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Deep‐blue multi‐resonance (MR) emitters with stable and narrow full‐width‐at‐half‐maximum (FWHM) are of great importance for widening the color gamut of organic light‐emitting diodes (OLEDs). However, most planar MR emitters are vulnerable to intermolecular interactions from both the host and guest, causing spectral broadening and exciton quenching in thin films. Their emission in the solid state is environmentally sensitive, and the color purity is often inferior to that in solutions. Herein, a molecular design strategy is presented that simultaneously narrows the FWHM and suppresses intermolecular interactions by combining intramolecular locking and peripheral shielding within a carbonyl/nitrogen‐based MR core. Intramolecularly locking carbonyl/nitrogen‐based bears narrower emission of 2,10‐dimethyl‐12,12‐diphenyl‐4H‐benzo[9,1]quinolizino[3,4,5,6,7‐defg]acridine‐4,8(12H)‐dione in solution and further with peripheral‐shielding groups, deep‐blue emitter (12,12‐diphenyl‐2,10‐bis(9‐phenyl‐9H‐fluoren‐9‐yl)−4H‐benzo[9,1]quinolizino[3,4,5,6,7‐defg]acridine‐4,8(12H)‐dione, DPQAO‐F) exhibits ultra‐pure emission with narrow FWHM (c.a., 24 nm) with minimal variations (∆FWHM ≤ 3 nm) from solution to thin films over a wide doping range. An OLED based on DPQAO‐F presents a maximum external quantum efficiency (EQEmax) of 19.9% and color index of (0.134, 0.118). Furthermore, the hyper‐device of DPQAO‐F exhibits a record‐high EQEmax of 32.7% in the deep‐blue region, representing the first example of carbonyl/nitrogen‐based OLED that can concurrently achieve narrow bandwidth in the deep‐blue region and a high electroluminescent efficiency surpassing 30%. [ABSTRACT FROM AUTHOR]

A simple strategy to simultaneously achieve fast reverse intersystem crossing (RISC) and low non‐radiative decay rates in thermally activated delayed fluorescence (TADF) emitters is still lacking. Here, the green TADF emitters containing aromatic ketones and prepared D‐Ph and D‐PhCz containing different amounts of deuterium are deuterated to study the mechanism of deuterium on the performance improvement of TADF devices. Due to the heavy atom effect of deuterium, the non‐radiative transition rate constant (knr) of D‐Ph and D‐PhCz decreases. Most importantly, deuterium reduces the reorganization energy (λ) of (T1‐S1), which greatly improves the reverse intersystem crossing rate constant (kRISC) and the exciton utilization efficiency. The results show that the external quantum efficiency of D‐Ph and D‐PhCz increases to 25.69% and 24.92%, respectively. This study provides a simple and efficient strategy for reducing non‐radiative energy loss and increasing kRISC to achieve high‐performance TADF emitters. [ABSTRACT FROM AUTHOR]

Rationally tuning the emission position and narrowing the full width at half‐maximum (FWHM) of an emitter is of great importance for many applications. By synergistically improving rigidity, strengthening the resonant strength, inhibiting molecular bending and rocking, and destabilizing the HOMO energy level, a deep‐blue emitter (CZ2CO) with a peak wavelength of 440 nm and an ultranarrow spectral FWHM of 16 nm (0.10 eV) was developed via intramolecular cyclization in a carbonyl/N resonant core (QAO). The dominant υ0‐0 transition character of CZ2CO gives a Commission Internationale de I'Éclairage coordinates (CIE) of (0.144, 0.042), nicely complying with the BT.2020 standard. Moreover, a hyper‐fluorescent device based on CZ2CO shows a high maximum external quantum efficiency (EQEmax) of 25.6 % and maintains an EQE of 22.4 % at a practical brightness of 1000 cd m−2. [ABSTRACT FROM AUTHOR]

