Highly efficient green top-emitting organic light-emitting devices with metal electrode structure

In this work, the electrical and optical characteristics of top-emitting organic light-emitting device (TEOLED) using metal Ag as anode with different thicknesses have been investigated. The emission peak of fabricated TEOLED is 512 nm for a full-width at half-maximum (FWHM) of 48 nm in forward direction. The TEOLED turns on at 3 V with luminance of 2.38 cd/m² and reaches 16,300 cd/m² at 9 V. The maximum of current efficiency is 5.2 cd/A at 7 V, corresponding to the external quantum efficiency of 1.72%.     

Carrier transport of inverted quantum dot LED with PEIE polymer

An inverted-type quantum-dot light-emitting-diode (QD LED), employing low-work function organic material polyethylenimine ethoxylated (PEIE) as electron injection layer, was fabricated by all solution processing method, excluding anode electrode. From transmission electron microscopy (TEM) and scanning electron microscopy (SEM) studies, it was confirmed that CdSe@ZnS QDs with 7 nm size were uniformly distributed as a monolayer on PEIE layer. In this inverted QD LED, two kinds of hybrid organic materials, [poly (9,9-di-n-octyl-fluorene-alt-benzothiadiazolo)(F8BT) + poly(N,N′-bis(4-butylphenyl)-N,N′-bis(phenyl)benzidine (poly-TPD)] and [4,4′-N,N′-dicarbazole-biphenyl (CBP) + poly-TPD], were adopted as hole transport layer having high highest occupied molecular orbital (HOMO) level for improving hole transport ability. At a low-operating voltage of 8 V, the device emits orange and red spectral radiation with high brightness up to 2450 and 1420 cd/m², and luminance efficacy of 1.4 cd/A and 0.89 cd/A, respectively, at 7 V applied bias. Also, the carrier transport mechanisms for the QD LEDs are described by using several models to fit the experimental I–V data.     

Cadmium-free quantum dots based violet light-emitting diodes: High-efficiency and brightness via optimization of organic hole transport layers

Bright and efficient violet quantum dot (QD) based light-emitting diodes (QD-LEDs) with heavy-metal-free ZnSe/ZnS have been demonstrated by choosing different hole transport layers, including poly(4-butyl-phenyl-diphenyl-amine) (poly-TPD), poly[9,9-dioctylfluorene-co-N-[4-(3-methylpropyl)]-diphenylamine] (TFB), and poly-N-vinylcarbazole (PVK). Violet QD-LEDs with maximum luminance of about 930 cd/m², the maximum current efficiency of 0.18 cd/A, and the peak EQE of 1.02% when poly-TPD was used as HTL. Higher brightness and low turn-on voltage (3.8 V) violet QD-LEDs could be fabricated when TFB was used as hole transport material. Although the maximum luminance could reach up to 2691 cd/m², the devices exhibited only low current efficiency (∼0.51 cd/A) and EQE (∼2.88%). If PVK is used as hole transport material, highly efficient violet QD-LEDs can be fabricated with lower maximum luminance and higher turn-on voltages compared with counterpart using TFB. Therefore, TFB and PVK mixture in a certain proportion has been used as HTL, turn-on voltage, brightness, and efficiency all have been improved greatly. The QD-LEDs is fabricated with 7.39% of EQE and 2856 cd/m² of maximum brightness with narrow FWHM less than 21 nm. These results represent significant improvements in the performance of heavy-metal-free violet QD-LEDs in terms of efficiency, brightness, and color purity.     

Organic alternating current electroluminescence device based on 4,4′-bis(N-phenyl-1-naphthylamino) biphenyl/1,4,5,8,9,11-hexaazatriphenylene charge generation unit

An organic alternating current electroluminescence (OACEL) device based on 4,4′-bis(N-phenyl-1-naphthylamino) biphenyl (NPB)/1,4,5,8,9,11-hexaazatriphenylene (HAT-CN)/tris(8-hydroxy-quin-olinato) aluminum (Alq₃) doped with cesium carbonate (Cs₂CO₃) internal charge generation unit is demonstrated. Maximum luminance of 299 cd/m² is observed for Alq₃ doped with 10-(2-Benzothiazolyl)-2,3,6,7-tetrahydro-1,1,7,7-tetramethyl-1H,5H, 11H-(1) benzopyropyrano (6,7-8-I,j)quinolizin-11-one (C545T) fluorescent emission layer when driven with a peak–peak voltage of 80 V at 120 kHz. The key charge-generation role of NPB/HAT-CN interface is studied experimentally. Furthermore, influence of evaporation sequence of this internal charge generation unit on OACEL performance is investigated. This work demonstrated that the undoped charge generation unit – NPB/HATCN, can also be a good candidate for charge generation unit of OACEL device.     

