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1.
Polyfluorene (PF)‐based light‐emitting diodes (LEDs) typically exhibit device degradation under operation with the emergence of a strong low‐energy emission band (at ~ 2.2–2.4 eV). This longer wavelength band converts the desired blue emission to blue–green or even yellow. We have studied both the photoluminescence (PL) and electroluminescence (EL) of PFs with different molecular structures and found that the low‐energy emission band originates from fluorenone defects which are introduced by photo‐oxidization, thermal oxidation, or during device fabrication. X‐ray photo‐emission spectroscopy (XPS) results show that the oxidation of PF is strongly catalyzed by the presence of calcium. The fluorenone defects generate a stronger contribution to the EL than to the PL. By utilization of a novel electron‐transporting material as a buffer layer between the emissive PF and the Ca/Ag (Ba/Ag) cathode, the blue EL emission from the PF was stabilized.  相似文献   

2.
A blend of two hole‐dominant polymers is created and used as the light emissive layer in light‐emitting diodes to achieve high luminous efficiency up to 22 cd A?1. The polymer blend F81?xSYx is based on poly(9,9‐dioctylfluorene) (F8) and poly(para‐phenylene vinylene) derivative superyellow (SY). The blend system exhibits a preferential vertical concentration distribution. The resulting energy landscape modifies the overall charge transport behavior of the blend emissive layer. The large difference between the highest unoccupied molecular orbital levels of F8 (5.8 eV) and SY (5.3 eV) introduces hole traps at SY sites within the F8 polymer matrix. This slows down the hole mobility and facilitates a balance between the transport behavior of both the charge carriers. The balance due to such energy landscape facilitates efficient formation of excitons within the emission zone well away from the cathode and minimizes the surface quenching effects. By bringing the light‐emission zone in the middle of the F81?xSYx film, the bulk of the film is exploited for the light emission. Due to the charge trapping nature of SY molecules in F8 matrix and pushing the emission zone in the center, the radiative recombination rate also increases, resulting in excellent device performance.  相似文献   

3.
Electron injection from the source–drain electrodes limits the performance of many n‐type organic field‐effect transistors (OFETs), particularly those based on organic semiconductors with electron affinities less than 3.5 eV. Here, it is shown that modification of gold source–drain electrodes with an overlying solution‐deposited, patterned layer of an n‐type metal oxide such as zinc oxide (ZnO) provides an efficient electron‐injecting contact, which avoids the use of unstable low‐work‐function metals and is compatible with high‐resolution patterning techniques such as photolithography. Ambipolar light‐emitting field‐effect transistors (LEFETs) based on green‐light‐emitting poly(9,9‐dioctylfluorene‐alt‐benzothiadiazole) (F8BT) and blue‐light‐emitting poly(9,9‐dioctylfluorene) (F8) with electron‐injecting gold/ZnO and hole‐injecting gold electrodes show significantly lower electron threshold voltages and several orders of magnitude higher ambipolar currents, and hence light emission intensities, than devices with bare gold electrodes. Moreover, different solution‐deposited metal oxide injection layers are compared. By spin‐coating ZnO from a low‐temperature precursor, processing temperatures could be reduced to 150 °C. Ultraviolet photoemission spectroscopy (UPS) shows that the improvement in transistor performance is due to reduction of the electron injection barrier at the interface between the organic semiconductor and ZnO/Au compared to bare gold electrodes.  相似文献   