High‐performance nondoped organic light‐emitting diodes (OLEDs) are promising technologies for future commercial applications. Herein, we synthesized two new thermally activated delayed fluorescence (TADF) emitters that enable us, for the first time, to combine three effective approaches for enhancing the efficiency of nondoped OLEDs. First, the two emitters are designed to have high steric hindrances such that their emitting cores will be suitably isolated from those of their neighbors to minimize concentration quenching. On the other hand, each of the two emitters has two stable conformations in solid films. In their neat films, molecules with the minority conformation behave effectively as dopants in the matrix composing of the majority conformation. One hundred percent exciton harvesting is thus theoretically feasible in this unique architecture of "self‐doped" neat films. Furthermore, both emitters have relatively high aspect ratios in terms of their molecular shapes. This leads to films with preferred molecular orientations enabling high populations of horizontal dipoles beneficial for optical out‐coupling. With these three factors, OLEDs with nondoped emitting layers of the respective emitters both achieve nearly 100% exciton utilization and deliver over 30% external quantum efficiencies and ultralow efficiency roll‐off at high brightness, which have not been observed in reported nondoped OLEDs. [ABSTRACT FROM AUTHOR]

Multiple resonance (MR) type thermally activated delayed fluorescence (TADF) material is currently a research hotspot in organic light‐emitting diodes (OLEDs) due to their high color purity and high exciton utilization. However, there are only a handful of MR‐TADF emitters with emissions beyond the blue‐to‐green region. The very limited emission colors for MR‐TADF emitters are mainly caused by the fact that so far molecular modifications of MR‐TADF do not offer much change in the emission colors. Here, we report a new approach to modifying a prototypical MR core of DABNA by fusing carbazoles to the MR framework. The carbazole‐fused molecule (TCZ‐F‐DABNA) basically maintains the MR‐dominated features of DABNA while red‐shifting the emission. Its OLED achieves an external quantum efficiency of 39.2 % with a peak at 588 nm, which is a record‐high efficiency for OLEDs with peaks beyond 560 nm. This work provides a new approach for significantly tunning emission colors of MR‐TADF emitters. [ABSTRACT FROM AUTHOR]

Non‐doped organic light‐emitting diodes (OLEDs) are particularly appealing due to the merit of the extremely simple device structure. However, the performance of non‐doped OLEDs is usually far inferior than that of doped devices, mainly due to the lack of desirable emitters. An ideal emitter for non‐doped OLEDs should not merely be highly emissive in the host matrix but also be capable of delivering excellent properties in its condensed state. Herein, through molecular engineering, an "axial and equatorial carbazolyl extension" approach to manipulate the molecular packing behavior is developed, and thus, the emitter is awarded with superior properties in its neat film. Based on this approach, through simply modifying the conventional acridine donor in a thermally activated delayed fluorescence (TADF) emitter with carbazole moieties in the way of hyper‐conjugation, two new TADF emitters with the molecular skeleton being extended both horizontally and vertically by carbazole moieties are constructed. The resulted TADF emitters reveal superb properties with simultaneous excellent thermal and morphological stabilities, photophysical behaviors, and charge transporting ability in their neat film. Owing to the merits of these synergistic superior properties, highly efficient non‐doped green emissive OLED with the state‐of‐the‐art external quantum efficiency of nearly 30% is realized. [ABSTRACT FROM AUTHOR]

The conformational distribution and mutual interconversion of thermally activated delayed fluorescence (TADF) emitters significantly affect the exciton utilization. However, their influence on the photophysics in amorphous film states is still not known due to the lack of a suitable quantitative analysis method. Herein, we used temperature‐dependent time‐resolved photoluminescence spectroscopy to quantitatively measure the relative populations of the conformations of a TADF emitter for the first time. We further propose a new concept of "self‐doping" for realizing high‐efficiency nondoped OLEDs. Interestingly, this "compositionally" pure film actually behaves as a film with a dopant (quasi‐equatorial form) in a matrix (quasi‐axial form). The concentration‐induced quenching that may occur at high concentrations is thus expected to be effectively relieved. The "self‐doping" OLED prepared with the newly developed TADF emitter TP2P‐PXZ as a neat emitting layer realizes a high maximum external quantum efficiency of 25.4 % and neglectable efficiency roll‐off. [ABSTRACT FROM AUTHOR]

