the high‐lying lowest unoccupied molecular orbital (LUMO) of ?3.42 eV of the PMI‐F‐PMI acceptor and the low‐lying highest occupied molecular orbital (HOMO) of ?5.31 eV of the polymer donor. Very interestingly, the exciton dissociation efficiency in the active layer is quite high, even though the LUMO and HOMO energy differences between the donor and acceptor materials are as small as ≈0.08 and 0.19 eV, respectively. The PCE of 6% is the highest for the PSCs with a V _oc as high as 1.3 V. The results indicate that the active layer based on PTZ1/PMI‐F‐PMI can be used as the front layer in tandem PSCs for achieving high V _oc over 2 V.     

Extremely Low Operating Voltage Green Phosphorescent Organic Light‐Emitting Devices

Organic light‐emitting devices (OLEDs) are expected to be adopted as the next generation of general lighting because they are more efficient than fluorescent tubes and are mercury‐free. The theoretical limit of operating voltage is generally believed to be equal to the energy gap, which corresponds to the energy difference between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) for the emitter molecule divided by the electron charge (e). Here, green OLEDs operating below a theoretical limit of the energy gap (E_g) voltage with high external quantum efficiency over 20% are demonstrated using fac‐tris(2‐phenylpyridine)iridium(III) with a peak emission wavelength of 523 nm, which is equivalent to a photon energy of 2.38 eV. An optimized OLED operates clearly below the theoretical limit of the E_g voltage at 2.38 V showing 100 cd m^?2 at 2.25 V and 5000 cd m^?2 at 2.95 V without any light outcoupling enhancement techniques.     

Structural Origins for Tunable Open‐Circuit Voltage in Ternary‐Blend Organic Solar Cells

Ternary‐blend bulk‐heterojunction solar cells have provided a unique opportunity for tuning the open‐circuit voltage (V_oc) as the “effective” highest occupied molecular orbital (HOMO) or lowest unoccupied molecular orbital (LUMO) energy levels shift with active‐layer composition. Grazing‐incidence X‐ray diffraction (GIXD) measurements performed on such ternary‐blend thin films reveal evidence that the two polymer donors interact intimately; their ionization potentials are thus reflections of the blend compositions. In ternary‐blend thin films in which the two polymer donors do not interact physically, the polymer donors each retain their molecular electronic character; solar cells constructed with these ternary blends thus exhibit V_ocs that are pinned to the energy level difference between the highest of the two lying HOMO and the LUMO of the electron acceptor. These observations are consistent with the organic alloy model proposed earlier. Quantification of the square of the square‐root differences of the surface energies of the components provides a proxy for the Flory–Huggins interaction parameter for polymer donor pairs in these ternary‐blend systems. Of the three ternary‐blend systems examined herein, this quantity has to be below 0.094 in order for ternary‐blend solar cells to exhibit tunable V_oc.     

Highly Sensitive Non‐Classical Strain Gauge Using Organic Heptazole Thin‐Film Transistor Circuit on a Flexible Substrate

A non‐classical organic strain gauge as a voltage signal sensor is reported, using an inverter‐type thin‐film transistor (TFT) circuit, which is able to sensitively measure a large quantity of elastic strain (up to ≈2.48%), which approaches an almost folding state. Novel heptazole‐based organic TFTs are chosen to be incorporated in this gauge circuit; organic solid heptazole has small domain size in general. While large crystal domain‐pentacene TFTs seldom show sufficient current variation upon mechanical bending for tensile strain, these heptazole TFTs demonstrate a significant variation for the same strain condition as applied to pentacene devices. In addition, the pentacene channel does not recover to its original electric state after bending but heptazole channels are very elastic and reversible, even after going through serious bending. More interesting is that the heptazole TFTs show only a little variation of signal current under horizontal direction strain, while they make a significant amount of current decrease under vertical direction strain. Utilizing the anisotropic response to the tensile bending strain, an ultrasensitive voltage output strain gauge composed of a horizontally and vertically oriented TFT couple is demonstrated.     

