Highly Efficient Near-Infrared Thermally Activated Delayed Fluorescent Emitters in Non-Doped Electroluminescent Devices.

Constructing organic near-infrared (NIR) luminescent materials to confront the formidable barrier of "energy gap law" remains challenging. Herein, two NIR thermally activated delayed fluorescence (TADF) molecules named T-ß-IQD and TIQD were developed by connecting N,N-diphenylnaphthalen-2-amine and triphenylamine with a novel electron withdrawing unit 6-(4-(tert-butyl)phenyl)-6H-indolo[2,3-b]quinoxaline-2,3-dicarbonitrile. It is confirmed NIR-TADF emitters concurrent with aggregation-induced emission effect, J-aggregate with intra- and intermolecular CN⋅⋅⋅H-C and C-H⋅⋅⋅π interactions, and large center-to-center distance in solid states can boost the emissive efficiencies both in thin films and non-doped organic light-emitting diodes (OLEDs). Consequently, the T-ß-IQD-based non-doped NIR-OLED achieved the maximum external quantum efficiency (EQEmax ) of 9.44 % with emission peak at 711 nm, which is one of the highest efficiencies reported to date for non-doped NIR-OLEDs.

Large Orientation Angle Buried Substrate Enables Efficient Flexible Perovskite Solar Cells and Modules.

Flexible perovskite solar cells (f-PSCs) have emerged as potential candidates for specific mechanical applications owing to their high foldability, efficiency, and portability. However, the power conversion efficiency (PCE) of f-PSC remains limited by the inferior contact between perovskite and flexible buried substrate. Here, an asymmetric π-extended self-assembled monolayer (SAM) (4-(9H-dibenzo[a,c]carbazol-9-yl)butyl)phosphonic acid (A-4PADCB) is reported as a buried substrate for efficient inverted f-PSCs. Employing this design strategy, A-4PADCB exhibits a significant orientation angle away from the surface normal, homogenizing the distribution of contact potentials. This enhancement improves the SAM/perovskite interface quality, controlling the growth of favorable perovskite films with low defect density and slight tensile stress. Integration of A-4PADCB into small-area f-PSCs and large-area flexible perovskite solar modules with an aperture area of 20.84 cm2 achieves impressive PCEs of up to 25.05% and 20.64% (certified 19.51%), respectively. Moreover, these optimized A-4PADCB-based f-PSCs possess enhanced light, thermal, and mechanical stability. This research paves a promising avenue toward the design of SAM-buried substrates with a large orientation angle, regulating perovskite growth, and promoting the commercialization of large-area flexible perovskite photovoltaics.

Optimizing the energy level alignment for achieving record-breaking efficiency in hot exciton deep red OLEDs.

To effectively compete with the quenching process in long-wavelength regions like deep red (DR) and near-infrared (NIR), rapid radiative decay is urgently needed to address the challenges posed by the "energy gap law". Herein, we confirmed that it is crucial for hot exciton emitters to attain a narrow energy gap (ΔES1-T2) between the lowest singlet excited (S1) state and second triplet excited (T2) state, while ensuring that T2 slightly exceeds S1 in the energy level. Two proofs-of-concept of hot exciton DR emitters, namely αT-IPD and ßT-IPD, were successfully designed and synthesized by coupling electron-acceptors N,N-diphenylnaphthalen-2-amine (αTPA) and N,N-diphenylnaphthalen-1-amine (ßTPA) with an electron-withdrawing unit 5-(4-(tert-butyl) phenyl)-5H-pyrazino[2,3-b]indole-2,3-dicarbonitrile (IPD). Both emitters exhibited a narrow ΔES1-T2, with T2 being slightly higher than S1. Additionally, both emitters showed significantly large ΔET2-T1. Moreover, due to their aggregation-induced emission characteristics, J-aggregated packing modes, moderate strength intermolecular CN⋯H-C and C-H⋯π interactions, and unique, comparatively large center-to-center distances among trimers in the crystalline state, both αT-IPD and ßT-IPD emitters exhibited remarkable photoluminescence quantum yields of 68.5% and 73.5%, respectively, in non-doped films. Remarkably, the corresponding non-doped DR-OLED based on ßT-IPD achieved a maximum external quantum efficiency of 15.5% at an emission peak wavelength of 667 nm, representing the highest reported value for hot exciton DR-OLEDs.

Hot-Exciton Mechanism and AIE Effect Boost the Performance of Deep-Red Emitters in Non-Doped OLEDs.

Luminescent materials possessing a "hot-exciton" mechanism and aggregation-induced emission (AIE) qualities are well-suited for use as emitting materials in nondoped organic light-emitting diodes (OLEDs), particularly in deep-red regions where their ground state and singlet excited state surfaces are in proximity, leading to the formation of multiple nonradiative channels. However, designing molecules that artificially combine the hot-exciton mechanism and AIE attributes remains a formidable task. In this study, a versatile strategy is presented to achieve hot-exciton fluorescence with AIE property by increasing the first singlet excited (S1 ) state through modulation of the conjugation length of the newly created acceptor unit, matching the energy level of high-lying triplet (Tn ) states, and enhancing exciton utilization efficiency by employing suitable donor moieties. This approach reduces the aggregation-caused quenching (ACQ) in the aggregate state, resulting in the proof-of-concept emitter DT-IPD, which produces an unprecedented external quantum efficiency (EQE) of 12.2% and Commission Internationale de I'Eclairage (CIE) coordinates of (0.69, 0.30) in a deep-red non-doped OLED at 685 nm, representing the highest performance among all deep-red OLEDs based on materials with hot-exciton mechanisms. This work provides novel insights into the design of more efficient hot-exciton emitters with AIE properties.

Pioneering research on blue "hot exciton" polymers and their application in solution-processed organic light-emitting diodes.

An innovative novel category of polymeric hybridized local and charge-transfer (HLCT) blue materials prepared via solution processing has yet to be reported. This study introduces three polymers, namely PZ1, PZ2, and PZ3, incorporating donor-acceptor-donor (D-A-D) structures with carbazole functioning as the donor and benzophenone as the acceptor. To regulate the luminescence mechanism and conjugation length, carbonyl and alkyl chains are strategically inserted into the backbone. Theoretical calculation and transient absorption spectroscopy illustrate that the robust spin-orbit coupling between high-lying singlet excited states (Sm: m ⩽ 4) and triplet excited states (Tn: n ⩽ 7) of the polymers hastens and significantly heightens the efficiency of reverse intersystem crossing processes from Tn states. Furthermore, the existence of multiple degenerated frontier molecular orbits and significant overlaps between Tn and Sm states give rise to added radiative pathways that boost the radiative rate. This study marks a fundamental and initial manifestation of HLCT materials within the polymer field and provides a new avenue for the design of highly efficient polymeric emitters.