Nondoped organic light‐emitting diodes (OLEDs) have drawn enormous attention for their merits of process simplicity, reduced fabrication cost, and phase stability. Herein, a novel approach of utilizing intermolecular hydrogen bonding for enhancing performance of nondoped OLEDs with a new thermally activated delayed fluorescence (TADF) emitter 10‐(4‐(2,6‐di(pyrimidin‐5‐yl)pyridin‐4‐yl)phenyl)‐10H‐phenoxazine (DPmP‐PXZ) is investigated. Endowing with suitable intermolecular hydrogen bonds linking the ends of neighboring DPmP‐PXZ molecules, the molecules tend to form extended 1D molecular chain in solid. This 1D structure effectively keeps the electron‐rich PXZ cores in neighboring molecules apart from each other such that triplet‐related exciton quenching can be well suppressed. In addition, it also improves the balance of carrier mobilities and the optical out‐coupling from the emitting layer. With these merits, OLEDs using DPmP‐PXZ as a dopant emitter, from 10 to 100 wt%, can maintain high external quantum efficiencies (EQEs) of over 20%. More importantly, its nondoped OLED shows a yellow emission and an excellent maximum EQE of 21.8% with little efficiency roll‐off which is even comparable with state‐of‐the‐art yellow OLEDs. These results provide new insight on the role of hydrogen bonding in molecular packing and its subsequent influences on the performance of OLEDs. [ABSTRACT FROM AUTHOR]

Organic light‐emitting diodes (OLEDs) with simple nondoped device structure are extremely attractive for real applications since excitons can be utilized without considering the possible charge trapping and morphology issues in the host–dopant systems. Emitters with suppressed concentration annihilation capability are essential for nondoped devices. Herein, two thermally activated delayed fluorescence (TADF) emitters based on a novel 3D electron donor, namely, TDMAC, are constructed. The TDMAC donor consists of a conventional donor with fused triptycene scaffold. Benefitting from the unique rigid and bulky triptycene moiety, these TADF emitters exhibit excellent thermal, morphological, and photophysical properties. Consequently, highly efficient OLEDs with external quantum efficiencies up to 24.2% and 23% are realized for doped and nondoped devices, respectively. [ABSTRACT FROM AUTHOR]

While monochrome organic light‐emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) emitters have achieved over 30% external quantum efficiencies (EQEs), all‐TADF white OLEDs (WOLEDs) are still lagging behind. Herein, a simple system based on two color‐complementary TADF emitters is exploited to realize high‐performance WOLEDs. By doping a high‐performance orange–red TADF fluorophor (BPPZ‐DPXZ) into a blue TADF host (DBFCz‐Trz), energy transfer, and triplet‐to‐singlet conversion in the host‐dopant system can be optimized to simultaneously achieve full exciton utilization and color balance. With this design, all‐TADF single‐emitting‐layer WOLEDs with a maximum EQE up to 32.8% are demonstrated. This high efficiency surpasses EQEs of reported WOLEDs based on both TADF as well as phosphorescence. It is expected that this finding can provide new insight for designing highly efficient all‐TADF WOLEDs. [ABSTRACT FROM AUTHOR]

Developing red thermally activated delayed fluorescence (TADF) emitters for high‐performance OLEDs is still facing great challenge. Herein, three red TADF emitters, pDBBPZ‐DPXZ, pDTBPZ‐DPXZ, and oDTBPZ‐DPXZ, are designed and synthesized with same donor–acceptor (D‐A) backbone with different peripheral groups attaching on the A moieties. Their lowest triplet states change from locally excited to charge transfer character leading to significantly enhance reverse intersystem crossing process. In particular, oDTBPZ‐DPXZ exhibits efficient TADF feature and exciton utilization. It not only achieves an external quantum efficiency (EQE) of 20.1 % in red vacuum‐processed OLED, but also realize a high EQE of 18.5 % in a solution‐processed OLED, which is among the best results in solution‐processed red TADF OLEDs. This work provides an effective strategy for designing red TADF molecules by managing energy level alignments to facilitate the up‐conversion process and thus enhance exciton harvesting. [ABSTRACT FROM AUTHOR]