High-efficiency red electroluminescence from europium complex containing a neutral dipyrido(3,2-a:2′,3′-c)phenazine ligand in PLEDs

In order to obtain high-efficiency monochromatic red emission in polymer light-emitting devices, a tris(dibenzoylmethanato)(dipyrido(3,2-a:2′,3′-c)phenazine) europium [Eu(DBM)₃(DPPZ)] doped single-emissive-layer devices were fabricated using a blend of poly(9,9-dioctyl-fluorence) and 2-tert-butyl-phenyl-5-biphenyl-1,3,4-oxadiazole as a host matrix by solution process. Significantly improved electro-luminescent properties with sharp red emission at 611.5 nm were displayed in the Eu(DBM)₃(DPPZ)-doped devices at dopant concentrations from 1 to 8 wt.%. The highest luminance up to 1783 cd/m² at 2 wt.% dopant concentration, as well as the maximum external quantum efficiency of 2.5% and current efficiency of 3.8 cd/A were obtained at 1 wt.% dopant concentration.     

Efficient fluorescent white organic light-emitting diodes using co-host/emitter dual-role possessed di(triphenyl-amine)-1,4-divinyl-naphthalene

Efficient fluorescent white organic light-emitting diodes with low carrier-injection barriers were fabricated with device structure of indium tin oxide/N,N′-bis-(1-naphthy)-N,N′-diphenyl-1,1′-biphenyl-4-4′-diamine/white emission layer/1,3,5-tris(N-phenyl-benzimidazol-2-yl)benzene/lithium fluoride/aluminium. By blending in the blue host of 1-butyl-9,10-naphthalene-anthracene in the emissive layer an efficient electro-luminescent greenish-blue co-host of di(triphenyl-amine)-1,4-divinyl-naphthalene, with the doping of a trace amount of red dye of 4-(dicyano-methylene)-2-methyl-6-(julolidin-4-yl-vinyl)-4H-pyran, bright and colour-stable white emission with high power-efficiency of 14.6 lm/W at 100 cd/m² or current efficiency of 19.2 cd/A at 300 cd/m² or 18.7 cd/A at 10,000 cd/m² was obtained. The resulted synergistic increase in brightness and efficiency may be attributed to the presence of cascading new routes with comparatively lower electron injection barrier.     

High-performance green phosphorescent top-emitting organic light-emitting diodes based on FDTD optical simulation

We have successfully applied finite-difference time-domain (FDTD) method in top-emitting organic light-emitting diodes (TOLEDs) for structure optimization, demonstrating good agreement with experimental data. A mixed host with both hole transport and electron transport materials is employed for the green phosphorescent emitter to avoid charge accumulation and broaden the recombination zone. The resulting TOLEDs exhibit ultra-high efficiencies, low current efficiency roll-off, and a highly saturated color, as well as hardly detectable spectrum shift with viewing angles. In particular, a current efficiency of 127.0 cd/A at a luminance of 1000 cd/m² is obtained, and maintains to 116.3 cd/A at 10,000 cd/m².     

High-efficiency and multi-function blue fluorescent material for organic electroluminescent devices

We demonstrate one high-efficiency blue fluorescent material, N-(4-((E)-2-(6-((E)-4-(diphenylamino)styryl)naphthalen-2-yl)vinyl)phenyl)-N-phenylbenzenamine, with an emissive peak of 472 nm and the hole-transporting property speculated from different devices. It can function either as the single emissive layer or as the dye doped in N,N′-dicarbazolyl-4-4′-biphenyl (CBP). The former shows a maximum current efficiency and luminance of 7.06 cd/A (0.04 mA/cm²) and 16 930 cd/m², in contrast to 11.5 cd/A (4.35 mA/cm²) and 25 690 cd/m² for the latter. The better performance of the latter can be attributed to the bipolar carrier transport property of CBP and the hole-blocking and electron-transporting characteristic of 4,7-diphenyl-1,10-phenanthroline (BPhen), which resulting in a good balance of holes and electrons. Moreover, the Commission Internationale De L’Eclairage coordinates of the latter change slightly from (0.162, 0.3) to (0.148, 0.268) upon increasing the voltage from 3 V to 14 V.     

