High-performance azure blue quantum dot light-emitting diodes via doping PVK in emitting layer

Highly bright and efficient azure blue quantum dot-based light-emitting diodes (QD-LEDs) have been demonstrated by employing ZnCdSe core/multishell QDs as emitters and the crucial development we report here is the ability to dramatically enhance the efficiency and brightness through doping poly vinyl(N-carbazole) (PVK) in the emissive layer to balance the charge injection. The best device displays remarkable features like maximum luminance of 13,800 cd/m², luminous efficiency of 6.41 cd/A, and external quantum efficiency (EQE) of 8.76%, without detectable red-shift and broadening in electroluminescence (EL) spectra with increasing voltage as well as good spectral matching between photoluminescence (PL) and EL. Such azure blue quantum-dot LEDs show a 140% increase in external quantum efficiency compared with QD-LEDs without PVK. More important, the peak efficiency of the QD-LEDs with PVK dopant is achieved at luminance of about 1000 cd/m², and high efficiency (EQE > 8%) can be maintained with brightness ranging from 200 to 2400 cd/m². There are two main aspects of the role of PVK in the proposed system. Firstly, the lower HOMO of PVK than (poly[9,9-dioctylfluorene-co-N-[4-(3-methylpropyl)]-diphenylamine] (TFB) can reduce the potential barrier for 0.4 eV at the interface of QDs and hole transport layer which could result in higher hole injection efficiency along with good EQE as compared to TFB-only HTLs. Secondly, with PVK acting as buffer layer of TFB and QDs, the exciton energy transfer from the organic host to the QDs can be effectively improved.     

Wide color-range tunable and low roll-off fluorescent organic light emitting devices based on double undoped ultrathin emitters

We demonstrated a novel wide color-range tunable, highly efficient and low efficiency roll-off fluorescent organic light-emitting diode (OLED) using two undoped ultrathin emitters having complementary colors and an interlayer between them. The OLED can be tuned to emit sky blue (0.22, 0.30), cold white (0.29, 0.33), warm white (0.43, 0.42) and yellow (0.40, 0.45) according to the Commission Internationale de L’Eclairage (CIE) 1931 (x, y) chromaticity diagram. The device fabrication was simplified by eliminating doping process in the emission layers. The influence of interlayer thickness on luminous efficiency, efficiency roll-off and color tuning mechanism is thoroughly studied. The recombination zone is greatly broadened in the optimized device, which contributes to stable energy transfer to both emitters and suppressed concentration quenching. With a threshold voltage of 2.82 V, the color tunable organic light emitting diode (CT-OLED) shows a maximum luminance of 39,810 cd/m², a peak external quantum efficiency (EQE) 6% and the efficiency roll-off as low as 11.1% at the luminance from 500 cd/m² to 5000 cd/m². This structure of CT-OLED has great advantages of easy fabrication and low reagent consumption. The fabricated CT-OLEDs are tunable from cold white (0.30, 0.36) to warm white (0.43, 0.42) with correlated color temperature (CCT) 6932 K and 3072 K, respectively, demonstrating that our proposed approach helps to meet the need for lighting with various CCTs.     

Low driving voltage white organic light-emitting diodes with high efficiency and low efficiency roll-off

Single emission layer white organic light-emitting diodes (WOLEDs) showing high color stability, low turn-on voltage, high efficiency and low efficiency roll-off by incorporating iridium(III) bis[(4,6-difluo-rophenyl)-pyridinato-N,C2] (FIrpic) and bis(2-phenylbenzothiazolato) (acetylacetonate)iridium(III) (Ir(BT)₂(acac)) phosphors dyes have been demonstrated. Our WOLEDs without any out-coupling schemes as well as n-doping strategies show low operating voltages, low turn-on voltage (defined for voltage to obtain a luminance of 1 cd/m²) of 2.35 V, 79.2 cd/m² at 2.6 V, 940.5 cd/m² at 3.0 V and 10 300 cd/m² at 4.0 V, respectively, and achieve a current efficiency of 40.5 cd/A, a power efficiency of 42.6 lm/W at a practical brightness of 1000 cd/m², and a low efficiency roll-off 14.7% calculated from the maximum efficiency value to that of 5000 cd/m². Such improved properties are attributed to phosphors assisted carriers transport for achieving charge carrier balance in the single light-emitting layer (EML). Meanwhile the host–guest energy transfer and direct exciton formation process are two parallel pathways serve to channel the overall excitons to dopants, greatly reduced the unfavorable energy losses.     