Near‐infrared organic light‐emitting diodes (NIR OLEDs) enable many unique applications ranging from night‐vision displays and photodynamic therapies. However, the development of efficient NIR OLEDs with a low efficiency roll‐off is still challenging. Here, a series of new heteroleptic Pt(II) complexes (1–4) flanked by both pyridyl pyrimidinate and functional azolate chelates are synthesized. The reduced ππ* energy gap of the pyridyl pyrimidinate chelate, and strong intermolecular interaction and high crystallinity in vacuum‐deposited thin films engender strong intermolecular charge transfer transition including metal–metal‐to‐ligand charge transfer; thereby, exhibiting efficient photoluminescence within 776–832 nm and short radiative lifetimes of 0.52–0.79 µs. Consequently, nondoped NIR‐emitting OLEDs based on these Pt(II) complexes are fabricated, to which Pt(II) complexes 2 and 4 give record high maximum external quantum efficiency of 10.61% at 794 nm and 9.58% at 803 nm, respectively. Moreover, low efficiency roll‐off is also observed, among which the device efficiencies of 2 and 4 are at least four times higher than that of the best NIR‐emitting OLEDs recorded at current density of 100 mA cm−2. [ABSTRACT FROM AUTHOR]

Thermally activated delayed fluorescence (TADF) provides great potential for the realization of efficient and stable organic light‐emitting diodes (OLEDs). However, it is still challenging for blue TADF emitters to simultaneously achieve high efficiency, high brightness, and low Commission Internationale de l'Eclairage (CIE) y coordinate (CIEy) value. Here, the design and synthesis of two new benzonitrile‐based TADF emitters (namely 2,6‐di(9H‐carbazol‐9‐yl)‐3,5‐bis(3,6‐diphenyl‐9H‐carbazol‐9‐yl)benzonitrile (2PhCz2CzBn) and 2,6‐di(9H‐carbazol‐9‐yl)‐3,5‐bis(3,6‐di‐tert‐butyl‐9H‐carbazol‐9‐yl)benzonitrile (2tCz2CzBn)) with a symmetrical and rigid heterodonor configuration are reported. The TADF OLEDs doped with both the emitters can achieve a high external quantum efficiency (EQE) over 20% and narrowband blue emission of 464 nm with a CIEy < 0.2. Moreover, the incorporation of a terminal tert‐butyl group can weaken the intermolecular π–π stacking in the nondoped TADF emitter, and thus significantly suppress self‐aggregation‐caused emission quenching for enhanced delayed fluorescence. A peak EQE of 21.6% is realized in the 2tCz2CzBn‐based nondoped device with an extremely low turn‐on voltage of 2.7 V, high color stability, a high brightness over 20 000 cd m−2, a narrow full‐width at half‐maximum of 70 nm, and CIE color coordinates of (0.167, 0.248). [ABSTRACT FROM AUTHOR]

High efficiency white organic light-emitting diodes (WOLEDs) with simple device architecture are desirable for next-generation light sources. However, it is still challenging in the construction of high-performance WOLEDs with a simple device structure. Based on a thermally activated delayed fluorescence (TADF) blue emitter 2SPAc-MPM and a TADF yellow emitter TXO-TPA, high performance two-color WOLEDs with simple device architecture are demonstrated. Benefiting from efficient energy transfer and wide coverage over the visible spectrum, optimized WOLED devices that have a single emitting layer (s-EML) provide a maximum color rendering index (CRI) and maximum external quantum efficiency (EQE) of 78.1 and 21.8%, respectively. More importantly, with multiple emitting layers (m-EMLs), a maximum EQE of 14.5% and a high CRI of 90.7 can be achieved. These results are among the best for the two-color WOLEDs with two TADF emitters. [ABSTRACT FROM AUTHOR]

