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To utilize thermally activated delayed fluorescence (TADF) technology for future displays, it is necessary to develop host materials which harness the full potential of blue TADF emitters. However, no publication has reported such hosts yet. Although the most popular host for blue TADF, bis[2‐(diphenylphosphino)phenyl]ether oxide (DPEPO) guarantees high‐maximum external quantum efficiency (EQEmax) TADF devices, they exhibit very short operational lifetimes. In contrast, long‐lifespan blue TADF devices employing stable hosts such as 3′,5‐di(9H‐carbazol‐9‐yl)‐[1,1′‐biphenyl]‐3‐carbonitrile (mCBP‐CN) exhibit much lower EQEmax than the DPEPO‐employed devices. Here, an elaborative approach for designing host molecules is suggested to achieve simultaneously stable and efficient blue TADF devices. The approach is based on engineering the molecular geometry, ground‐ and excited‐state dipole moments of host molecules. The engineered hosts significantly enhance delayed fluorescence quantum yields of TADF emitters, as stabilizing the charge‐transfer excited states of the TADF emitters and suppressing exciton quenching, and improve the charge balance. Moreover, they exhibit both photochemical and electrochemical stabilities. The best device employing one of the engineered hosts exhibits 79% increase in EQEmax compared to the mCBP‐CN‐employed device, together with 140% and 92‐fold increases in operational lifetime compared to the respective mCBP‐CN‐ and the DPEPO‐based devices. [ABSTRACT FROM AUTHOR]

Much effort has been dedicated to increase the operational lifetime of blue phosphorescent materials in organic light‐emitting diodes (OLEDs), but the reported device lifetimes are still too short for the industrial applications. An attractive method for increasing the lifetime of a given emitter without making any chemical change is exploiting the kinetic isotope effect, where key CH bonds are deuterated. A computer model identifies that the most vulnerable molecular site in an Ir‐phenylimidazole dopant is the benzylic CH bond and predicts that deuteration may hamper the deactivation pathway involving CH/D bond cleavage notably. Experiments show that the device lifetime until the initial luminance diminishes to 70% (LT70) of a prototype phosphorescent OLED device can be doubled to 355 hours with a maximum external quantum efficiency of 25.1% at 1000 cd m−2. This is one of the best operational performances of blue phosphorescent OLEDs observed to date in a single stacked cell. [ABSTRACT FROM AUTHOR]

Novel homoleptic cyclometalated Ir(III) complexes are designed to improve their emission dipole orientations in the emitting layer of blue phosphorescent organic light emitting devices. Biphenyl group is introduced into the imidazole of cyclometalated Ir(III) complexes to simultaneously achieve enhanced efficiency and operation lifetime, resulting in one of the best device performances of single‐stacked organic light emitting diodes with 91% emission dipole orientation, 26.3% maximum external quantum efficiency (maximally calculated as 41%), and 169 h lifetime at 1000 cd m−2 (LT80), color coordinate (0.17, 0.30). To elucidate the physical origin of this significant improvements, the orientational and positional distributions of the homoleptic dopants are analyzed with consideration on intermolecular interactions through atomistic modeling of the emitting layer. With the findings, the phosphorescent dopants could be designed in the future to achieve enhanced performance. [ABSTRACT FROM AUTHOR]

The short material lifetime of thermally activated delayed fluorescence (TADF) technology is a major obstacle to the development of economically feasible, highly efficient, and durable devices for commercial applications. TADF devices are also hampered by insufficient operational stability. In this paper, we report the design, synthesis, and evaluation of new TADF molecules possessing a sterically twisted skeleton by interlocking donor and acceptor moieties through a C–C bond. Compared to C–N-bond TADF molecules, such as CPT2, the C–C-bond TADF molecules showed a large dihedral angle increase by more than 30 times and a singlet–triplet energy-gap decrease to less than 0.22 eV because of the steric hindrance caused by the direct C–C bond connection. With the introduction of a dibenzofuran core structure, devices comprising BMK-T317 and BMK-T318 exhibited a magnificent display performance, especially their external quantum efficiencies, which were as high as 19.9% and 18.8%, respectively. Moreover, the efficiency roll-off of BMK-T318 improved significantly (26.7%). These results indicate that stability of the material can be expected through the reduction of their singlet–triplet splitting and the precise adjustment of dihedral angles between the donor–acceptor skeletons. [ABSTRACT FROM AUTHOR]

Advances in electroluminescence demand the development of emissive molecules capable of utilizing all of the electrogenerated excitons. Here, a molecular strategy to harvest the excitons without relying on late transition metals or thermal activation is designed and evaluated. The key process deployed is an exergonic, El‐Sayed rule‐allowed reverse intersystem crossing (ES‐rISC) from the triplet n–π * transition state to the singlet π–π * transition state, followed by fluorescent decay of the latter. To demonstrate the strategy, a series of fluorescent molecules consisting of a 9,10‐diphenylanthracene core and different carbonyl n–π * units (SY compounds) is created. The compounds display a strong blue fluorescence emission with high photoluminescence quantum yields of up to 0.93. Multilayer organic electroluminescence devices containing the SY compounds exhibit maximum external quantum efficiencies greater than that obtained from a singlet‐exciton‐only control device. This improvement is due to their capacity to utilize triplet excitons for fluorescence emission. The studies demonstrate that exergonic ES‐rISC can serve as a promising pathway for creating inexpensive and tractable organic dopants for high‐efficiency electroluminescence. [ABSTRACT FROM AUTHOR]

We report blue thermally activated delayed fluorescent (TADF)organic light emitting diodes(OLEDs) with high efficiencies which areattributed toemployingdonor-acceptor type TADF compounds having highreverse intersystem crossing (RISC)rates. Carbazole derivatives and a triphenyltriazine (or a dibenzothiophene) are employed as the donor (D) and the acceptor (A)moieties, respectively. We can achieve four D-A type blue TADF compounds through the combination of the moieties and adjust the energy gap between the lowest excited singlet and triplet statesand accordingly the RISC rate (k RISC) for the compounds. A blue OLED using one of the TADF molecules,9-(9H-carbazol-9-yl)-12-(4-(4,6-diphenyl-1,3,5-triazin-2-yl)phenyl)-5-phenyl-5,12-dihydroindolo[3,2- a ]carbazole exhibitshigh maximum external quantum efficiency (22.3%)due to itsshort excitonlifetime (6.1 μs) induced by its high k RISC (1.825 × 106s−1). Image 1 • A simple combinatorial study of D-A compounds is performed which is effective in making a profound impact on their RISC rates. • A compound having the highest RISC rate exhibits the shortest exciton lifetime and the best OLED performance. • The D-A combination impacts on the charge transfer properties and accordingly govern their OLED driving voltages. [ABSTRACT FROM AUTHOR]