A hybrid white organic light-emitting diode with stable color and reduced efficiency roll-off by using a bipolar charge carrier switch

A hybrid white organic light-emitting diode (WOLED) with an emission layer (EML) structure composed of red phosphorescent EML/green phosphorescent EML/spacer/blue fluorescent EML was demonstrated. This hybrid WOLED shows high efficiency, stable spectral emission and low efficiency roll-off at high luminance. We have attributed the significant improvement to the wide distribution of excitons and the effective control of charge carriers in EMLs by using mixed 4,4′,4″-tri(9-carbazoyl) triphenylamine (TCTA) and bis[2-(2-hydroxyphenyl)-pyridine] beryllium (Bepp₂) as the host of phosphorescent EMLs as well as the spacer. The bipolar mixed TCTA:Bepp_2, which was proved to be a charge carrier switch by regulating the distribution of charge carriers and then the exciton recombination zone, plays an important role in improving the efficiency, stabilizing the spectrum and reducing the efficiency roll-off at high luminous. The hybrid WOLED exhibits a current efficiency of 30.2 cd/A, a power efficiency of 32.0 lm/W and an external quantum efficiency of 13.4% at a luminance of 100 cd/m², and keeps a current efficiency of 30.8 cd/A, a power efficiency of 27.1 lm/W and an external quantum efficiency of 13.7% at a 1000 cd/m². The Commission Internationale de l’Eclairage (CIE) coordinates of (0.43, 0.43) and the color rendering index (CRI) of 89 remain nearly unchanged in the whole range of luminance.     

蓝绿色磷光OLED的制备及发光性能研究

以mCP为主体发光材料,蓝绿色磷光染料BGIr1作 为掺杂剂,制备了6种不同BGIr1掺杂量的蓝绿色磷光有机电致发光器件(OLED),研究了不 同掺杂量对蓝绿色磷光OLED器件发光特性的影 响。制得器件的结构为ITO/MoO₃(20nm)/NPB(40nm)/mCP:BGIr1(x%,30nm)/BCP(10nm)/Alq₃(20 nm)/LiF/Al(100nm),其中x%为发光层中磷光染料BGIr1的掺杂量(质量分数)。结果表明,BGIr1掺杂量 为18%时,获得器件的发光性能最佳。18% BGIr 1掺杂器件在488nm和 512nm处获得两个主发射峰,当电 流密度为26.5mA/cm²时,获得最大发光效率为6.2cd/A;在15V驱动电压下,获得最大亮度为6970cd/cm², CIE坐标为(0.17,0.31)。这说明,BGI r1掺杂改善了器件的发光亮度和色纯度,提高了器件的发光效率。     

Understanding the influence of doping in efficient phosphorescent organic light-emitting diodes with an organic p–i–n homojunction

We report on the development and detailed investigation of highly efficient p–i–n phosphorescent organic light-emitting diodes (PhOLEDs) using 4,4′-bis(carbazol-9-yl)-biphenyl (CBP) as a single organic semiconductor matrix. Following optimization of doping concentration of both the phosphorescent emitter molecule and of the p- and n-type dopants, an external quantum efficiency (EQE) of 15% and a power efficiency (PE) of 28 lm/W are realized at a luminance of 1000 cd/m². These values are comparable to the state-of-the-art for conventional complex multilayered PhOLEDs. By analyzing the device characteristics (i.e. electroluminescence spectra, the current density–voltage behavior of single carrier devices, the transient electroluminescent decay, and the impedance spectroscopy response), we find that the device performance is closely linked to the charge carrier balance in the device, which in turn is governed by the interplay of the conductivities of the doped layers and the transport of each charge carrier species within the emitting layer.     

