Chihaya Adachi

Nearly 100% internal phosphorescence efficiency in an organic light-emitting device

We demonstrate very high efficiency electrophosphorescence in organic light-emitting devices employing a phosphorescent molecule doped into a wide energy gap host. Using bis(2-phenylpyridine)iridium(III) acetylacetonate [(ppy)2Ir(acac)] doped into 3-phenyl-4(1′-naphthyl)-5-phenyl-1,2,4-triazole, a maximum external quantum efficiency of (19.0±1.0)% and luminous power efficiency of (60±5) lm/W are achieved. The calculated internal quantum efficiency of (87±7)% is supported by the observed absence of thermally activated nonradiative loss in the photoluminescent efficiency of (ppy)2Ir(acac). Thus, very high external quantum efficiencies are due to the nearly 100% internal phosphorescence efficiency of (ppy)2Ir(acac) coupled with balanced hole and electron injection, and triplet exciton confinement within the light-emitting layer.

Highly efficient organic light-emitting diodes from delayed fluorescence

The inherent flexibility afforded by molecular design has accelerated the development of a wide variety of organic semiconductors over the past two decades. In particular, great advances have been made in the development of materials for organic light-emitting diodes (OLEDs), from early devices based on fluorescent molecules to those using phosphorescent molecules. In OLEDs, electrically injected charge carriers recombine to form singlet and triplet excitons in a 1:3 ratio; the use of phosphorescent metal–organic complexes exploits the normally non-radiative triplet excitons and so enhances the overall electroluminescence efficiency. Here we report a class of metal-free organic electroluminescent molecules in which the energy gap between the singlet and triplet excited states is minimized by design, thereby promoting highly efficient spin up-conversion from non-radiative triplet states to radiative singlet states while maintaining high radiative decay rates, of more than 106 decays per second. In other words, these molecules harness both singlet and triplet excitons for light emission through fluorescence decay channels, leading to an intrinsic fluorescence efficiency in excess of 90 per cent and a very high external electroluminescence efficiency, of more than 19 per cent, which is comparable to that achieved in high-efficiency phosphorescence-based OLEDs.

High-efficiency organic electrophosphorescent devices with tris(2-phenylpyridine)iridium doped into electron-transporting materials

We demonstrate high-efficiency organic light-emitting devices employing the green electrophosphorescent molecule, fac tris(2-phenylpyridine)iridium [Ir(ppy)3], doped into various electron-transport layer (ETL) hosts. Using 3-phenyl-4-(1′-naphthyl)-5-phenyl-1,2,4-triazole as the host, a maximum external quantum efficiency (ηext) of 15.4±0.2% and a luminous power efficiency of 40±2 Im/W are achieved. We show that very high internal quantum efficiencies (approaching 100%) are achieved for organic phosphors with low photoluminescence efficiencies due to fundamental differences in the relationship between electroluminescence from triplet and singlet excitons. Based on the performance characteristics of single and double heterostructures, we conclude that exciton formation in Ir(ppy)3 occurs within close proximity to the hole-transport layer/ETL:Ir(ppy)3 interface.

Endothermic energy transfer: A mechanism for generating very efficient high-energy phosphorescent emission in organic materials

Intermolecular energy transfer processes typically involve an exothermic transfer of energy from a donor site to a molecule with a substantially lower-energy excited state (trap). Here, we demonstrate that an endothermic energy transfer from a molecular organic host (donor) to an organometallic phosphor (trap) can lead to highly efficient blue electroluminescence. This demonstration of endothermic transfer employs iridium(III)bis(4,6-di-fluorophenyl)-pyridinato-N,C2′)picolinate as the phosphor. Due to the comparable energy of the phosphor triplet state relative to that of the 4,4′-N,N′-dicarbazole-biphenyl conductive host molecule into which it is doped, the rapid exothermic transfer of energy from phosphor to host, and subsequent slow endothermic transfer from host back to phosphor, is clearly observed. Using this unique triplet energy transfer process, we force emission from the higher-energy, blue triplet state of the phosphor (peak wavelength of 470 nm), obtaining a very high maximum organic light-emi...

Design of efficient thermally activated delayed fluorescence materials for pure blue organic light emitting diodes

Efficient thermally activated delayed fluorescence (TADF) has been characterized for a carbazole/sulfone derivative in both solutions and doped films. A pure blue organic light emitting diode (OLED) based on this compound demonstrates a very high external quantum efficiency (EQE) of nearly 10% at low current density. Because TADF only occurs in a bipolar system where donor and acceptor centered (3)ππ* states are close to or higher than the triplet intramolecular charge transfer ((3)CT) state, control of the π-conjugation length of both donor and acceptor is considered to be as important as breaking the π-conjugation between them in blue TADF material design.

