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Deep‐red and near‐infrared emitters with twisted donor–acceptor (D–A) structures often exhibit suboptimal performance in organic light‐emitting diodes (OLEDs) due to constraints imposed by the energy gap law. In this work, a pure hydrogen carbon (PHC) host material named SBF‐DTP is purposefully tailored for deep‐red OLEDs. The excellent capacity of SBF‐DTP to support D–A type DR emitters effectively arises from its distinctive attributes: localized excitation states, 3D configuration, and low polarity. When employing SBF‐DTP as the host for the fluorescence emitter DCPA‐TPA and the thermally activated delayed fluorescence emitter APDC‐DTPA, doped films exhibit substantially enhanced photoluminescence quantum yields. This improvement leads to high‐efficiency OLEDs with external quantum efficiencies of 5.47% for DCPA‐TPA and 20.03% for APDC‐DTPA, respectively, which is about twice as high as the initial reports. This findings underscore the paramount significance of developing efficient host materials in the pursuit of high‐performance deep red and even near‐infrared OLEDs. [ABSTRACT FROM AUTHOR]

A novel bipolar host molecule di-spiro [fluorene-9,5′-quinolino [3,2,1-de] acridine-9′,9″-fluorene]-2,2″,7,7″-tetracarbonitrile (QACN) featuring an Acceptor-σ-Donor-σ-Acceptor structure was developed. Systematic investigations into its photophysical, electrochemical, and thermal properties unveiled exceptional thermal stability, a three-dimensional spatial configuration, and bipolar carrier transport capability. Employing QACN as the host material in red phosphorescent and thermally activated delayed fluorescent (TADF) organic light-emitting diodes (OLEDs) yielded a maximum external quantum efficiency of 25.3 % and 16.5 %, respectively. Compared with the commercial material TPBi (EQE = 12.0 %, λ EL = 668 nm) and mCP (EQE = 14.5 %, λ EL = 652 nm), the TADF OLEDs based on QACN achieved a higher EQE and a large red-shift emission (EQE = 16.5 %, λ EL = 694 nm). These findings underscore the potential of QACN as an effective host material for red phosphorescent and TADF emitters and provide a new auxiliary finesse for realizing deep red and near-infrared (NIR) OLEDs. [Display omitted] • A highly twisted bipolar host material QACN with A-σ-D-σ-A structure was designed and synthesized. • The orthogonal structure, thermal stability, and desirable energy levels of QACN make it an effective host for red emitters. • QACN-based TADF OLEDs achieved higher EQE and significant red-shifted emission compared to commercial host materials. [ABSTRACT FROM AUTHOR]