Hydroxyethyl cellulose filled with M2+ chelate complexes with ethylenediaminetetraacetic acid (EDTA) as an effective electron-injection layer for polymer light-emitting diodes

An effective electron-injection layer (EIL) is crucial to the development of highly efficient polymer light-emitting diodes (PLEDs) using stable, high work-function aluminium as the cathode. This work presents the first investigation using hydroxyethyl cellulose (HEC), filled with chelate complexes [(CH₃COO)₂-M, EDTA-M; M: Ca²⁺, Mg²⁺], as an electron-injection layer (EIL) to fabricate multilayer polymer light-emitting diodes (ITO/PEDO:PSS/HY-PPV/EIL/Al) by spin-coating processes. Devices based on HEC doped with EDTA-M provided the best performance. The maximum luminance and maximum current efficiency of polymer light-emitting diodes with EDTA-Ca in an HEC layer were 7502 cd/m² and 2.85 cd/A, respectively, whereas those with EDTA-Mg were 8443 cd/m² and 3.12 cd/A, which was approximately seven- to eight-fold of that without EIL. This performance enhancement was attributed to electron donation from the chelator that reduces metal cations to a “pseudo-metallic state”, enabling it to act as an intermediate step to facilitate electron injection. The results demonstrate that chelates of bivalent cations with EDTA can potentially serve as electron-injection materials for optoelectronic applications.     

Great improvement of operation-lifetime for all-solution OLEDs with mixed hosts by blade coating

We investigated some effective device designs and fabrication methods for long operation-lifetime all-solution-processed Phosphorescent OLEDs (PhOLEDs) and fluorescent OLEDs with mixed-hosts system and thin Poly [(9, 9-dioctylfluorenyl-2, 7-diyl)-co-(4, 4′-(N-(4-sec-butylphenyl) diphenylamine)] (TFB). The all-solution-processed green PhOLEDs had high current efficiency (30.3 cd/A) and long operation-lifetime. The best half-lifetime of green PhOLEDs with thin HTL, MH-hosts EML and optimized deposition was 310 h at an initial luminance 1000 cd/m², 250 h at an initial luminance 500 cd/m² for green PhOLEDs with thin HTL, and MH-hosts EML, and the lifetime of triple layer PhOLEDs device was only 0.5 h for the same materials. The red PhOLEDs exhibited a high current efficiency (10.93 cd/A) and half-lifetime with 157.9 h at an initial luminance 500 cd/m². For the blue fluorescent OLEDs, the thin polymer TFB, mixed-hosts EML, double EMLs and optimization deposition yield a high current efficiency (5.68 cd/A) and long operation-lifetime with 117.7 h at an initial luminance 500 cd/m². Single host fluorescent device had half-lifetime of 73.5 h only at an initial luminance 100 cd/m². Finally, by doping red emitter Rubrene into stable blue device, we achieved soft yellow OLEDs with high efficiency (10.87 cd/A) and 8 fold improvement operation-lifetime (1200 h). We believe that such all-solution-processed OLEDs which showed greatly improved operational lifetimes would be suitable for the indoor supportive lighting with natural colors.     

High efficiency green phosphorescent top-emitting organic light-emitting diode with ultrathin non-doped emissive layer

Ultrathin non-doped emissive layer (EML) has been employed in green phosphorescent top-emitting organic light-emitting diodes (TOLEDs) to take full advantages of the cavity standing wave condition in a microcavity structure. Much higher out-coupling efficiency has been observed compared to conventional doped EML with relatively wide emission zone. A further investigation on dual ultrathin non-doped EMLs separated by a special bi-layer structure demonstrates better charge carrier balance and improved efficiency. The resulting device exhibits a high efficiency of 125.0 cd/A at a luminance of 1000 cd/m² and maintains to 110.9 cd/A at 10,000 cd/m².     

High-efficiency orange and white phosphorescent organic light-emitting diodes based on homojunction structure

We demonstrate high-efficiency orange and white phosphorescent organic light-emitting diodes based on homojunction structure. Excellent performance is realized by using step-graded p- and n-type doping structure in orange homojunction device. The resulting orange homojunction device exhibits a maximum current efficiency of 30.0 cd/A and low efficiency roll-off. The improvements are mainly attributed to the utilization of step-graded doped profile, which facilitates balanced charge carrier injection and transport. Moreover, one optimized white homojunction device based on two complementary colors shows a maximum efficiency of 15.4 cd/A, and superior color-stability in a wide range of luminance.     