High-efficiency red electrophosphorescence devices

We demonstrate high-efficiency red electrophosphorescent organic light-emitting devices employing bis(2-(2′-benzo[4,5-a]thienyl)pyridinato-N,C3′) iridium(acetylacetonate) [Btp2Ir(acac)] as a red phosphor. A maximum external quantum efficiency of ηext=(7.0±0.5)% and power efficiency of ηp=(4.6±0.5) lm/W are achieved at a current density of J=0.01 mA/cm2. At a higher current density of J=100 mA/cm2, ηext=(2.5±0.3)% and ηp=(0.56±0.05) lm/W are obtained. The electroluminescent spectrum has a maximum at a wavelength of λmax=616 nm with additional intensity peaks at λsub=670 and 745 nm. The Commission Internationale de L’Eclairage coordinates of (x=0.68, y=0.32) are close to meeting video display standards. The short phosphorescence lifetime (∼4 μs) of Btp2Ir(acac) leads to a significant improvement in ηext at high currents as compared to the previously reported red phosphor, 2,3,7,8,12,13,17,18-octaethyl-12H, 23H-prophine platinum (II) PtOEP with a lifetime of ∼50 μs.

Blue light-emitting organic electroluminescent devices

Organic electroluminescent (EL) devices with multilayered thin‐film structures which emitted bright blue light were constructed. Two empirical guides for the selection of blue‐emitting materials were established. The keys to obtain the EL cells with high EL efficiency were excellent film‐forming capability of an emitter layer and the appropriate combinations of emitter and carrier transport materials for avoiding the formation of exciplexes. In one of our organic electroluminescent devices, blue emission with a luminance of 700 cd/m2 was achieved at a current density of 100 mA/cm2 and a dc drive voltage of 10 V.

Organic electroluminescent device having a hole conductor as an emitting layer

We have succeeded in fabricating a novel thin‐film electroluminescent device with a luminescent hole transport layer as an emitter. The cell structure is composed of an indium‐tin‐oxide substrate, a luminescent hole transport layer (emitter), an electron transport layer, and a MgAg electrode. The most essential feature of our device owes for adoption of an oxadiazole derivative as an electron transport layer. The emission intensity of 1000 cd/m2 was achieved at a current of 100 mA/cm2.

100% phosphorescence quantum efficiency of Ir(III) complexes in organic semiconductor films

We demonstrate that three Ir(III) complexes used as principal dopants in organic electrophosphorescent diodes have very high photoluminescence quantum efficiency (ηPL) in a solid-state film. The green emitting complex, fac-tris(2-phenylpyridinato)iridium(III) [Ir(ppy)3], the red-emitting bis[2-(2′-benzothienyl)pyridinato-N,C3′] (acetylacetonato)iridium(III) [Btp2Ir(acac)], and the blue complex bis[(4,6-difluorophenyl)pyridinato-N,C2](picolinato)iridium(III) (FIrpic) were prepared as codeposited films of varying concentration with 4,4′-bis(N-carbazolyl)-2,2′-biphenyl, a commonly used host material. The maximum ηPL values for Ir(ppy)3, Btp2Ir(acac), and FIrpic were, respectively, 97%±2% (at 1.5mol%), 51%±1% (at 1.4mol%), and 78%±1% (at 15mol%). Furthermore, we also observed that the maximum ηPL of FIrpic reached 99%±1% when doped into the high triplet energy host, m-bis(N-carbazolyl)benzene, at an optimal concentration of 1.2mol%.

Highly efficient blue electroluminescence based on thermally activated delayed fluorescence

Organic compounds that exhibit highly efficient, stable blue emission are required to realize inexpensive organic light-emitting diodes for future displays and lighting applications. Here, we define the design rules for increasing the electroluminescence efficiency of blue-emitting organic molecules that exhibit thermally activated delayed fluorescence. We show that a large delocalization of the highest occupied molecular orbital and lowest unoccupied molecular orbital in these charge-transfer compounds enhances the rate of radiative decay considerably by inducing a large oscillator strength even when there is a small overlap between the two wavefunctions. A compound based on our design principles exhibited a high rate of fluorescence decay and efficient up-conversion of triplet excitons into singlet excited states, leading to both photoluminescence and internal electroluminescence quantum yields of nearly 100%.