Small π-conjugated organic molecules based transistor and inverter with Cu electrodes

In absence of metallurgical Ohmic contacts in organic semiconductors, the relative position of metal work function with respect to highest occupied molecular orbital (HOMO) or lowest unoccupied molecular orbital (LUMO) decides whether a metal electrode is Ohmic or non-Ohmic. Here we report that Cu whose work function is close to HOMO of the small π-conjugated organic molecules: pentacene and copper phthalocyanine (CuPc), can be used to achieve high performance of transistors and inverters. Fermi level is pinned at metal/copper hexadecafluoro phthalocyanine (F₁₆CuPc) interface resulting the barrier for carrier injection from metal to F₁₆CuPc independent of metal work functions. We have fabricated organic field effect transistors and inverters based on pentacene, CuPc and F₁₆CuPc with Cu and Au electrodes and observed that the performance of the devices with Cu electrodes are comparable to the devices with Au electrodes.     

1‐Methyl‐2‐(anthryl)‐imidazo[4,5‐f][1,10]‐phenanthroline: A Highly Efficient Electron‐Transport Compound and a Bright Blue‐Light Emitter for Electroluminescent Devices

A new organic blue‐light emitter 1‐methyl‐2‐(anthryl)‐imidazo[4,5‐f][1,10]‐phenanthroline ( 1 ) has been synthesized and fully characterized. The utility of compound 1 as a blue‐light emitter in electroluminescent (EL) devices has been evaluated by fabricating a series of EL devices A where compound 1 functions as an emitter. The EL spectrum of device series A has the emission maximum at 481 nm with the CIE (Commission Internationale de l'Eclairage) color coordinates 0.198 and 0.284. The maximum luminance of devices in series A is 4000 cd m^–2 and the best external quantum efficiency of device series A is 1.82 %. The utility of compound 1 as an electron injection–electron transport material has been evaluated by constructing a set of EL devices B where 1 is used as either the electron‐injection layer or the electron injection–electron transport layer. The performance of device series B is compared to the standard device in which Alq₃ (tris(8‐hydroxyquinoline) aluminum) is used as the electron injection–electron transport layer. The experimental results show that the performance of 1 as an electron injection–electron transport material is considerably better than Alq₃. The stability of device series B is comparable to that of the standard Alq₃ device. The excellent performance of 1 as an electron injection/transport material may be attributed to the strong intermolecular interactions of 1 in the solid state as revealed by single‐crystal X‐ray diffraction analysis. In addition, compound 1 is a colorless material with a much larger highest occupied molecular orbital–lowest unoccupied molecular (HOMO–LUMO) gap than Alq₃, which renders it potentially useful for a wide range of applications in EL devices.     

Dithienocarbazole‐Based Ladder‐Type Heptacyclic Arenes with Silicon,Carbon, and Nitrogen Bridges: Synthesis,Molecular Properties,Field‐Effect Transistors,and Photovoltaic Applications