4.
This paper reports state‐of‐the‐art fluorene‐based yellow‐green conjugated polymer blend gain media using Förster resonant‐energy‐transfer from novel blue‐emitting hosts to yield low threshold (≤7 kW cm?2) lasers operating between 540 and 590 nm. For poly(9,9‐dioctylfluorene‐co‐benzothiadiazole) (F8BT) (15 wt%) blended with the newly synthesized 3,6‐bis(2,7‐di([1,1′‐biphenyl]‐4‐yl)‐9‐phenyl‐9H‐fluoren‐9‐yl)‐9‐octyl‐9H–carbazole (DBPhFCz) a highly desirable more than four times increase (relative to F8BT) in net optical gain to 90 cm?1 and 34 times reduction in amplified spontaneous emission threshold to 3 µJ cm?2 is achieved. Detailed transient absorption studies confirm effective exciton confinement with consequent diffusion‐limited polaron‐pair generation for DBPhFCz. This delays formation of host photoinduced absorption long enough to enable build‐up of the spectrally overlapped, guest optical gain, and resolves a longstanding issue for conjugated polymer photonics. The comprehensive study further establishes that limiting host conjugation length is a key factor therein, with 9,9‐dialkylfluorene trimers also suitable hosts for F8BT but not pentamers, heptamers, or polymers. It is additionally demonstrated that the host highest occupied and lowest unoccupied molecular orbitals can be tuned independently from the guest gain properties. This provides the tantalizing prospect of enhanced electron and hole injection and transport without endangering efficient optical gain; a scenario of great interest for electrically pumped amplifiers and lasers.  相似文献   

5.
n‐Doping electron‐transport layers (ETLs) increases their conductivity and improves electron injection into organic light‐emitting diodes (OLEDs). Because of the low electron affinity and large bandgaps of ETLs used in green and blue OLEDs, n‐doping has been notoriously more difficult for these materials. In this work, n‐doping of the polymer poly[(9,9‐dioctylfluorene‐2,7‐diyl)‐alt‐(benzo[2,1,3]thiadiazol‐4,7‐diyl)] (F8BT) is demonstrated via solution processing, using the air‐stable n‐dopant (pentamethylcyclopentadienyl)(1,3,5‐trimethylbenzene)ruthenium dimer [RuCp*Mes]2. Undoped and doped F8BT films are characterized using ultraviolet and inverse photoelectron spectroscopy. The ionization energy and electron affinity of the undoped F8BT are found to be 5.8 and 2.8 eV, respectively. Upon doping F8BT with [RuCp*Mes]2, the Fermi level shifts to within 0.25 eV of the F8BT lowest unoccupied molecular orbital, which is indicative of n‐doping. Conductivity measurements reveal a four orders of magnitude increase in the conductivity upon doping and irradiation with ultraviolet light. The [RuCp*Mes]2‐doped F8BT films are incorporated as an ETL into phosphorescent green OLEDs, and the luminance is improved by three orders of magnitude when compared to identical devices with an undoped F8BT ETL.  相似文献   

6.
A series of dicarbazolyl derivatives bridged by various aromatic spacers and decorated with peripheral diarylamines were synthesized using Ullmann and Pd‐catalyzed C–N coupling procedures. These derivatives emit blue light in solution. In general, they possess high glass‐transition temperatures (Tg > 125 °C) which vary with the bridging segment and methyl substitution on the peripheral amine. Double‐layer organic light‐emitting devices were successfully fabricated using these molecules as hole‐transporting and emitting materials. Devices of the configuration ITO/HTL/TPBI/Mg:Ag (ITO: indium tin oxide; HTL: hole‐transporting layer; TPBI: 1,3,5‐tris(N‐phenylbenzimidazol‐2‐yl)benzene) display blue emission from the HTL layer. The EL spectra of these devices appear slightly distorted due to the exciplex formation at the interfaces. However, for the devices of the configuration ITO/HTL/Alq3/Mg:Ag (Alq3 = tris(8‐hydroxyquinoline)aluminum) a bright green light from the Alq3 layer was observed. This clearly demonstrates the facile hole‐transporting property of the materials described here.  相似文献   