Developing red thermally activated delayed fluorescence (TADF) emitters, attainable for both high‐efficient red organic light‐emitting diodes (OLEDs) and non‐doped deep red/near‐infrared (NIR) OLEDs, is challenging. Now, two red emitters, BPPZ‐PXZ and mDPBPZ‐PXZ, with twisted donor–acceptor structures were designed and synthesized to study molecular design strategies of high‐efficiency red TADF emitters. BPPZ‐PXZ employs the strictest molecular restrictions to suppress energy loss and realizes red emission with a photoluminescence quantum yield (ΦPL) of 100±0.8 % and external quantum efficiency (EQE) of 25.2 % in a doped OLED. Its non‐doped OLED has an EQE of 2.5 % owing to unavoidable intermolecular π–π interactions. mDPBPZ‐PXZ releases two pyridine substituents from its fused acceptor moiety. Although mDPBPZ‐PXZ realizes a lower EQE of 21.7 % in the doped OLED, its non‐doped device shows a superior EQE of 5.2 % with a deep red/NIR emission at peak of 680 nm. [ABSTRACT FROM AUTHOR]

Abstract: Multifunctional emitting materials are scarce and need to be further explored. Now, a newly anthraquinone derivative, 2‐(phenothiazine‐10‐yl)‐anthraquinone (PTZ‐AQ) was designed and synthesized and found to demonstrate polymorphism, multi‐color emission, aggregation‐induced emission (AIE), mechanochromic luminescence (MCL), and thermally activated delayed fluorescence (TADF) in its different solid forms. It is shown for the first time that TADF properties of a compound can be systematically tuned via its aggregation state. The optimized PTZ‐AQ crystal shows a small singlet–triplet energy splitting of 0.01 eV and exhibits red TADF with a photoluminescence quantum yield as high as 0.848. This study shows that the unique multiple functions can be integrated into one single compound through controlling the aggregation states, which provides a new strategy for the investigation and application of multifunctional organic materials. [ABSTRACT FROM AUTHOR]

A new series of molecules, T1-T4, possessing thermally activated delayed fluorescence (TADF) have been strategically designed and synthesized. Molecules T1-T4 contain the dimethyl acridine as the electron donor, which is linked to either symmetrical or unsymmetrical diphenyl pyrimidine as an acceptor. In comparison to the ubiquitous triazine acceptor, the selection of pyrimidine as an acceptor has advantages of facile functionalization and less stabilized unoccupied π orbitals, so that the energy gap toward the blue region can be accessed. Together with acridine donors, the resulting donor-acceptor functional materials reveal remarkable TADF properties. In the solid state, molecules T1-T4 all exhibit intriguing mechanochromism. The crystal structures, together with spectroscopy and dynamics acquired upon application of stressing, lead us to propose two types of structural arrangement that give distinct emission properties, one with and the other without TADF. Upon fabricating organic light-emitting diodes, the T1-T4 films prepared from sublimation all exhibit dominant TADF behavior; this accounts for their high performance: an electroluminescent emission at λ=490 nm, with an external quantum efficiency of 14.2 %, can be attained when T2 is used as an emitter. [ABSTRACT FROM AUTHOR]

We applied organic nanostructures based on thermally activated delayed fluorescent (TADF) emitters for singlet oxygen generation. Due to the extremely small energy gaps between the excited singlet states (S1) and triplet states (T1) of these heavy-metal-free organic nanostructures, intersystem conversion between S1 and T1 can occur easily. This strategy also works well for exciplex-type TADF emitters prepared by mixing suitable donors and acceptors which have no TADF characteristics themselves. [ABSTRACT FROM AUTHOR]

Sind gründlich studiert worden, allerdings verlief die Entwicklung von roten/nahinfraroten TADF-Emittern viel langsamer als die von grünen und blauen Emittern (TADF: thermisch aktivierte verzögerte Fluoreszenz). Sind gründlich studiert worden, allerdings verlief die Entwicklung von roten/nahinfraroten TADF-Emittern viel langsamer als die von grünen und blauen Emittern (TADF: thermisch aktivierte verzögerte Fluoreszenz). Zhang et al. präsentieren in ihrem Forschungsartikel auf S. 14808 zwei neuartige rote TADF-Emitter. [Extracted from the article]