A new class of ladder‐type dithienosilolo‐carbazole ( DTSC ), dithienopyrrolo‐carbazole ( DTPC ), and dithienocyclopenta‐carbazole ( DTCC ) units is developed in which two outer thiophene subunits are covalently fastened to the central 2,7‐carbazole cores by silicon, nitrogen, and carbon bridges, respectively. The heptacyclic multifused monomers are polymerized with the benzothiadiazole ( BT ) acceptor by palladium‐catalyzed cross‐coupling to afford three alternating donor‐acceptor copolymers poly(dithienosilolo‐carbazole‐alt‐benzothiadiazole) ( PDTSCBT) , poly(dithienocyclopenta‐carbazole‐alt‐benzothiadiazole) ( PDTCCBT), and poly(dithienopyrrolo‐carbazole‐alt‐benzothiadiazole) ( PDTPCBT) . The silole units in DTSC possess electron‐accepting ability that lowers the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energy levels of PDTSCBT , whereas stronger electron‐donating ability of the pyrrole moiety in DTPC increases the HOMO and LUMO energy levels of PDTPCBT . The optical bandgaps (E_g^opt) deduced from the absorption edges of thin film spectra are in the following order: PDTSCBT (1.83 eV) > PDTCCBT (1.64 eV) > PDTPCBT (1.50 eV). This result indicated that the donor strength of the heptacyclic arenes is in the order: DTPC > DTCC > DTSC . The devices based on PDTSCBT and PDTCCBT exhibited high hole mobilities of 0.073 and 0.110 cm² V^?1 s^?1, respectively, which are among the highest performance from the OFET devices based on the amorphous donor‐acceptor copolymers. The bulk heterojunction photovoltaic device using PDTSCBT as the p‐type material delivered a promising efficiency of 5.2% with an enhanced open circuit voltage, V_oc, of 0.82 V.     

Single‐Electron Tunneling through Molecular Quantum Dots in a Metal‐Insulator‐Semiconductor Structure

A sigle‐electron tunneling (SET) in a metal‐insulator‐semiconductor (MIS) structure is demonstrated, in which C₆₀ and copper phthalocyanine (CuPc) molecules are embedded as quantum dots in the insulator layer. The SET is found to originate from resonant tunneling via the energy levels of the embedded molecules, (e.g., the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO)). These findings show that the threshold voltages for SET are tunable according to the energy levels of the molecules. Furthermore, SET is observable even near room temperature. The results suggest, together with the fact that these properties are demonstrated in a practical device configuration, that the integration of molecular dots into the Si‐MIS structure has considerable potential for achieving novel SET devices. Moreover, the attempt allows large‐scale integration of individual molecular functionalities.     

Singlet–Triplet Splitting Energy Management via Acceptor Substitution: Complanation Molecular Design for Deep‐Blue Thermally Activated Delayed Fluorescence Emitters and Organic Light‐Emitting Diodes Application

A barely reached balance between weak intramolecular‐charge‐transfer (ICT) and small singlet–triplet splitting energy (ΔE_ST) for reverse intersystem crossing from non‐emissive triplet state to radiative singlet state impedes the realization of deep‐blue thermally activated delayed fluorescence (TADF) materials. By discarding the twisted‐ICT framework for a flattened molecular backbone and introducing a strong acceptor possessing n–π* transition character, hypsochromic color, a large radiative rate (k_F), and small ΔE_ST are achieved simultaneously. Six molecules with a 9,9‐dimethyl‐10‐phenyl‐9,10‐dihydroacridine (i‐DMAc) donor are synthesized and investigated. Coinciding with time‐dependent density functional theory, the reduced dihedral angles between donor (D) and acceptor (A) weaken ICT from dispersed charge density and enable a large k_F from increased frontier molecular orbitals overlap. Despite the separated highest occupied (HOMO) and lowest unoccupied molecular orbital (LUMO) population, the intercalation of phenyl bridges between D–A increases k_F but significantly lowers the local triplet excited state, indicating small HOMO and LUMO overlap is not a sufficient, but necessary condition for reduced ΔE_ST. Integrating short conjugation length and carbonyl or triazine acceptors into the complanation molecules, deep‐blue TADF organic light‐emitting diodes demonstrate maximum external quantum efficiencies of 11.5% and 10.9% with Commission Internationale de l'Eclairage coordinates of (0.16, 0.09) and (0.15, 0.11), respectively, which is quite close to the stringent National Television System Committee blue standard.     

