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Conformational engineering is essential to further reinforce the luminescent properties of thermally activated delayed fluorescence (TADF) materials featuring through‐space charge transfer (TSCT) characteristics. Herein, two TSCT‐TADF emitters (8MeDM‐B and 8FDM‐B) with the methyl and fluorine moieties substituted at the C8 site of the rigid spiro‐fluorene bridge is reported. Derivation of the C8 site is first proposed to control the molecular configuration with the ability to indirectly tune the intramolecular interaction between donor and acceptor groups. As a result, 8MeDM‐B and 8FDM‐B both present small singlet‐triplet energy gaps, fast reverse intersystem crossing rates, and high photoluminescence quantum yields. Interestingly, the smaller fluorine atom not the bigger methyl group exhibits more evident electrostatic repulsive force onto the central donor and thus rectifies the central spiro structure. Consequently, the high external quantum efficiency values of 28.8% and 31.7% for 8MeDM‐B and 8FDM‐B‐based electroluminescence devices are achieved, respectively. This study offers a measure for enhancing TSCT‐TADF emitters without directly modifying the donor or acceptor. [ABSTRACT FROM AUTHOR]

Organic materials with multi‐stimulus response (MSR) properties have demonstrated many potential and practical applications. Herein, a π‐stacked thermally activated delayed fluorescence (TADF) material with multi‐stimulus response (MSR) properties, named SDMAC, was designed and synthesized using distorted 9,9‐dimethyl‐10‐phenyl‐9,10‐dihydroacridine as a donor. SDMAC possesses a rigid π‐stacked configuration with intramolecular through‐space interactions and exhibits aggregation‐induced emission enhancement (AIEE), solvatochromic, piezochromic, and circularly polarized luminescence (CPL) under different external stimuli. The rigid molecular structure and efficient TADF properties of SDMAC can be used in displays and lighting. Using SDMAC as an emitter, the maximum external quantum efficiency (EQE) of the fabricated organic light‐emitting diodes (OLEDs) is as high as 28.4 %, which make them the most efficient CP‐TADF OLEDs based on the through‐space charge transfer strategy. The CP organic light‐emitting diodes (CP‐OLEDs) exhibit circularly polarized electroluminescence (CPEL) signals. [ABSTRACT FROM AUTHOR]

Multi‐layer π‐stacked emitters based on spatially confined donor/acceptor/donor (D/A/D) patterns have been developed to achieve high‐efficiency thermally activated delayed fluorescence (TADF). In this case, dual donor moieties and a single acceptor moiety are introduced to form two three‐dimensional (3D) emitters, DM‐BD1 and DM‐BD2, which rely on spatial charge transfer (CT). Owing to the enforced face‐to‐face D/A/D pattern, effective CT interactions are realized, which lead to high photoluminescence quantum yields (PLQYs) of 94.2 % and 92.8 % for the two molecules, respectively. The resulting emitters exhibit small singlet–triplet energy splitting (ΔEST) and fast reverse intersystem crossing (RISC) processes. Maximum external quantum efficiencies (EQEs) of 28.0 % and 26.6 % were realized for devices based on DM‐BD1 and DM‐BD2, respectively, which are higher than those of their D/A‐type analogues. [ABSTRACT FROM AUTHOR]

Derivatives based on anthryleno[1,2‐b]pyrazine‐2,3‐dicarbonitrile (DCPA) are used as luminescent materials, to realize near‐infrared (NIR) electroluminescence. By functionalizing DCPA with aromatic amine donors, two emitters named DCPA‐TPA and DCPA‐BBPA are designed and synthesized. Both molecules have large dipole moments owing to the strong intramolecular charge transfer interactions between the amine donors and the DCPA acceptor. Thus, compared with doped films, the emission of neat films of DCPA‐TPA and DCPA‐BBPA can fully fall into the NIR region (>700 nm) with increasing surrounding polarity by increasing doping ratio. Moreover, the non‐doped devices based on DCPA‐TPA and DCPA‐BBPA provide NIR emission with peaks at 838 and 916 nm, respectively. A maximum radiance of 20707 mW Sr−1 m−2 was realized for the further optimized device based on DCPA‐TPA. This work provides a simple and efficient strategy of molecular design for developing NIR emitting materials. [ABSTRACT FROM AUTHOR]