Charge-Transfer Complexes: Deep-Red/Near-Infrared Electroluminescence from Single-Component Charge-Transfer Complex via Thermally Activated Delayed Fluorescence Channel (Adv. Funct. Keywords: intermolecular charge transfer; near-infrared; organic light-emitting diode; single-component charge-transfer complex; thermally activated delayed fluorescence Intermolecular charge transfer, near-infrared, organic light-emitting diode, single-component charge-transfer complex, thermally activated delayed fluorescence. [Extracted from the article]

Formation of a single‐component charge‐transfer complex (SCCTC) is unveiled in solid state of an intermolecular charge‐transfer molecule 2‐(4‐(1‐phenyl‐1H‐phenanthro[9,10‐d]imidazol‐2‐yl)phenyl)anthracene‐9,10‐dione (PIPAQ). Intermolecular donor–acceptor interactions between two PIPAQ molecules is the primary driving force for self‐association and contributes to intermolecular charge transfer. The SCCTC character is fully verified by crystallographic, photophysical, electron spin resonance, and vibrational characterizations. The PIPAQ‐based SCCTC is first applied in light‐emitting devices as an emissive layer to realize efficient deep‐red/near‐infrared electroluminescence. This work provides new insights into SCCTC and represents an important step toward their applications in optoelectronic devices. [ABSTRACT FROM AUTHOR]

The long-/short-range charge-transfer (LR/SR-CT) type thermally activated delayed fluorescence (TADF) emitter is designed to solve the problem of slow reverse intersystem crossing rate (k RISC) of the traditional MR-TADF emitter and obtain the full-color emission. However, the introduction of LR-CT transition inevitably leads to the broadening of the emission spectrum. In the design of LR/SR-CT type TADF emitters, it is still quite difficult to balance the smaller singlet-triplet energy gap (Δ E ST) and the narrower full-width at half-maximum (FWHM). Here, we investigated the LR-CT and SR-CT proportion of LR/SR-CT TADF emitters by adjusting the strength and position of the peripheral electron-donating units on the MR skeleton (TSBA), and prepared three MR-TADF emitters. The investigation of photophysical properties reveals that the increase in the strength and number of donors significantly reduces the Δ E ST and accelerates the RISC process. The double substitution strategy of the TSBA skeleton effectively reduces the dihedral angle between the MR skeleton and the electron donor unit, and the highest occupied molecular orbital (HOMO)/hole is more distributed on the MR skeleton, which realizes the increase of the excited state SR-CT component. Consequently, the dual-substituted DTPA-TSBA emitter overcomes the contradiction between the small Δ E ST and the narrow FWHM, and achieves the reduction of both. The corresponding device based on DTPA-TSBA achieved a green light emission with a maximum external quantum efficiency (EQE max) of 26.2 % and a FWHM of only 55 nm. This work provides profound guidance for the development of high-performance narrowband TADF emitters. In this paper, the conformation and excited state characteristics of the emitters are adjusted by adjusting the strength and position of the peripheral substituents, endows the long-/short-range charge-transfer (LR/SR-CT) type TADF emitter with a smaller singlet-triplet energy gap (Δ E ST) and a narrower full-width at half-maximum (FWHM). This work provides profound guidance for the development of high-performance narrowband full-color emitters. [Display omitted] • The excited state characteristics of LR/SR-CT type emitters are regulated by peripheral substitution. • By increasing the proportion of SR-CT in the S 1 state of the LR/SR-CT type emitters to achieve a smaller FWHM. • The multi-donor strategy significantly reduces Δ E ST , accelerates RISC process and increases EQE. [ABSTRACT FROM AUTHOR]