7.
Herein, we address the reduction in the external quantum efficiency (EQE) of solution‐processed organic photodetectors caused by the room temperature phase demixing of components in the composite material of the photoactive layer. The reduction takes place under ambient conditions and after the completion of device fabrication. As a model system, we study photoactive blend films that consist of the electron acceptor N,N’‐bis(alkyl)‐3,4,9,10‐perylene tetracarboxylic diimide) (PDI) and the electron donor polymer poly(9,9’‐dioctylfluorene‐co‐benzothiadiazole) (F8BT). The ambient ageing of these photo­active layers is a consequence of the PDI component segregation; however, the final PDI domain size remains smaller than the resolution limit of optical microscopy. We find that the photophysical properties of the aged F8BT:PDI layer and the EQE of the aged device are significantly altered. The fabrication of F8BT:PDI layers from solvents of increasing boiling point allows for the spectroscopic monitoring of the ageing‐induced phase segregation (a‐PSG) process. For each solvent used, the extent of a‐PSG is correlated with the PDI dispersion in the F8BT matrix as received immediately after layer deposition. The tendency for room temperature phase demixing becomes stronger as PDI is more finely dispersed in the freshly spun F8BT:PDI layer. The evolution of the room temperature phase segregation of PDI has a negative impact on the photophysical processes that are essential for charge photogeneration in the F8BT:PDI photoactive layer.  相似文献   

8.
Evidence for a correlation between the dynamics of emissive non‐geminate charge recombination within organic photovoltaic (OPV) blend films and the photocurrent generation efficiency of the corresponding blend‐based solar cells is presented. Two model OPV systems that consist of binary blends of electron acceptor N′‐bis(1‐ethylpropyl)‐3,4,9,10‐perylene tetracarboxy diimide (PDI) with either poly(9,9‐dioctylfluorene‐co‐benzothiadiazole) (F8BT) or poly(9,9‐dioctylindenofluorene‐co‐benzothiadiazole) (PIF8BT) as electron donor are studied. For the F8BT:PDI and PIF8BT:PDI devices photocurrent generation efficiency is shown to be related to the PDI crystallinity. In contrast to the F8BT:PDI system, thermal annealing of the PIF8BT:PDI layer at 90 °C has a positive impact on the photocurrent generation efficiency and yields a corresponding increase in PL quenching. The devices of both blends have a strongly reduced photocurrent on higher temperature annealing at 120 °C. Delayed luminescence spectroscopy suggests that the improved efficiency of photocurrent generation for the 90 °C annealed PIF8BT:PDI layer is a result of optimized transport of the photogenerated charge‐carriers as well as of enhanced PL quenching due to the maintenance of optimized polymer/PDI interfaces. The studies propose that charge transport in the blend films can be indirectly monitored from the recombination dynamics of free carriers that cause the delayed luminescence. For the F8BT:PDI and PIF8BT:PDI blend films these dynamics are best described by a power‐law decay function and are found to be temperature dependent.  相似文献   

9.
The electronic structure of the interfaces formed after deposition of MoO3 hole‐injection layers on top of a polymer light‐emitting material, poly(dioctylfluorene‐alt‐benzothiadiazole) (F8BT), is studied by ultraviolet photoelectron spectroscopy (UPS), X‐ray photoelectron spectroscopy and metastable atom electron spectroscopy. Significant band bending is induced in the F8BT film by MoO3 “acceptors” that spontaneously diffuse into the F8BT “host” probably driven by kinetic energy of the deposited hot MoO3. Further deposition leads to the saturation of the band bending accompanied by the formation of MoO3 overlayers. Simultaneously, a new electronic state in the vicinity of the Fermi level appears on the UPS spectra. Since this peak does not appear in the bulk MoO3 film, it can be assigned as an interface state between the MoO3 overlayer and underlying F8BT film. Both band bending and the interface state should result from charge transfer from F8BT to MoO3, and they appear to be the origin of the hole‐injection enhancement by the insertion of MoO3 layers between the F8BT light‐emitting diodes and top anodes.  相似文献   

