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In purely organic room‐temperature phosphorescence (RTP) materials, fluorescence radiative transitions generally compete against inter‐system crossing (ISC) transitions to give fluorescence/phosphorescence dual emission. In order to achieve pure phosphorescence in RTP organic light‐emitting diodes (OLEDs), extended π‐conjugation is introduced into Se‐containing donors to suppress the fluorescence radiative transitions by the symmetry excited state orbitals in the introduced π–π* transitions that cancel the overlap of the orbitals, and two novel nonaromatic amine donor containing orange RTP emitters namely 2‐(benzo[c]phenoxaselenin‐10‐yl)‐4,6‐diphenyl‐1,3,5‐triazine (BPXSeDRZ) and 2‐(dibenzo[a,c]phenoxaselenin‐11‐yl)‐4,6‐diphenyl‐1,3,5‐triazine (DBPXSeDRZ) are developed, both of which exhibit efficient orange pure phosphorescence in doped films thanks to the sufficient ISC transitions. As a result, high external quantum efficiencies of 17.2% and 17.9% are respectively achieved for the orange RTP‐OLEDs based on BPXSeDRZ and DBPXSeDRZ for the first time, and they also exhibit stable pure electro‐phosphorescence spectra in a wide driving voltage. Moreover, by adopting DBPXSeDRZ as a sensitizer to harvest the triplet excitons and tetraphenyldibenzoperiflanthene as a conventional fluorescent emitter, the external quantum efficiency of the sensitized red fluorescent OLED can be elevated to 10.1%, which greatly expands the potential applications of the metal‐free phosphors in OLEDs. [ABSTRACT FROM AUTHOR]

Polycyclic aromatic hydrocarbon (PAH) compounds are prospective materials for highly efficient narrowband organic light‐emitting diodes. Specifically, boron‐nitrogen doped PAHs exhibit multiple resonance (MR) effect toward thermally activated delayed fluorescence (TADF) and narrow full width at half‐maximum (FWHM). Currently, the molecular design strategy for bathochromic‐shifted narrowband MR‐TADF emitters is a hotspot and challenging puzzle. Herein, a carbonyl is fused in the boron‐nitrogen doped PAH for constructing a boron/nitrogen/carbonyl MR‐TADF emitter. Benefiting from the carbonyl, the developed emitter exhibits enhanced intramolecular charge transfer and decreased reorganization energy, which displays bathochromic‐shifted narrowband emission pertinently. As a consequence, the proof‐of‐concept compound TCZBAO achieves an emission peak at 522 nm and narrow FWHM of 39 nm, while the carbonyl‐free TCZBAC exhibits an emission peak at 502 nm and FWHM of 46 nm. Maximum external quantum efficiencies of 36.1 % and 32.4 % are realized for the devices based on TCZBAO and TCZBAC, respectively, indicating the guiding significance of the proposed design strategy for developing bathochromic‐shifted narrowband MR‐TADF emitters. [ABSTRACT FROM AUTHOR]

Hyperfluorescent organic light‐emitting diodes (HF‐OLEDs) approach has made it possible to achieve excellent device performance and color purity with low roll‐off using noble‐metal‐free pure organic emitter. Despite significant progress, the performance of HF‐OLEDs is still unsatisfactory due to the existence of a competitive dexter energy transfer (DET) pathway. In this contribution, two boron dipyrromethene (BODIPY)‐based donor‐acceptor emitters (BDP‐C‐Cz and BDP‐N‐Cz) with hybridized local and charge transfer characteristics (HLCT) are introduced in the HF‐OLED to suppress the exciton loss by dexter mechanism, and a breakthrough performance with low‐efficiency roll‐off (0.3%) even at high brightness (1000 cd m−2) is achieved. It is demonstrated that the energy loss via the DET channel can be suppressed in HF‐OLEDs utilizing the HLCT emitter, as the excitons from the dark triplet state of such emitters are funneled to its emissive singlet state following the hot‐exciton mechanism. The developed HF‐OLED device has realized a good maximum external quantum efficiency (EQE) of 19.25% at brightness of 1000 cd m−2 and maximum luminance over 60 000 cd m−2, with an emission peak at 602 nm and Commission International de L'Eclairage (CIE) coordinates (0.57, 0.41), which is among the best‐achieved results in solution‐processed HF‐OLEDs. This work presents a viable methodology to suppress energy loss and achieve high performance in the HF‐OLEDs. [ABSTRACT FROM AUTHOR]