Organic light-emitting diodes on shape memory polymer substrates for wearable electronics

Green electrophosphorescent organic light-emitting diodes (OLEDs) with inverted top-emitting structures are demonstrated on bio-compatible shape memory polymer (SMP) substrates for wearable electronic applications. The combination of the unique properties of SMP substrates with the light-emitting properties of OLEDs pave to the way for new applications, including conformable smart skin devices, minimally invasive biomedical devices, and flexible lighting/display technologies. In this work, SMPs were designed to exhibit a considerable drop in modulus when a thermal stimulus is applied, allowing the devices to bend and conform to new shapes when its glass transition temperature is reached. These SMP substrates were synthesized using 1,3,5-triallyl-1,3,5-triazine-2,4,6(1H,3H,5H)-trione (TATATO), trimethylolpropane tris(3-mercaptopropionate) (TMTMP), and tricyclo[5.2.1.0^2,6]decanedimethanol diacrylate (TCMDA), and show a low glass transition temperature of 43 °C, as measured using dynamic mechanical analysis (DMA). The OLEDs fabricated on these substrates exhibit high performance with a maximum efficacy of 33 cd/A measured at a luminance of 1000 cd/m², and a peak luminance of over 30,000 cd/m².     

Small molecule interlayer for solution processed phosphorescent organic light emitting device

Using a 4,4′,4′′-tris(N-carbazolyl)-triphenylamine (TCTA) small molecule interlayer, we have fabricated efficient green phosphorescent organic light emitting devices by solution process. Significantly a low driving voltage of 3.0 V to reach a luminance of 1000 cd/m² is reported in this device. The maximum current and power efficiency values of 27.2 cd/A and 17.8 lm/W with TCTA interlayer (thickness 30 nm) and 33.7 cd/A and 19.6 lm/W with 40 nm thick interlayer are demonstrated, respectively. Results reveal a way to fabricate the phosphorescent organic light emitting device using TCTA small molecule interlayer by solution process, promising for efficient and simple manufacturing.     

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.     

Fluorene-based cathode interlayer polymers for high performance solution processed organic optoelectronic devices

A hydrophilic polyfluorene-based conjugated polyelectrolyte (CPE) Poly[9,9-bis(4′-(6″-(diethanolamino)hexyloxy) phenyl)fluorene], PPFN-OH (Scheme 1) has been synthesized and utilized as cathode interlayer for both polymer light emitting diodes (PLEDs) and solar cells (PSCs). For comparison, another CPE namely Poly[9,9-bis(6′-(diethanolamino)hexyl)fluorene] (PFN-OH) has also been investigated. They comprise the same polyfluorene backbone structures with, respectively, diethanolaminohexyl (PFN-OH) and diethanolaminohexoxyphenyl (PPFN-OH) substituents attached to the C9 carbon of the fluorene repeat unit. In comparison to reference devices with more reactive Ca/Al cathodes, utilizing these CPEs as interlayers allowed an Al cathode to be used for blue light emission PLEDs, yielding 51% and 92% enhancement of maximum luminous efficiency (LE) for PFN-OH and PPFN-OH, respectively. The PLEDs with PPFN-OH showed both higher maximum LE and maximum luminance (L) (LE = 2.53 cd/A at 6.2 V, L = 9917 cd/m² at 8.3 V) than devices with PFN-OH (2.00 cd/A at 4.1 V, 3237 cd/m² at 7.2 V). The PPFN-OH PLEDs also showed no significant roll-off in efficiency with increasing current density up to 400 mA/cm², indicating excellent electron injection ability and stability for this interlayer. The insertion of alkoxy-phenyl groups at the C9-position in PPFN-OH is clearly advantageous. This simple modification significantly improves the CPE cathode interlayer performance. Parallel investigations of the electron extraction properties of PPFN-OH in inverted architecture PSCs with PCDTBT:PC₇₀BM bulk heterojunction active layers demonstrated a power conversion efficiency enhancement of ∼19% (from 4.99% to 5.95%) for indium tin oxide cathode devices compared with reference devices using Ca/Al cathodes. These results confirm PPFN-OH to be a promising interlayer material for high performance solution processed organic optoelectronic devices.     

Synthesis and characterization of fluorene-based copolymers as electron-transporting materials for PLEDs

Owing to their low cost, easy processing, and the possibility of flexible fabrication, polymer light-emitting diodes (PLEDs) are emerging as an important class of materials. Despite promising characteristics, the relatively easy ionization of the well-known low-work-function cathodes such as Ca and Ba prevents the full usage of these materials. Herein, we report the syntheses of three alcohol-soluble conjugated polymers with different conjugation lengths and electron affinities as electron injection and transport materials for PLEDs: poly[9,9-bis(2-dihexylaminoethoxy)fluorene-co-tetrafluorobenzene] (PFOH-1), poly[9,9-bis(2-dihexylaminoethoxy)fluorene-co-thiophene] (PFOH-2), and poly[9,9-bis(2-dihexylaminoethoxy)fluorene-co-benzo-thiadiazole] (PFOH-3). For comparison, devices using Al, Ca, and Al cathodes were also fabricated. The device based on the Al cathode showed lower performance with a luminescence efficiency of 0.93 cd/A and a luminance of 248 cd/m²; that based on the low-work-function metal Ca as the cathode showed a near-threefold increase in luminescence efficiency at 2.51 cd/A and brightness at 856 cd/m² owing to greatly enhanced electron injection from the cathode; and the device employing the PFOH-3/Al cathode exhibited a luminescence efficiency of 2.35 cd/A and a brightness of 667 cd/m² at a current density of 35 mA/cm², which is comparable with the performance of the device with the Ca cathode.     