[Display omitted] • A clear inverse relationship between efficiencies and dipole moments was found. • Three new blue molecules were designed and synthesized as proof-of-concept. • Record-high performance in non-doped blue OLEDs was achieved. • State-of-the-art performances were delivered in non-doped, doped and hyper-OLEDs. Non-doped and solution-processable deep blue emitters can greatly reduce the manufacturing cost of organic light-emitting diodes (OLEDs). However, influences of parameters concerning intermolecular interactions in solid state have not yet been explored. Herein, we proposed molecular dipole moment as a pre-experimental parameter to evaluate an emitter's performance in the solid state. By extracting efficiency data of OLEDs based on blue-emitting molecules from literature and calculating the dipole moments of these molecules, we found a clear inverse relationship. Three deep blue TADF emitters with similar molecular emitting properties were designed and synthesized. The PL efficiency of their solid films and device performance was found to decrease as the molecular dipole increased. Specifically, TDBA-SPQ with the smallest dipole moments of 1.86 D delivered much better performance in both vacuum-processed and solution-processed non-doped OLEDs with record-high EQE max of 22.7% and 15.2% with CIE-y coordinates of 0.136 and 0.123, respectively. [ABSTRACT FROM AUTHOR]

[Display omitted] • Fullerene fragments are used as acceptor to prepare TADF emitters for the first time. • OLED using one of the fullerenes fragment-based TADF emitter shows high EQE of 20.2%. • Acceptor without heteroatom can be used for designing efficient TADF emitter. • This strategy may open a new path for enhancing operation stability of TADF emitters. Fragments of fullerene are used as acceptor segments for the first time to construct two thermally activated delayed fluorescence (TADF) compounds DBCP and FAP. Both compounds exhibit similar highly twisted geometries and separated frontier molecular orbital distributions. While on the other hand, their locally exited triplet energy levels from acceptor moieties (3LE A) are fine-tunable owning to the different structural stress in the fragments, resulting in different lowest triplet excited state (T 1) features. In DBCP, the 3LE A is the high lying state and thus DBCP exhibits a small singlet–triplet energy difference of 0.10 eV and a high photoluminescence quantum yield (Φ PL) of 89% with excellent TADF characteristics; while T 1 of FAP is 3LE A , and thus, FAP displays poor triplet exciton utilization with Φ PL of only 54%. In organic light-emitting diodes (OLEDs) based on DBCP and FAP as dopants, maximum external quantum efficiencies of 20.2% and 12.8% are respectively achieved. This work not only demonstrates for the first time that fullerene fragments can be used as key building blocks for TADF emitters, it also proves in principle that pure hydrocarbon mobilities without any electronegative heteroatom can also be employed as acceptor segment in high performance TADF emitters. [ABSTRACT FROM AUTHOR]

• Facile synthesis of 3,5-dicyanapyridine acceptors with different side substituents. • Three TADF emitters with rigid structures achieve high photoluminescent quantum yield. • Highly efficient TADF-OLEDs with external quantum efficiency up to 29.1%. As the blooming of thermally activated delayed fluorescent (TADF) materials, organic light-emitting diodes (OLEDs) possessing high external quantum efficiency (EQE) and low efficiency roll-off are under eager pursuit. Herein, three molecules, 4-(4-(9,9-dimethylacridin-10(9 H)-yl)phenyl)-2,6-diphenylpyridine-3,5-dicarbonitrile (Ph-DMAC), 4-(4-(9,9-dimethylacridin-10(9 H)-yl)phenyl)-2,6-di(naphthalen-1-yl)pyridine-3,5-dicarbonitrile (Na-DMAC) and 4′-(4-(9,9-dimethylacridin-10(9 H)-yl)phenyl)-[3,2′:6′,3″-terpyridine]-3′,5′-dicarbonitrile (3Py-DMAC) with a twisted donor–acceptor structure comprising 3,5-dicynanopryidine with different 2,6-substutents as acceptor and 9,10-dimethylacridan as donor were designed and synthesized. With the highly twisted conformations, effective TADF is achieved in these molecules. Ph-DMAC delivers a high photoluminescent quantum yield (PLQY) of 89% ascribed to its rigid acceptor geometry. Na-DMAC and 3Py-DMAC suffer a slight decrease in efficiency due to excess vibration induced by their naphthyl and pyridinyl moieties. A Ph-DMAC based OLED achieves a very high maximum EQE of 29.1% due to its high PLQY and efficient TADF. With a relatively short delayed lifetime, 3Py-DMAC based OLEDs show only mild efficiency roll-off. [ABSTRACT FROM AUTHOR]