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 10(6) 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.
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%.
An orange-red organic light-emitting diode containing a heptazine derivative exhibits high performance with a maximum external quantum efficiency of 17.5 ± 1.3% and a peak luminance of 17000 ± 1600 cd m⁻² without any light out-coupling enhancement. The high electroluminescence performance can be ascribed to the presence of an efficient up-conversion channel from the lowest triplet state to the lowest singlet state.
Make your OLED fluorescent: an aromatic molecule based on a spiro-acridine derivative was designed, and its photoluminescence and electroluminescence were characterized. By combining the donor and acceptor moieties a small energy gap between the lowest singlet and triplet states was achieved. This design leads to an organic light-emitting diode (OLED) that rivals phosphorescent devices regarding exciton generation efficiency.
The development of efficient metal-free organic emitters with thermally activated delayed fluorescence (TADF) properties for deep-blue emission is still challenging. A new family of deep-blue TADF emitters based on a donor-acceptor architecture has been developed. The electronic interaction between donor and acceptor plays a key role in the TADF mechanism. Deep-blue OLEDs fabricated with these TADF emitters achieved high external quantum efficiencies over 19.2 % with CIE coordinates of (0.148, 0.098).
We developed highly-efficient thermally activated delayed fluorescence (TADF) emitters containing 2,5-diphenyl-1,3,4-oxadiazole (OXD) or 3,4,5-triphenyl-4H-1,2,4-triazole (TAZ) electron acceptor and phenoxazine (PXZ) electron donor moieties. Oxadiazole-based compounds PXZ-OXD and 2PXZ-OXD showed green emission, while the triazole-based ones PXZ-TAZ and 2PXZ-TAZ exhibited sky-blue emission. In toluene solution, the donor-acceptor-donor-type molecules 2PXZ-OXD and 2PXZ-TAZ showed more efficient TADF and higher photoluminescence quantum yields (PLQYs) than the donoracceptor-type molecules PXZ-OXD and PXZ-TAZ. When doped into a host material, 2PXZ-OXD displayed a high PLQY of 87%. An organic light-emitting diode using 2PXZ-OXD as an emitter exhibited an external quantum efficiency (EQE) of 14.9%, which exceeds those obtained with conventional fluorescent emitters. This high EQE results from the efficient generation of TADF in 2PXZ-OXD.
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