Highly efficient phosphorescent organic light-emitting diodes using a homoleptic iridium(III) complex as a sky-blue dopant

Homoleptic triscyclometalated iridium(III) complex Ir(dbi)₃ was used as a dopant for sky blue phosphorescent organic light-emitting diodes (PHOLEDs). Its photophysical, thermal, electrochemical properties as well as the device performances were investigated. Ir(dbi)₃ exhibited high quantum yield of 0.52 in solution at room temperature. A maximum current efficiency and external quantum efficiency (EQE) of 61.5 cd A⁻¹ and 23.1% were obtained, which are the highest ever reported for blue homoleptic iridium complexes. High efficiencies of 53.5 cd A⁻¹ and 20.1% EQE were achieved even at the luminance of 1000 cd m⁻².     

High-efficiency host free deep-blue organic light-emitting diode with double carrier regulating layers

A bright high-efficiency host-free deep-blue organic light-emitting diode (OLED) is demonstrated. Without the aid of any carrier regulating layer, the deep-blue OLED shows a power efficiency of 1.7 lm W⁻¹ with CIE coordinates of (0.143, 0.098) at 1000 cd m⁻². The respective power efficiency is increased from 1.7 to 2.1 and 2.2 lm W⁻¹ as a single- and double-carrier regulating layers were incorporated. The respective peak luminance also increases from 5250 to 7620 and 9130 cd m⁻², an increment of 45% and 74%. The marked brightness improvement may be attributed to the incorporated carrier regulating layers that effectively lead carriers to recombine in a wider zone. Moreover, the blue emission can be hypsochromic shifted by varying the incorporation position of the carrier regulating layer and the emissive layer thickness.     

Bright green organic light-emitting devices having a composite electron transport layer

A bright green organic light-emitting device employing a co-deposited Al-Alq₃ layer has been fabricated. The device structure is glass/indium tin oxide (ITO)/ N, N′-diphenyl-N, N′- (3-methylphenyl)-1, 1′-biphenyl-4, 4′-diamine (TPD)/tris(8-quinolinolato) aluminum (Alq₃)/ Al-Alq₃/Al. In this device, Al-Alq₃ is used as electron transport layer (ETL). The device shows an operation voltage of 6.1 V at 20 mA/cm². At optimal condition, the brightness of a device at 20 mA/cm² is 2195 cd/m² achieved a luminance efficiency of 5.64lm/W. The result proves that the composite Al-Alq₃ layer is suitable for the ETL of organic light-emitting devices (OLEDs).     

Improved property in organic light-emitting diode utilizing two Al/Alq3 layers

We reported on the fabrication of organic light-emitting devices (OLEDs) utilizing the two Al/Alq₃ layers and two electrodes. This novel green device with structure of Al(110 nm)/tris(8-hydroxyquinoline) aluminum (Alq₃)(65 nm)/Al(110 nm)/Alq₃(50 nm)/N,N′-dipheny1-N, N′-bis-(3-methy1phyeny1)-1, 1′-bipheny1-4, 4′-diamine (TPD)(60 nm)/ITO(60 nm)/Glass. TPD were used as holes transporting layer (HTL), and Alq₃ was used as electron transporting layer (ETL), at the same time, Alq₃ was also used as emitting layer (EL), Al and ITO were used as cathode and anode, respectively. The results showed that the device containing the two Al/Alq₃ layers and two electrodes had a higher brightness and electroluminescent efficiency than the device without this layer. At current density of 14 mA/cm², the brightness of the device with the two Al/Alq₃ layers reach 3693 cd/m², which is higher than the 2537 cd/m² of the Al/Alq₃/TPD:Alq₃/ITO/Glass device and the 1504.0 cd/m² of the Al/Alq₃/TPD/ITO/Glass. Turn-on voltage of the device with two Al/Alq₃ layers was 7 V, which is lower than the others.     

Gravure printed flexible small-molecule organic light emitting diodes

Small-molecule based flexible organic light-emitting diodes (SMOLEDs) were fabricated by gravure printing. In order to modify rheological properties of the functional ink, the green emitter was embedded into an ultrahigh molecular weight polystyrene (UHMW-PS) matrix. The viscosity of the ink was characterized as a function of the small molecule:UHMW-PS weight ratio and solvent type. The gravure printed SMOLEDs exhibited a maximum luminance of 850 cd m⁻², a maximum efficiency of up to 7.7 cd A⁻¹, and turn on voltage of ∼3.5 V. The gravure printed SM:UHMW-PS device exhibits ∼67% higher luminance efficiency comparing to the spin-coated pristine SM device.     