Multi‐resonance (MR) based organoboron emitters exhibiting high‐efficiency narrowband thermally activated delayed fluorescence (TADF) have become a critical material component for constructing high‐performance organic light‐emitting diodes (OLEDs) with high color purity and high color gamut. However, most of the MR‐TADF devices suffer from severe efficiency roll‐off at high current density due to the relatively large singlet–triplet splitting energy, long excited state lifetime, and slow reverse intersystem crossing rate (kRISC). Herein, by utilizing a sulfur atom‐fused donor unit, 7H‐benzo[4,5]thieno[2,3‐b]carbazole, an organic boron emitter (BTC‐BNCz) capable of high efficiency and low efficiency roll‐off narrowband TADF emission is developed. Benefitting from the heavy atom effect of the sulfur atom, kRISC up to 1.6 × 105 s−1 is achieved, which could greatly reduce the undesired quenching effect. Consequently, the OLED using BTC‐BNCz as dopant exhibits high external quantum efficiency (EQE) of 27.0% with full width at half maximum (FWHM) of 35 nm. Moreover, by utilizing a TADF material with a high horizontal dipole ratio as assistant host, outstanding device performance is achieved with a maximum EQE of 35.2% and FWHM of 37 nm, featuring slow efficiency roll‐off. [ABSTRACT FROM AUTHOR]

Doping‐free organic light‐emitting diodes (OLEDs) are beneficial to reduce manufacturing costs for mass production, which, however, are limited by the ubiquitous aggregation‐caused quenching (ACQ) effect, especially for thermally activated delayed fluorescence (TADF) emitters with relatively long exciton lifetimes. Herein, two typical TADF emitters pACRS and pACRSO with different sulfur atom valence states are developed, where pACRS with a thioether unit exhibits suppressed intermolecular interaction, alleviated ACQ effect, and higher efficiency in a conventional doping‐free device, in contract to pACRSO with a sulfone unit. It is of interest that comparable efficiencies are achieved for both emitters in doping‐free OLEDs with an ultrathin emission layer (UEML), in which the emitter molecules are deposited onto the surface of the underlying organic layer of host material to form an ultrathin quasi‐host‐guest system with alleviated ACQ effect. Besides, the suppressed trap effect is the key to guarantee the efficiency of UEML‐OLEDs, while different intermolecular interactions of emitters that determine the optimized UEML thickness will affect the efficiency roll‐off. Furthermore, benefiting from the UEML structure, highly efficient doping‐free OLEDs are also successfully achieved for red TADF emitters with stronger intermolecular interactions. Such an UEML strategy meeting efficiency and cost demands holds great promise for doping‐free OLEDs. [ABSTRACT FROM AUTHOR]

High‐quality hosts are indispensable for simultaneously realizing stable, high efficiency, and low roll‐off blue solution‐processed organic light‐emitting diodes (OLEDs). Herein, three solution processable bipolar hosts with successively reduced triplet energies approaching the T1 state of thermally activated delayed fluorescence (TADF) emitter are developed and evaluated for high‐performance blue OLED devices. The smaller T1 energy gap between host and guest allows the quenching of long‐lived triplet excitons to reduce exciton concentration inside the device, and thus suppresses singlet‐triplet and triplet‐triplet annihilations. Triplet‐energy‐mediated hosts with high enough T1 and better charge balance in device facilitate high exciton utilization efficiency and uniform triplet exciton distribution among host and TADF guest. Benefited from these synergetic factors, a high maximum external quantum efficiency (EQEmax) of 20.8%, long operational lifetime (T50 of 398.3 h @ 500 cd m−2), and negligible efficiency roll‐off (EQE of 20.1% @ 1000 cd m−2) are achieved for bluish‐green TADF OLEDs. Additionally introducing a narrowband emission multiple‐resonance TADF material as terminal emitter to accelerate exciton dynamic and improve exciton utilization, a higher EQEmax of 23.1%, suppressed roll‐off and extended lifetime of 456.3 h are achieved for the sky‐blue sensitized OLEDs at the same brightness. [ABSTRACT FROM AUTHOR]