Synergistic Use of Pyridine and Selenophene in a Diketopyrrolopyrrole‐Based Conjugated Polymer Enhances the Electron Mobility in Organic Transistors

To achieve semiconducting materials with high electron mobility in organic field‐effect transistors (OFETs), low‐lying energy levels (the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO)) and favorable molecular packing and ordering are two crucial factors. Here, it is reported that the incorporation of pyridine and selenophene into the backbone of a diketopyrrolopyrrole (DPP)‐based copolymer produces a high‐electron‐mobility semiconductor, PDPPy‐Se. Compared with analogous polymers based on other DPP derivatives and selenophene, PDPPy‐Se features a lower LUMO that can decrease the electron transfer barrier for more effective electron injection, and simultaneously a lower HOMO that, however, can increase the hole transfer barrier to suppress the hole injection. Combined with thermal annealing at 240 °C for thin film morphology optimization to achieve large‐scale crystallite domains with tight molecular packing for effective charge transport along the conducting channel, OFET devices fabricated with PDPPy‐Se exhibit an n‐type‐dominant performance with an electron mobility (μ_e) as high as 2.22 cm² V^?1 s^?1 and a hole/electron mobility ratio (μ_h/μ_e) of 0.26. Overall, this study demonstrates a simple yet effective approach to boost the electron mobility in organic transistors by synergistic use of pyridine and selenophene in the backbone of a DPP‐based copolymer.     

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.     

High‐Mobility Air‐Stable Solution‐Shear‐Processed n‐Channel Organic Transistors Based on Core‐Chlorinated Naphthalene Diimides

High charge carrier mobility solution‐processed n‐channel organic thin‐film transistors (OTFTs) based on core‐chlorinated naphthalene tetracarboxylic diimides (NDIs) with fluoroalkyl chains are demonstrated. These OTFTs were prepared through a solution shearing method. Core‐chlorination of NDIs not only increases the electron mobilities of OTFTs, but also enhances their air stability, since the chlorination in the NDI core lowers the lowest unoccupied molecular orbital (LUMO) levels. The air‐stability of dichlorinated NDI was better than that of the tetrachlorinated NDIs, presumably due to the fact that dichlorinated NDIs have a denser packing of the fluoroalkyl chains and less grain boundaries on the surface, reducing the invasion pathway of ambient oxygen and moisture. The devices of dichlorinated NDIs exhibit good OTFT performance, even after storage in air for one and a half months. Charge transport anisotropy is observed from the dichlorinated NDI. A dichlorinated NDI with ?CH₂C₃F₇ side chains reveals high mobilities of up to 0.22 and 0.57 cm² V^?1 s^?1 in parallel and perpendicular direction, respectively, with regard to the shearing direction. This mobility anisotropy is related to the grain morphology. In addition, we find that the solution‐shearing deposition affects the molecular orientation in the crystalline thin films and lowers the d(001)‐spacing (the out‐of‐plane interlayer spacing), compared to the vapor‐deposited thin films. Core‐chlorinated NDI derivatives are found to be highly suitable for n‐channel active materials in low‐cost solution‐processed organic electronics.     

Crosslinkable TAPC‐Based Hole‐Transport Materials for Solution‐Processed Organic Light‐Emitting Diodes with Reduced Efficiency Roll‐Off

1‐Bis[4‐[N,N‐di(4‐tolyl)amino]phenyl]‐cyclohexane (TAPC) has been widely used in xerography and organic light‐emitting diodes (OLEDs), but derivatives are little known. Here, a new series of solution‐processable, crosslinkable hole conductors based on TAPC with varying highest occupied molecular orbital (HOMO) energies from ?5.23 eV to ?5.69 eV is implemented in blue phosphorescent OLEDs. Their superior perfomance compared with the well‐known N4,N4,N4′,N4′‐tetraphenylbiphenyl‐4,4′‐diamine (TPDs) analogues regarding hole‐injection and mobility, electron and exciton blocking capabilities, efficiency, and efficiency roll‐off is demonstrated. Overall, the TAPC‐based devices feature higher luminous and power efficiency over a broader range of brightness levels and reduced efficiency roll off. A systematic broadening of the emission zone is observed as the hole‐injection barrier between the anode and the hole‐transporting layer increased.     