Non-interlayer and color stable WOLEDs with mixed host and incorporating a new orange phosphorescent iridium complex

In this work, we have synthesized a new phosphorescent iridium complex (Bppya)₂Ir(acac), as an orange dopant for organic light-emitting diodes (OLEDs). The device achieved an external quantum efficiency (EQE) of 22.4%, a current efficiency of 49.5 cd A⁻¹ and a power efficiency of 38.9 lm W⁻¹, which are among the highest values for orange OLEDs. Furthermore, color stable and high efficiency phosphorescent white OLED (WOLED) was demonstrated by utilizing a mixed-host in the emissive layers (EMLs) composed of a blue phosphor and the new orange phosphorescent emitter, as well as by avoiding the use of interlayers that commonly exist between different EMLs in WOLEDs. Our WOLED presented decent white emission with maximum efficiencies of 25.3 cd A⁻¹ and 12.6%. Furthermore, the 1931 Commission Internationale de l’Eclairage color coordinates exhibited extremely small variation of (0.3940 ± 0.0102, 0.4323 ± 0.0046) in a wide luminance range from 49 to 38,035 cd m⁻² when driving voltages increased from 4 V to 12 V. The root cause for this excellent color stability is the utilization of the mixed-host to obtain bipolar transport properties in EMLs as well as the eliminating of interlayer between different EMLs, which, on one hand, effectively broaden the exciton recombination zone; on the other hand, reduce the accumulation of triplet excitons at the emissive interface.     

Stable and efficient blue fluorescent organic light-emitting diode by blade coating with or without electron-transport layer

Multi-layer small-molecule blue fluorescent organic light-emitting diode (OLED) is fabricated by blade coating. The emission layer is based on a mixed host of 1-(7-(9,9′-bianthracen-10-yl)-9,9-dioctyl-9H-fluoren-2-yl)pyrene (PT-404) and electron-transport material 2,7-Bis(diphenylphosphoryl)-9,9′ -spirobifluorene (SPPO13), and the blue guest emitter is 4-4′-(1E,1′E)-2,2′-(naphthalene-2,6-diyl)bis(ethane-2,1-diyl)bis(N,N-bis(4-hexyl- Phenyl) aniline) (Blue D). A hole-transport layer of Poly-(9, 9-dioctylfluorenyl-2, 7-diyl)-co-(4, 4-(N-(4-sec-butylphenyl)) diphenylamine) (TFB) is added on top of PEDOT: PSS anode. The electrons are blocked away from TFB by a layer of pure host emission layer of PT-404 between TFB and the mixed –host emission layer. For the device with the electron transport layer of Tris(8-hydroxyquinolinato)aluminum (Alq₃) blade-coated over the emission layer the efficiency and lifetime at initial brightness of 500 cd m⁻² are 7.5 cd A⁻¹ and 150 h for Alq₃/CsF/Al cathode. When the Alq₃/CsF/Al is replaced by simply CsF/Al over the mixed-host emission layer the efficiency and lifetime are 6.4 cd A⁻¹ and 300 h (2 times longer than that of the Alq₃/CsF/Al cathode). The lifetime depends on the electron-hole balance tuned by the mixed-host blending ratio as well as the electron injection from the cathode. This work shows good stability is possible for all-solution-processed blue OLED.     

Constructing a novel single-layer white organic light-emitting device through a new sky-blue fluorescent bipolar host

A novel device concept was realized for simple single-layer small-molecule white organic light emitting devices. The single organic active layer here is simply comprised of a newly synthesized sky-blue fluorescent bipolar host (TPASO) and a common orange phosphorescent dopant. Suppressed singlet Föster energy transfer induced by a low-concentration doping and spontaneous high- to low-lying triplet energy transfer, respectively, lead to sky-blue fluorescence from TPASO and orange phosphorescence from the dopant. The resulting two-organic-component device exhibits a low turn-on voltage of 2.4 V, maximum current/power efficiencies up to 11.27 ± 0.02 cd A⁻¹ and 14.15 ± 0.03 lm W⁻¹, and a warm-white CIE coordinate of (0.42, 0.45) at 1000 cd m⁻².     