Improved electron injection from silver electrode for all solution-processed polymer light-emitting diodes with Cs2CO3:conjugated polyelectrolyte blended interfacial layer

This study demonstrates the incorporation of a Cs₂CO₃:conjugated polyelectrolyte blended interfacial layer between the emissive layer and a silver (Ag) cathode, for realizing all-solution processed polymer light-emitting diodes. For a device with poly(9,9-dioctylfluorene-co-benzothiadiazole) (F8BT) as the emissive layer, this approach improves the maximum luminance of approximately 80,000 cd/m² and maximum current efficiency of 10.6 cd/A. It is clarified that the interfacial layer prevents Ag nanoparticles from penetrating into the emissive layer, resulting in yellow–green emission from F8BT. We also demonstrate the possibility of all-solution processed polymer light-emitting diodes utilizing solution-processed Cs₂CO₃:conjugated polyelectrolyte interfacial layer and Ag nano-ink.     

Fluorene bilayer for polymer organic light-emitting diode using efficient ionization method for atomized droplet

We present a solution-processed planar fluorene bilayer by an ultrasonic atomized deposition method in combination with a needle electrode as an ionization part for an atomized droplet. An important advantage of our method is that the atomized droplet is efficiently charged using a needle electrode, which speeds up the deposition rate of the polymer thin film. The deposition rate increases 2 to 3 times compared to a that obtained with a conventional technique without using the ionization method, and real-time monitoring of landed droplets indicates that the number of droplets increased as the voltage applied to the needle electrode was increased, owing to the highly charged atomized droplets. Furthermore, the TFB/F8BT bilayer was achieved by optimizing the substrate temperature, and the polymer organic light-emitting diode exhibits a luminance value exceeding 12,000 cd/m² by insertion of the TFB as an electron blocking layer. The maximum current efficiency of the fluorene bilayer device was 6.64 cd/A, which was a 3.2-fold increase compared to that obtained with the reference device without the TFB electron blocking layer.     

Deep blue light-emitting diode based on high molecular weight poly(9,9-dioctylfluorene) with high efficiency and color stability

A highly efficient deep blue polymer light-emitting diode based on poly(9,9-dioctylfluorene) is demonstrated. The performance is found to increase significantly with the molecular weight. Two different molecular weights are compared, one is 71,000 and the other is 365,000. The electroluminescent efficiency and color stability are improved by slightly doping hole traps into the emission layer and bilayer structure. The maximum efficiency is 3.8 cd/A with the corresponding external quantum efficiency of 3.7% at deep blue with Commission Internationale de L’Eclairage (CIE) coordinate at (0.15, 0.09). Stable blue emission is maintained up to 6600 cd/m² without growth of green shoulder in emission spectrum.     

Enhancing the efficiency of alternating current driven organic light-emitting devices by optimizing the operation frequency

We report efficient and bright organic light-emitting devices operated by capacitive energy coupling. In this approach, the organic layers are enclosed between sputter-deposited hafnium dioxide layers to prevent charge carrier injection. When a sinusoidal voltage signal is applied to the electrodes, the devices emit bright green light whereas no detectable emission is generated upon application of a constant voltage. The efficiency of the process depends heavily on the frequency of the applied voltage signal. By optimizing the driving scheme, a record luminous efficacy for AC driven OLEDs of 2.7 lm/W at 500 cd/m² is achieved.     

Stable Light-Emitting Electrochemical Cells Using Hyperbranched Polymer Electrolyte

The choice of an adequate electrolyte is a fundamental aspect in polymer light-emitting electrochemical cells (PLECs) as it provides the in situ electrochemical doping and influences the performance of these devices. In this study, a hyperbranched polymer (Hybrane DEO750 8500) blended with a Li salt is used as a novel electrolyte in state-of-the-art Super Yellow (a polyphenylenevinylene) based LECs. Due to the desirable properties of the hyperbranched polymer and the homogeneous and smooth films that it forms with the emitting polymer, PLEC with excellent electroluminescent properties are obtained using a pulsed current bias scheme. The devices are very stable, with lifetimes in excess of 2000 h with initial luminance values above 450 cd m⁻², a peak efficiency of 12.6 lm W⁻¹, and sub-minute turn-on times. The stability of the devices is also studied by measuring the photoluminescence (PL) of the semiconductor during electroluminescent operation. The findings suggest that it is possible to observe the quenching of the PL in vertically stacked devices due to the advancement of the doped fronts in the film and an immediate PL recovery when the bias is removed.     