Alternating Copolymers of Cyclopenta[2,1‐b;3,4‐b′]dithiophene and Thieno[3,4‐c]pyrrole‐4,6‐dione for High‐Performance Polymer Solar Cells

A series of alternating copolymers of cyclopenta[2,1‐b;3,4‐b′]dithiophene (CPDT) and thieno[3,4‐c]pyrrole‐4,6‐dione (TPD) have been prepared and characterized for polymer solar cell (PSC) applications. Different alkyl side chains, including butyl (Bu), hexyl (He), octyl (Oc), and 2‐ethylhexyl (EH), are introduced to the TPD unit in order to adjust the packing of the polymer chain in the solid state, while the hexyl side chain on the CPDT unit remains unchanged to simplify discussion. The polymers in this series have a simple main chain structure and can be synthesized easily, have a narrow band gap and a broad light absorption. The different alkyl chains on the TPD unit not only significantly influence the solubility and chain packing, but also fine tune the energy levels of the polymers. The polymers with Oc or EH group have lower HOMO (highest occupied molecular orbital) and LUMO (lowest unoccupied molecular orbital) energy levels, resulting higher open circuit voltages (V_oc) of the PSC devices. Power conversion efficiencies (PCEs) up to 5.5% and 6.4% are obtained from the devices of the Oc substituted polymer (PCPDTTPD‐Oc) with PC₆₁BM and PC₇₁BM, respectively. This side chain effect on the PSC performance is related to the formation of a fine bulk heterojunction structure of polymer and PCBM domains, as observed with atomic force microscopy.     

Thioethyl‐Porphyrazine/Nanocarbon Hybrids for Photoinduced Electron Transfer

A novel pyrene‐substituted thioethyl‐porphyrazine ( PzPy ) and the formation of supramolecular assembly with nanocarbons demonstrating photoinduced electron transfer ability are designed. As revealed by spectroscopic and electrochemical studies, PzPy displays wide spectral absorption in the visible range, charge separation upon photoexcitation, as well as bandgap and highest occupied/lowest unoccupied molecular orbital (HOMO/LUMO) energy values, matching the key requirements of organic optoelectronic. Moreover, the presence of a pyrene moiety promotes attractive interactions with π‐conjugated systems. In particular, theoretical calculations show that in the PzPy the HOMO and LUMO are localized on different positions of the molecule, i.e., the HOMO on the pyrene moiety and the LUMO on the macrocycle. Therefore, HOMO–LUMO excitation gives rise to a charge separation, preventing excitons recombination. Two kinds of noncovalent hybrid composites are prepared by mixing the PzPy with single‐wall carbon nanotubes (SWNTs) and graphene nanoflakes (GNFs), respectively, and used for photocurrent generation through charge transfer processes between PzPy and nanocarbons. Photoconduction experiments show photocurrent generation upon visible light irradiation of both PzPy /SWNT and PzPy /GNF composites (0.78 and 0.71 mA W^?1 at 500 nm, respectively), demonstrating their suitability for optoelectronic applications and light harvesting systems.     

High Solid‐State Near Infrared Emissive Organic Fluorophores from Thiadiazole[3,4‐c]Pyridine Derivatives for Efficient Simple Solution‐Processed Nondoped Near Infrared OLEDs