High efficiency p-i-n organic light-emitting diodes with a novel n-doping layer

This study demonstrated p-i-n organic light-emitting diodes (OLEDs) incorporating a novel n-doping transport layer which is comprised of cesium iodide (CsI) doped into tris-(8-hydroxyquinoline) aluminum (Alq₃) as n-doping electron transport layer (n-ETL) and a p-doping hole transport layer (p-HTL) which includes molybdenum oxide (MoO₃) doped into 4,4′,4″-tris[2-naphthyl(phenyl)amino] triphenylamine (2-TNATA). The device with a 15 wt.% CsI-doped Alq₃ layer shows a turn on voltage of 2.4 V and achieves a maximum power efficiency of to 4.67 lm/W as well, which is significantly improved compared to these (3.6 V and 3.21 lm/W, respectively) obtained from the device with un-doped Alq₃. This improvement is attributed to an increase in the number of electron carriers in the transportation layer leading to an efficient charge balance in the emission zone. A possible mechanism behind the improvement is discussed based on X-ray photoelectron spectroscopy (XPS).     

Ultra high-efficiency multi-photon emission blue phosphorescent OLEDs with external quantum efficiency exceeding 40%

We developed high-efficiency multi-photon emission (MPE) blue phosphorescent OLEDs with external quantum efficiency exceeding 40% at 100 cd m⁻². In these MPE devices, we used a blue phosphorescent emitter, FIrpic and pyridine-containing electron-transporters, B3PyPB and B3PyMPM, B4PyMPM. We also used a well-known electron-transporter, BCP for comparison. We used a combination of TAPC/MoO₃/Al/Liq layers as the charge-generation layer unit. An optimized MPE device showed an extremely high current efficiency of over 90 cd A⁻¹ and a high power efficiency of over 40 lm W⁻¹ at 100 cd m⁻² without any outcoupling enhancement.     

Alternating current-driven,white field-induced polymer electroluminescent devices with high power efficiency

A solution-processed, all-phosphor, three-color (i.e., blue, green, and red), alternating current-driven white field-induced polymer electroluminescent device (WFIPEL), with low operational voltage, high luminance, high efficiency, high color-rendering index (CRI), and excellent color-stability, was demonstrated. The devices employed poly(vinylidene fluoride–trifluoroethylene–chlorofluoroethylene) [P(VDF–TrFE–CFE)] dielectric modified by single-walled carbon nanotubes (SWNTs) to further improve the dielectric characteristics, as the insulating layer. This significantly lowers the driving voltage of the device. Moreover, hole-generation layer and electron-transporting layer with high conductivity were used to more efficiently form and confine excitons in the emissive layer. The resulting WFIPEL devices show significant improvements in performance as compared to previous reports. Specifically, the devices exhibit a low turn-on voltage of 10 V, a maximum luminance of 7210 cd m⁻², a maximum current efficiency and power efficiency of 33.8 cd A⁻¹ and 10.5 lm W⁻¹, and a CRI of 82. The power efficiency is even 10 times higher than the highest previous report (1 lm W⁻¹).     

Single walled carbon nanotube anodes based high performance organic light-emitting diodes with enhanced contrast ratio

Commercially-available single walled carbon nanotubes (SWCNTs) were used to fabricate SWCNT sheets for anodes of organic light-emitting diodes (OLEDs) by spray-coating process without any use of surfactant or acid treatment. A layer of DMSO doped PEDOT:PSS was spray-coated on the SWCNT sheets to not only lessen the surface roughness to an acceptable level, but also improve the conductivity by more than three orders of magnitude. For our SWCNT-based OLEDs of tris-(8-hydroxquinoline) aluminum (Alq₃) emission layers, a maximum luminance 4224 cd/m² and current efficiency 3.12 cd/A were achieved, which is close to the efficiency of ITO-based OLEDs. We further found out that our OLEDs based on the PEDOT:PSS covered SWCNT anodes tripled the contrast ratio of the conventional indium tin oxide (ITO) based OLEDs.     