Sulfone‐embedded heterocyclics are of great interest in organic light‐emitting diodes (OLEDs), however, exploring highly efficient narrowband emitters based on sulfone‐embedded heterocyclics remains challenging. Herein, five emitters with different sulfur valence state and molecular rigidity, namely tP, tCPD, 2tCPD, tPD and tPT, are thoroughly analysed. With restricted twisting of flexible peripheral phenyl by strengthening molecular rigidity, molecular emission spectra can be enormously narrowed. Further, introducing the sulfone group with bending vibration in low‐frequency region that suppresses high‐frequency vibration, sharp narrow full‐widths at half‐maximum of 28 and 25 nm are achieved for 2tCPD and tPD, respectively. Maximum external quantum efficiencies of 22.0 % and 27.1 % are successfully realized for 2tCPD‐ and tPD‐based OLED devices. These results offer a novel design strategy for constructing narrowband emitters by introducing sulfone group into a rigid molecular framework. [ABSTRACT FROM AUTHOR]

Generally, the charge transfer character of thermally activated delayed fluorescence (TADF) materials results in a long excitonic lifetime and broad‐band emission. With the combination of unity exciton utilization of TADF material and high radiative rate and narrow‐band emission of conventional fluorescence (CF) dopant, hyperfluorescence organic light‐emitting diodes (HF‐OLEDs) attract extensive attention in industry and academia recently. Till now, Dexter energy transfer (DET) from the triplet state of TADF assistant host to the dark triplet state of CF guest is the top‐drawer energy loss issue root in HF‐OLEDs. Herein, the energy loss of DET is blocked through one‐step substitution of TADF assistant host by electronically inert phenyl‐fluorene terminal for the first time. The blocking effect on DET process in HF‐OLEDs is investigated by means of photophysical characterization, theoretical calculation, device fabrication, and Monte Carlo simulation. The maximum external quantum efficiency of 18.1% with Commission Internationale de L'Eclairage coordinates of (0.61, 0.38) is achieved, which is on par with the state‐of‐the‐art efficiency for red HF‐OLEDs. This work presents a feasible design strategy for TADF assistant host aimed at achieving highly efficient HF‐OLEDs with narrow‐band emission. [ABSTRACT FROM AUTHOR]

• Hosts with TADF, conventional fluorescence and RTP characters are developed. • Exciton utilization efficiency is improved by the host with TADF character. • An EQE of 36.1% was achieved for sky blue OLED with DspiroAc-TRZ as emitter. • An EQE of 34.0% was achieved for the sensitized device with v -DABNA dopant. Spiral donor units have attracted extensive research focuses in designing highly emissive thermally activated delayed fluorescence (TADF) emitters. Herein, to reveal the significance of spiral donor units for constructing highly efficient host materials, several spiral donor-based host materials are developed. With the incorporation of spiral donor, increased intermolecular distance is achieved to reduce the concentration quenching effect of dopant. Moreover, the high triplet energy level of spiral donor can provide an additional energy transfer channel to further improve the device performance. Noteworthy, by connecting spiral donors or conventional carbazole unit with different electron-withdrawing units phenoxathiine 10,10-dioxide (PX) or phenoxathiine (PA), these hosts are given different photophysical properties of TADF, room-temperature phosphorescence (RTP) and conventional fluorescence (CF). The strong electron-withdrawing ability of PX is beneficial to the TADF character of spiral donor-based molecules, while the weak electron-withdrawing ability of PA is beneficial to the RTP property. Consequently, the blue OLEDs with DspiroAc-TRZ as a dopant emitter based on the hosts with TADF characters exhibit higher performance than those with RTP and CF properties, and excellent external quantum efficiency (EQE) of 36.1 % and current efficiency of 84.6 cd/A are achieved in a simple device structure. Furthermore, peak EQEs of 34.0 % and 33.0 % are achieved, when DspiroS-PX and DspiroS-PA hosted DspiroAc-TRZ are used to sensitize blue multi-resonance TADF emitter v -DABNA. Our work may shed new light on designing highly efficient host materials for TADF emitters. [ABSTRACT FROM AUTHOR]