Efficient simplified orange and white phosphorescent organic light-emitting devices with reduced efficiency roll-off

Efficient orange phosphorescent organic light-emitting devices based on simplified structure with maximum efficiencies of 46.5 lm/W and 51.5 cd/A were reported. One device had extremely low efficiency roll-off with efficiencies of 50.6 cd/A, 45.0 cd/A and 39.2 cd/A at 1000 cd/m², 5000 cd/m² and 10,000 cd/m² respectively. The reduced efficiency roll-off was attributed to more balanced carrier injection and broader recombination zone. The designed simplified white device showed much lower efficiency roll-off than the control one based on multiple emitting layers. The efficiency of simplified white device was 40.8 cd/A at 1000 cd/m² with Commission Internationale de I’Eclairage coordinates of (0.39, 0.46).     

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.     

Improving the efficiency of light-emitting diode based on a thiophene polymer containing a cyano group

We report on the overall improvement of a single layer organic light-emitting diode device based on poly{[3-hethylthiophene]-co-3-[2-(p-cyano-phenoxy)ethyl]thiophene} or namely PTOPhCN. This polymer was recently developed by adding a cyano group as a side-chain substituent of the thiophenic backbone onto the main polymer chain and showed promising results for light-emitting diode devices. Using an improved device layout, bright red electroluminescence was obtained at 4 V and showed a luminance of about 400 cd/m² at 8 V with current densities in the order of 6000 A/m².     

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.     

Tandem white organic light-emitting device using non-modified Ag layer as cathode and interconnecting layer

Tandem white organic light-emitting device (WOLED) using non-modified Ag film as cathode and interconnecting layer is demonstrated. Effective electron injection is achieved when Ag is deposited on 4,7-diphenyl-1,10-phenanthroline electron transporting layer without any modified layer. Single OLED with Ag cathode shows comparable performance to that of device with Mg:Ag cathode. Such tandem WOLED exhibits low driving voltage, high power efficiency (15.1 lm/W at 1000 cd/m²) and low efficiency roll-off. The working mechanisms of single and tandem devices were discussed in detail. These results could provide a simple method to fabricate high performance tandem white OLED.     

New hole blocking material for green-emitting phosphorescent organic electroluminescent devices

The new amorphous molecular material, 2,5-bis(4-triphenylsilanyl-phenyl)-[1,3,4]oxadiazole, that functions as good hole blocker as well as electron transporting layer in the phosphorescent devices. The obtained material forms homogeneous and stable amorphous film. The new synthesized showed the reversible cathodic reduction for hole blocking material and the low reduction potential for electron transporting material in organic electroluminescent (EL) devices. The fabricated devices exhibited high performance with high current efficiency and power efficiency of 45 cd/A and 17.7 lm/W in 10 mA/cm², which is superior to the result of the device using BAlq (current efficiency: 31.5 cd/A and power efficiency: 13.5 lm/W in 10 mA/cm²) as well-known hole blocker. The ITO/DNTPD/α-NPD/6% Ir(ppy)₃ doped CBP/2,5-bis(4-triphenylsilanyl-phenyl)-[1,3,4]oxadiazole as both hole blocking and electron transporting layer/Al device showed efficiency of 45 cd/A and maximum brightness of 3000 cd/m² in 10 mA/cm².     

Highly efficient Organic Light-Emitting Diodes from thermally activated delayed fluorescence using a sulfone–carbazole host material

Organic Light-Emitting Diodes (OLEDs) using the thermally activated delayed fluorescence (TADF) emitter (4s,6s)-2,4,5,6-tetra(9H-carbazol-9-yl)isophthalonitrile (4CzIPN) are demonstrated using a novel ambipolar host 3,5-di(carbazol-9-yl)-1-phenylsulfonylbenzene (mCPSOB). When doped in a 5 wt.% concentration, OLEDs with EL efficiency values of more than 81 cd/A for current efficacy and 26.5% for external quantum efficiency are reported. These devices exhibit a low turn-on voltage of 3.2 V at 10 cd/m², as well as reduced efficiency roll-off at high current densities. To the best of our knowledge, these are among the highest ever reported efficiencies for TADF OLEDs, and are even comparable to the highest reported efficiencies for phosphorescent OLEDs.