10.
Strong intermolecular interactions usually result in decreases in solubility and fluorescence efficiency of organic molecules. Therefore, amorphous materials are highly pursued when designing solution‐processable, electroluminescent organic molecules. In this paper, a non‐planar binaphthyl moiety is presented as a way of reducing intermolecular interactions and four binaphthyl‐containing molecules ( BNCM s): green‐emitting BBB and TBT as well as red‐emitting BTBTB and TBBBT , are designed and synthesized. The photophysical and electrochemical properties of the molecules are systematically investigated and it is found that TBT , TBBBT , and BTBTB solutions show high photoluminescence (PL) quantum efficiencies of 0.41, 0.54, and 0.48, respectively. Based on the good solubility and amorphous film‐forming ability of the synthesized BNCM s, double‐layer structured organic light‐emitting diodes (OLEDs) with BNCM s as emitting layer and poly(N‐vinylcarbazole) (PVK) or a blend of poly[N,N′‐bis(4‐butylphenyl)‐N,N′‐bis(phenyl)benzidine] and PVK as hole‐transporting layer are fabricated by a simple solution spin‐coating procedure. Amongst those, the BTBTB based OLED, for example, reaches a high maximum luminance of 8315 cd · m−2 and a maximum luminous efficiency of 1.95 cd · A−1 at a low turn‐on voltage of 2.2 V. This is one of the best performances of a spin‐coated OLED reported so far. In addition, by doping the green and red BNCM s into a blue‐emitting host material poly(9,9‐dioctylfluorene‐2,7‐diyl) high performance white light‐emitting diodes with pure white light emission and a maximum luminance of 4000 cd · m−2 are realized.  相似文献   

11.
Despite the promising expectations of poly(fluorene) (PF)‐type materials as efficient blue‐light‐emitting polymers, the devices based on these materials are not yet fully utilized. Under prolonged operation of the devices, the PF‐type materials undergo degradation with the appearance of a long‐range emission around 2.2–2.3 eV. As a consequence, the emissive color changes from blue to green with a decrease in the device efficiency. Here, an innovative approach that leads to a new blue‐emitting polymer with remarkable color stability is reported. By modifying the chemical structure of PF to inhibit the formation of keto defects, it is demonstrated that the devices exhibit excellent color stability. This new blue‐emitting polymer, poly(2,6‐(4,4‐bis(2‐ethylhexyl)‐4H‐cyclopenta‐[def]phenanthrene)) (PCPP), emits a stabilized, efficient blue electroluminescence without exhibiting any peak in the long‐wavelength region even after prolonged operation of the devices in air.  相似文献   

12.
In this paper polymeric light‐emitting diodes (LEDs) based on alkoxy‐substituted poly(p‐phenylene ethynylene) EHO‐OPPE as emitter material in combination with poly(triphenyldiamine) as hole transport material are demonstrated. Different device configurations such as single‐layer devices, two‐layer devices, and blend devices were investigated. Device improvement and optimization were obtained through careful design of the device structure and composition. Furthermore, the influence of an additional electron transporting and hole blocking layer (ETHBL), spiroquinoxaline (spiro‐qux), on top of the optimized blend device was investigated using a combinatorial method, which allows the preparation of a number of devices characterized by different layer thicknesses in one deposition step. The maximum brightness of the investigated devices increased from 4 cd/m2 for a device of pure EHO‐OPPE to 260 cd/m2 in a device with 25 % EHO‐OPPE + 75 % poly(N,N′‐diphenylbenzidine diphenylether) (poly‐TPD) as the emitting/hole‐transporting layer and an additional electron‐transport/hole‐blocking spiro‐qux layer of 48 nm thickness.  相似文献   

13.
High‐performance, green, orange, and red top‐emitting organic light‐emitting diodes (TOLEDs) with p–i–n homojunction are demonstrated. An excellent ambipolar host, 2,5‐bis(2‐(9H‐carbazol‐9‐yl)phenyl)‐1,3,4‐oxadiazole (o‐CzOXD), which has good thermal and morphological stabilities, a high triplet energy level, and equally high electron and hole mobilities, is chosen as the organic host material for the homojunction devices. By electrical doping, the carrier injection and transporting characteristics are greatly improved. The optical structure is optimized in view of light emission of different colors to enhance the color purity and improve the view characte­ristics. As a result, high efficiency p–i–n homojunction TOLEDs with saturated intrinsic emission of the emitting materials and angular independence of the emission are realized. The performances of these p–i–n homojunction TOLEDs are even higher than the multi‐layer heterojunction bottom‐emitting devices using the same emitting layers.  相似文献   