Highly efficient,solution-processed orange–red phosphorescent OLEDs by using new iridium phosphor with thieno[3,2-c]pyridine derivative as cyclometalating ligand

A new orange iridium phosphor of (EtPy)₂Ir(acac) with thieno[3,2-c]pyridine derivative as cyclometalating ligand was designed and synthesized. The combination of thieno[3,2-c]pyridine with rigid fluorene moiety enlarged the π conjugation of ligand, and consequently caused the peak emission of (EtPy)₂Ir(acac) red-shift to 588 nm. By using (EtPy)₂Ir(acac) as the orange phosphor, the fully solution-processed PhOLEDs were fabricated with the following device configuration: ITO/PEDOT:PSS/PVK: PBD: (EtPy)₂Ir(acac)/CsF/Al. With PEDOT:PSS 8000 as the hole-injecting material, the orange device achieved a maximum current efficiency of 13.4 cd A⁻¹, a maximum power efficiency of 5.9 lm W⁻¹ and a maximum external quantum efficiency (EQE) of 11.2% with a CIE coordinate of (0.62, 0.38) that falls into the orange–red region. Moreover, at high luminance of 1000 cd m⁻², the device still remained high current efficiency of 8.7 cd A⁻¹ and EQE of 7.3%. To the best of our knowledge, these efficiencies were among the highest ever reported for solution-processed orange–red PhOLEDs.     

Two novel orange cationic iridium(III) complexes with multifunctional ancillary ligands used for polymer light-emitting diodes

Two novel orange cationic iridium complexes [(npy)₂Ir(o-phen)]PF₆ and [(npy)₂Ir(c-phen)]PF₆ were synthesized. Hnpy: 2-(naphthalen-1-yl)pyridine; o-phen: a 1,10-phenanthroline derivative containing an electron-transporting functional group of 2,5-diphenyl-1,3,4-oxadiazole and a crystallization-resistant tert-butyl functional group; c-phen: a 1,10-phenanthroline derivative containing a hole-transporting functional group of carbazole and a crystallization-resistant 2-ethylhexyl functional group. Both of them are amorphous and possess high thermal stability with 5% weight-reduction temperatures (ΔT_5%) of 386 °C and 383 °C, and glass-transition temperatures (T_g) of 267 °C and 195 °C respectively. They were used as phosphorescent dopants in polymer light-emitting diodes (PLEDs) fabricated by solution-processed technology with configuration of ITO/PEDOT:PSS/PVK:PBD:iridium complex/TPBI/CsF/Al. At the optimal doping concentration of 2.0 wt%, the corresponding PLEDs exhibited the maximum current efficiencies of 9.1 cd A⁻¹ and 10.0 cd A⁻¹, the maximum external quantum efficiencies of 6.5% and 7.1%, and the maximum luminance of 2314 cd m⁻² and 3157 cd m⁻² respectively, with the same CIE coordinates of (0.57, 0.40). The results indicate that cationic iridium complexes are promising candidates for PLED applications when they are designed reasonably.     

High-performance OLEDs based on 4,5-diaza-9,9′-spirobifluorene ligated rhenium(I) complex with enhanced steric hindrance

Highly efficient and emitter concentration insensitive phosphorescent electroluminescent devices based on a novel rhenium(I) [Re(I)] complex, i.e., (4,5-diaza-9,9′-spirobifluorene)Re(CO)₃Br (Re-DSBF), were established. Non-doped device based on Re-DSBF as emitter exhibited outstanding performances with the peak luminance of 8531 cd m⁻² and maximum current efficiency of 16.8 cd A⁻¹, which were the highest reported to date for non-doped phosphorescent electroluminescent devices based on Re(I) emitters. Such excellent performances are closely related to the steric hindrance, large Stokes shift, and short luminescent lifetime of Re-DSBF complex. The luminescent mechanisms of those devices were also investigated.     

Solution-processable tandem solid-state light-emitting electrochemical cells

Compared to organic light-emitting diodes (OLEDs), solid-state light-emitting electrochemical cells (LECs) exhibit simple single-layered structure and low operating voltages due to in situ electrochemical doped layers. However, device efficiencies of LECs are usually lower than those of sophisticatedly designed OLEDs. Furthermore, device efficiencies and lifetimes of LECs degrade significantly as brightness increases. In this work, we demonstrate tandem LECs to obtain nearly doubled light outputs (μW cm⁻²) in comparison with single-layered LECs under similar current densities. Since the output EL emission is modified by microcavity effect of the device structure, the EL spectra of tandem LECs exhibit EL emission peak at ca. 625 nm while the EL spectra of single-layered LECs center at ca. 660 nm. Better spectral overlap between the EL spectrum of tandem LECs and the luminosity function results in further enhanced candela values, rendering a tripled brightness (cd m⁻²). The device efficiencies can be optimized by adjusting the thickness of the connecting layer between the two emitting units of the tandem devices. The peak external quantum efficiency achieved in tandem LECs is up to 5.83%, which is higher than twice of that obtained in single-layered LECs due to improved carrier balance. When single-layered and tandem LECs are biased under higher voltages to reach similarly higher brightness, tandem LECs show higher device efficiencies and longer lifetimes simultaneously. These results indicate that device efficiencies and lifetimes of LECs can be improved by employing a tandem device structure.     