Many efforts have been dedicated to developing near infrared (NIR) fluorescent emitters with strong emission especially in the range of 700–1000 nm due to their potential applications in biomedical and optoelectronic fields. However, high solid state NIR emission fluorophores are still rare for applications. Herein, two efficient donor‐π‐acceptor type NIR emitters, C3HTP and C4HTP , are designed and synthesized by end‐capping two isomeric bis(n‐hexylthienyl)thiadiazole[3,4‐c]pyridines as π‐acceptor with structural bulky, electron rich tercarbazole moiety. They exhibit excellent solid state NIR emission with an emission peak at 725 nm, especially C3HTP , reaching a record high photoluminescence quantum yield (Φ_PL) of 34% for NIR organic fluorescent materials. By taking advantage of their Φ_PL values in the film state (Φ_PL = 10–34%), suitable energy levels (highest occupied molecular orbital (HOMO) level ≈ ?5.3 eV), high hole mobility (5.49 × 10^?8 cm² V^?1 s^?1) as well as good amorphous film forming ability by solution casting, they are used to fabricate a nondoped emissive layer (EML) in simple double‐layer solution processed NIR electroluminescent (EL) devices. The device containing C3HTP as the EML shows a NIR emission peaking at 726 nm and excellent EL performance with a high external quantum efficiency of 1.51%, which is the best solution processed nondoped NIR organic light‐emitting diodes reported to date. Importantly, this represents an advance in near infrared organic fluorescent materials and EL devices that meet the requirements of many applications.     

Enhanced Performance Consistency in Nanoparticle/TIPS Pentacene‐Based Organic Thin Film Transistors

In this study, inorganic silica nanoparticles are used to manipulate the morphology of 6,13‐bis(triisopropylsilylethynyl)‐pentacene (TIPS pentacene) thin films and the performance of solution‐processed organic thin‐film transistors (OTFTs). This approach is taken to control crystal anisotropy, which is the origin of poor consistency in TIPS pentacene based OTFT devices. Thin film active layers are produced by drop‐casting mixtures of SiO₂ nanoparticles and TIPS pentacene. The resultant drop‐cast films yield improved morphological uniformity at ～10% SiO₂ loading, which also leads to a 3‐fold increase in average mobility and nearly 4 times reduction in the ratio of measured mobility standard deviation (μ_Stdev) to average mobility (μ_Avg). Grazing‐incidence X‐ray diffraction, scanning and transmission electron microscopy as well as polarized optical microscopy are used to investigate the nanoparticle‐mediated TIPS pentacene crystallization. The experimental results suggest that the SiO₂ nanoparticles mostly aggregate at TIPS pentacene grain boundaries, and 10% nanoparticle concentration effectively reduces the undesirable crystal misorientation without considerably compromising TIPS pentacene crystallinity.     

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 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.     

Direct Threat of a UV‐Ozone Treated Indium‐Tin‐Oxide Substrate to the Stabilities of Common Organic Semiconductors

Ultraviolet‐ozone treated indium‐tin‐oxide (UV‐ITO) glass substrates have been widely and unquestioningly used in the field of organic electronics to improve both device performance and stability. Evidence is presented here for rapid decay of common organic films such as N,N′‐bis(naphthalen‐1‐ yl)‐N,N′‐bis(phenyl)‐benzidine (NPB), tris(8‐hydroxy‐quinolinato)aluminum (Alq₃), and rubrene when they are in contact with an UV‐ITO substrate. While the photoluminescence (PL) of these organic films deposited on an UV‐ITO substrate decay rapidly under illumination; those on quartz substrates are comparatively much more stable. Results from X‐ray and UV photoemission spectroscopies (XPS and UPS) further suggest that degradations of the rubrene films on UV‐ITO substrate are mainly attributed to active oxygen species generated upon UV‐ozone treatment. These reactive oxygen species on the UV‐ITO surface behave as a reservoir of oxygen that interacts with rubrene and shifts its highest occupied molecular orbital (HOMO) level away from the Fermi level. This interaction induces a gap‐state in the energy gap of rubrene, which acts as a charge recombination center. More importantly, enhanced stabilities of rubrene‐based organic photovoltaic (OPV) devices are demonstrated when they are fabricated on gold‐coated or trifluoromethane (CHF₃) plasma‐treated ITO. The presented works shows that the commonly used UV‐ITO substrate is a threat to the stability of addlayer organic semiconducting films.