14.
Novel hole‐transporting dendrimeric molecules containing dioctylfluorene, spirobi(fluorene) and spiro(cylododecane‐fluorene) as the core unit and different numbers of carbazole and thiophene moieties as the peripheral groups are synthesized. All the dendrimers are characterized by 1H NMR, 13C NMR, FTIR, UV–vis, PL spectroscopy, and MALDI‐TOF. They are thermally stable with high glass transition and decomposition temperatures and exhibit chemically reversible redox processes. They are used as the hole‐transporting layer (HTL) material for multilayer organic light emitting diodes (OLEDs) with a low turn‐on voltage of around 2.5 V and a bright green emission with a maximum luminance of around 25400 cd m?2.  相似文献   

15.
Organic photodiodes are presented that utilize solution‐processed perylene diimide bulk heterojunctions as the device photoactive layer. The polymer (9,9′‐dioctylfluorene‐co‐benzothiadiazole; F8BT) is used as the electron donor and the N,N′‐bis(1‐ethylpropyl)‐3,4,9,10‐perylene tetracarboxylic diimide (PDI) derivative is used as the electron acceptor. The thickness‐dependent study of the main device parameters, namely of the external quantum efficiency (EQE), the short‐circuit current (ISC), the open‐circuit voltage (VOC), the fill factor (FF), and the dark current (ID) is presented. In as‐spun F8BT:PDI devices the short‐circuit EQE reaches the maximum of 17% and the VOC value is as high as 0.8 V. Device ID is in the nA mm?2 regime and it correlates with the topography of the F8BT:PDI layer. For a range of annealing temperatures ID is monitored as the morphology of the photoactive layer changes. The changes in the morphology of the photoactive layer are monitored via atomic force microscopy. The thermally induced coalescence of the PDI domains assists the dark conductivity of the device. ID values as low as 80 pA mm?2 are achieved with a corresponding EQE of 9%, when an electron‐blocking layer (EB) is used in bilayer EB/F8BT:PDI devices. Electron injection from the hole‐collecting electrode to the F8BT:PDI medium is hindered by the use of the EB layer. The temperature dependence of the ID value of the as‐spun F8BT:PDI device is studied in the range of 296–216 K. In combination with the thickness and the composition dependence of ID, the determined activation energy Ea suggests a two‐step mechanism of ID generation; a temperature‐independent step of electric‐field‐assisted carrier injection from the device contacts to the active‐layer medium and a thermally activated step of carrier transport across the device electrodes, via the PDI domains of the photoactive layer. Moreover, device ID is found to be sensitive to environmental factors.  相似文献   

16.
Solution‐processed organic light‐emitting diodes (OLEDs) with thermally activated delayed fluorescent (TADF) material as emitter have attracted much attention because of their low cost and high performance. However, exciton quench at the interface between the hole injection layer, poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), and emitting layer (EML) in devices can lead to low device performance. Here, a novel high triplet energy (2.89 eV) and crosslinkable hole‐transporting material grafted with oxetane groups, N,N‐bis(4‐(6‐((3‐ethyloxetan‐3‐yl)methoxy)hexyloxy)phenyl)‐3,5‐di(9H‐carbazol‐9‐yl)benzenamine (Oxe‐DCDPA)), as crosslinked hole transport layer (HTL) into the interface of PEDOT:PSS layer and EML is proposed for prevention of exciton quenching, and among the reported devices with single HTL in solution‐processed TADF‐OLED, the highest external quantum efficiency (EQE)/luminous efficiency (ηL) of 26.1%/94.8 cd A?1 and 24.0%/74.0 cd A?1 are achieved for green emission (DACT‐II as emitter) and bluish‐green emission (DMAC‐TRZ as emitter), respectively. Further improvement, using double HTLs, composed of N,N′‐bis(4‐(6‐((3‐ethyloxetan‐3‐yl)methoxy))‐hexylphenyl)‐N,N′‐diphenyl‐4,4′‐diamine with high hole mobility and Oxe‐DCDPA with high triplet energy, leads to the highest EQE/ηL of 30.8%/111.9 cd A?1 and 27.2%/83.8 cd A?1 for green emission and bluish‐green emission, respectively. These two devices show the high maximum brightness of 81 100 and 70 000 cd m?2, respectively.  相似文献   