Organic light‐emitting diodes (OLEDs) employing exciplex cohosts have gained attractive interest due to the promising high efficiency, low driving voltage, and potential low cost in future solid‐state lighting sources and full‐color displays. However, their device lifetime is still the most challenging weakness and rarely studied, which is regarded as a time consuming and complicated work. Therefore, a simplified but effective and comprehensive approach is demonstrated to give prediction for the exciplex cohosts operating lifespan and analyze their possible degradation mechanisms by considering molecular dissociated activation energy with internal exciton dynamics correlations. As a consequence, strong chemical bond stability for the hole transport moieties and rapid reactive exciton relaxation have the intrinsic talent to access potentially long‐lived exciplex cohosts, achieving an extended lifetime of 10169 h for the predicted long‐lived exciplex cohost OLEDs. Degradation behaviors further confirm that the deteriorated source is attributed to the formation of exciton quenchers and hole traps from excited states and charged‐excited states, respectively. The current findings establish a universal technique to screen the stable exciplex cohost candidates with economic time consumption and expenses. By proposing a lifetime prediction method via coordinating dissociated activation energy description with exciton density as a function of time, exciplex cohost molecular stability and dominated dissociation mechanism are successfully predicted. The strong chemical bond for the hole transport moieties and rapid reactive exciton relaxation provide the managing strategies to access long‐lived exciplex cohosts. [ABSTRACT FROM AUTHOR]

[Display omitted] • Multiple CT channels and 3LE states contribute to the speedy k r and RISC processes. • High Θ and small FWHM are realized due to the rigid disk-like structure. • η r and η out above 30% are achieved owing to triplet exciton utilization and high Θ. • EQE above 10% was realized for the standard blue device based on BO3N. The efficiency of pure blue Organic light-emitting diodes (OLEDs) still needs to be improved, which is limited by the utilization of the forbidden transition triplet excitons and low light-out-coupling efficiency in devices. Herein, two blue emitters were developed through combining multiple diphenylamine (DPA) donors with an oxygen-bridged boron (DBA) or triphenyl triazine (TRZ) acceptor. Notably, a narrow-band deep blue emission with a peak of 423 nm and a Full-width at half-maximum (FWHM) of 34 nm is realized for the boron-based emitter in toluene solution. Thanks to their multiple Charge transfer (CT) channels and high orientated disk-like structure, high radiative transition rates (k r > 108 s−1) and high horizontal emitting dipole ratios (Θ > 80%) can be realized simultaneously. Meanwhile, the introduction of the peripheral DPA units can also provide multiple localized triplet (3LE) states for spin up-conversion of forbidden transition triplet excitons. Owing to the effective up-conversion of triplet excitons and high light-out-coupling efficiency, maximum external quantum efficiency of more than 10% is achieved for the boron emitter-based pure blue OLEDs with a Commission Internationale de l'Eclairage (CIE) coordinates of (0.14, 0.08). [ABSTRACT FROM AUTHOR]

Organic light-emitting diodes (OLEDs) employing purely organic functional materials indicate a low-cost manufacturing route towards the next-generation display and solid-state lighting owing to the avoidance of noble heavy metal complex phosphorescent emitters. In recent years, several mechanisms have been proposed to design high performance purely organic emitters. This new generation of purely organic emitters shed light on the realization of both low-cost and high performances. The main idea of this paper is to review how to use purely organic semiconductors to realize high-efficiency OLEDs. This guides us to pay special attention to two aspects: 1) how to break the efficiency bottleneck resulting from exciton spin-statistics, which is critical to determine internal quantum efficiency; 2) how to enhance out-coupling efficiency by molecular designs, which eventually influences on external quantum efficiency. Several significant material design strategies are thus introduced, and the relevant mechanisms are classified as triplet-triplet annihilation, thermally activated delayed fluorescence, hot excitons, room temperature phosphorescence, and luminescent radicals. Then, device strategies by employing organic heterojunctions as the main luminescent center towards high-performance fluorescent OLEDs were introduced. Finally, we outline the progress of enhancing out-coupling efficiency by tuning the dipole orientation of emitters and the operational stability of OLEDs excluding noble heavy metal complex phosphorescent emitters. [ABSTRACT FROM AUTHOR]