Highly efficient inverted blue light-emitting diodes by thermal annealing and interfacial modification

Inverted polymer light-emitting diodes (IPLED) were fabricated by using polyfluorene (PF-FSO10) as the emissive layer, polyethyleneimine ethoxylate (PEIE) as the interlayer, and 1,3,5-tris(N-phenylbenzimidazol-2-yl)benzene (TPBI) as the electron-transport layer with the configuration of ITO/ZnO/PEIE/TPBI/PF-FSO10/MoO₃/Al. Thermal annealing PF-FSO10 made the hole transporting ability decreased, the electron transporting ability enhanced, and thus, jointly promoted the carrier balances in the emissive layer. Inserting a TPBI layer between the PEIE and PF-FSO10 much enhanced the electron transportation and reduced the exciton quench on the ZnO interface. Therefore, the inverted blue light-emitting diode was obtained with a luminous efficiency of 6.8 cd A⁻¹ (an external quantum efficiency of 7.1%), and the CIE color coordinates of (0.15, 0.15), which was among the highest efficiency values in solution-processed inverted blue fluorescent light-emitting diodes.     

Single-Layered Hybrid DBPPV-CdSe–ZnS Quantum-Dot Light-Emitting Diodes

We have demonstrated the fabrication and characterization of single-layered hybrid polymer-quantum-dot light-emitting diodes (PQD-LEDs) with the emissive composite film of 2,3-dibutoxy-1,4-poly(phenylene vinylene) (DBPPV) and inorganic CdSe-ZnS core/shell quantum dots (QDs). It is observed that both the electrical and optical characteristics are significantly improved by adjusting the thickness of the emissive layer. For the device with composite film thickness of 103 nm, the turn-on voltage is 4.1 V, and the maximum luminance of 4100 cd/m as well as maximum luminous efficiency of 1.35 cd/A are achieved at 9.6 and 7.6 V, respectively. The optimum emission contribution of luminescence from QDs to the whole luminance is 38%. However, the QD luminescence is mainly limited by the Foumlrster energy transfer mechanism and no obvious QD-related injected carrier trapping is observed. To our knowledge, this is the first demonstration of PQD-LEDs that consist of DBPPV and CdSe-ZnS QDs.     

Controllable molecular doping in organic single crystals toward high-efficiency light-emitting devices

Organic single-crystalline semiconductors have drawn significant attention in the area of organic electronic and optoelectronic devices due to their superiorities of highly ordered structure, high carrier mobility and low impurity content. Molecular doping technique has made great progress in improving device performance via optimizing the optical and electrical properties of organic semiconductors. In particular, this technique has been attempted by taking fluorescent dye-molecules as the emissive dopants to tune emission color and improve device performance of organic single crystals. Up to now, there are few reports about the use of molecular doping in organic single crystals to optimize their intrinsic electrical properties. Here, we have introduced the controllable molecular doping as a feasible approach toward manipulating charge carrier transport properties of organic single crystals. Upon optimization of doping concentration, balanced carrier transport can be realized in 5,5′-bis(4-trifluoromethyl phenyl) [2,2’] bithiophene (P2TCF₃)-doped 1,4-bis(4-methylstyryl) benzene (BSB–Me) crystals. Organic light-emitting devices (OLEDs) based on these doped crystals achieve a maximum luminance of 423 cd/m² and current efficiency of 0.48 cd/A. It demonstrates that high-efficiency crystal-based OLEDs are of great significance for the development of organic electronics, especially for display and lighting applications.     

Highly efficient quasi-two dimensional perovskite light-emitting diodes by phase tuning

Tetraphenylphosphonium chloride (TPPCl) is used as an additive in the antisolvent for preparing the quasi-two Dimensional (quasi-2D) perovskite film. This strategy is not only beneficial for the morphology formation but also the phase tuning of the quasi-2D perovskite film. Highly efficient and stable perovskite light-emitting diodes (PeLEDs) were achieved with the maximum luminance of 35,000 cd/m², the maximum current efficiency of 48.0 cd/A and the maximum external quantum efficiency (EQE) of 12.42%. Due to the reduced exciton quenching rate, improved charge carrier injection and transport ability, the electroluminescent performance of the TPPCl-based PeLEDs has been enhanced.