17.
We investigate the Amplified Spontaneous Emission (ASE) properties of a prototypical host-guest polymer polymer blend, namely poly(9,9-dioctylfluorene) (PF8) and poly(9,9-dioctylfluorene-co-benzothiadiazole) (F8BT) blend, with different concentration ratio. We show that the initial F8BT content increase causes an increase of the F8BT ASE threshold, even leading to ASE suppression for F8BT contents between 25% and 75%. ASE is then recovered upon further increase of the F8BT relative content. We demonstrate that the ASE properties of the PF8:F8BT are dominated by morphology effects, like submicrometric phase segregation, determining the net gain of the active waveguides.  相似文献   

18.
A new hyperbranched polymer ( HB‐car ), constructed fully by carbazole moieties, is successfully synthesized through a one‐pot Suzuki coupling reaction. The resultant polymer is well‐characterized, and its hole‐transporting ability is studied carefully. The device, in which HB‐car is utilized as a hole‐transporting layer and tris‐(8‐hydroxyquinoline) aluminum as an electron‐emitting layer as well as electron‐transporting layer, gives a much higher efficiency (3.05 cd A–1), than that of a poly(N‐vinylcarbazole) based device (2.19 cd A–1) under similar experimental conditions. The remarkable performance is attributed to its low energy barrier and enhanced hole‐drifting ability in the HB‐car based device. In addition, for the first time, a field‐effect transistor (FET) based on the hyperbranched polymer is fabricated, and the organic FET device shows that HB‐car is a typical p‐type FET material with a saturation mobility of 1 × 10–5 cm2 V–1 s–1, a threshold voltage of –47.1 V, and an on‐to‐off current ratio of 103.  相似文献   

19.
The effect of solution‐processed p‐type doping of hole‐generation layers (HGLs) and electron‐transporting layer (ETLs) are systematically investigated on the performance of solution‐processable alternating current (AC) field‐induced polymer EL (FIPEL) devices in terms of hole‐generation capability of HGLs and electron‐transporting characteristics of ETLs. A variety of p‐type doping conjugated polymers and a series of solution‐processed electron‐transporting small molecules are employed. It is found that the free hole density in p‐type doping HGLs and electron mobility of solution‐processed ETLs are directly related to the device performance, and that the hole‐transporting characteristics of ETLs also play an important role since holes need to be injected from electrode through ETLs to refill the depleted HGLs in the positive half of the AC cycle. As a result, the best FIPEL device exhibits exceptional performance: a low turn‐on voltage of 12 V, a maximum luminance of 20 500 cd m?2, a maximum current and power efficiency of 110.7 cd A?1 and 29.3 lm W?1. To the best of the authors' knowledge, this is the highest report to date among FIPEL devices driven by AC voltage.  相似文献   

20.
Two novel naphtho[1,2‐d]imidazole derivatives are developed as deep‐blue, light‐emitting materials for organic light‐emitting diodes (OLEDs). The 1H‐naphtho[1,2‐d]imidazole based compounds exhibit a significantly superior performance than the 3H‐naphtho[1,2‐d]imidazole analogues in the single‐layer devices. This is because they have a much higher capacity for direct electron‐injection from the cathode compared to their isomeric counterparts resulting in a ground‐breaking EQE (external quantum efficiency) of 4.37% and a low turn‐on voltage of 2.7 V, and this is hitherto the best performance for a non‐doped single‐layer fluorescent OLED. Multi‐layer devices consisting of both hole‐ and electron‐transporting layers, result in identically excellent performances with EQE values of 4.12–6.08% and deep‐blue light emission (Commission Internationale de l'Eclairage (CIE) y values of 0.077–0.115) is obtained for both isomers due to the improved carrier injection and confinement within the emissive layer. In addition, they showed a significantly better blue‐color purity than analogous molecules based on benzimidazole or phenanthro[9,10‐d]imidazole segments.  相似文献   

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