Efficient nondoped blue organic light-emitting diodes based on phenanthroimidazole-substituted anthracene derivatives

A series of new blue materials based on highly fluorescent di(aryl)anthracene and electron-transporting phenanthroimidazole functional cores: 2-(4-(anthracen-9-yl)phenyl)-1-phenyl-1H-phenanthro[9,10-d]imidazole (ACPI), 2-(4-(10-(naphthalen-1-yl)anthracen-9-yl)phenyl)-1-p-henyl-1H-phenanthro[9,10-d]imidazole (1-NaCPI), 2-(4-(10-(naphthalen-2-yl)anthracen-9-yl)phenyl)-1-phenyl-1H-phenanthro[9,10-d]imidazole (2-NaCPI) were designed and synthesized. These materials exhibit good film-forming and thermal properties as well as strong blue emission in the solid state. To explore the electroluminescence properties of these materials, three layer, two layer and single layer organic light-emitting devices were fabricated. With respect to the three layer device 4 using ACPI as the emitting layer, its maximum current efficiency reaches 4.36 cd A⁻¹ with Commission Internationale del’Eclairage (CIE) coordinates of (0.156, 0.155). In the single layer device 10 based on ACPI, maximum current efficiency reaches 1.59 cd A⁻¹ with Commission Internationale del’Eclairage (CIE) coordinates of (0.169, 0.177). Interestingly, both device 4 and 10 has low turn on voltage and negligible efficiency roll off at high current densities.     

Influence of connecting units’ thicknesses on tandem organic devices’ performances

The present work investigates the influence of the Alq₃:Mg and MoO₃ thicknesses in the connecting unit on the performance of tandem organic light-emitting devices (OLEDs). By systematically varying the Alq₃:Mg and MoO₃ thicknesses, we obtained a higher current efficiency of 37.3 cd/A for a device with 30 nm Alq₃:Mg and 3 nm MoO₃ layer as connecting units. The optimal device performance is enhanced by at least 14%, compared with those of devices we fabricated in this paper. It suggests that appropriate Alq₃:Mg and MoO₃ thicknesses can enhance the charge generating ability for connecting units. On the other hand, it was found that the charge transporting layer would decrease strongly because of much thicker or thinner MoO₃ thicknesses. The results demonstrate that it is an effective method to improve the performance of OLEDs by using a optimal thickness for Alq₃:Mg and MoO₃ layers.     

Increase of current density and luminance in organic light-emitting diode with reverse bias driving

When applying the voltage pulses (6 V) to the organic light-emitting diode based on tris(8-hydroxyquinolinato) aluminium (Alq₃) as the electron transporting layer, current density and luminance increased by 16% and 20%, respectively, by providing the reverse bias (−16 V) during the off-period. By using displacement current measurement, we can deduce that such an enhancement resulted from the interfacial positive charges trapped at the Alq₃/cathode interface, with the relaxation time ∼0.4 ms. By doping the organic material as the carrier trapping sites at Alq₃/cathode interface, such current density and luminance increase can be further enhanced. 25% and 36% increase in current density and luminance was demonstrated with such driving technique, respectively.     

Efficient fluorescent white organic light-emitting devices based on a ultrathin 5,6,11,12-tetraphenylnaphthacene layer

White organic light-emitting devices (OLEDs) were fabricated using a ultrathin layer 5,6,11,12-tetraphenylnaphthacene as the yellow light-emitting layer and p-bis(p-N,N-diphenyl-aminostyryl)benzene (DSA-ph) doped in 2-methyl-9,10-di(2-naphthyl)anthracene (MADN) matrix as the blue light-emitting layer. The thickness of rubrene ultrathin layer will seriously affect the device performance, and the device with 1 nm rubrene achieves the best performance, with the maximum luminance of 33,152 cd/m² at 11 V and the maximum current efficiency of 8.69 cd/A at 7 V.