Highly Luminescent 2D-Type Slab Crystals Based on a Molecular Charge-Transfer Complex as Promising Organic Light-Emitting Transistor Materials

A new 2:1 donor (D):acceptor (A) mixed-stacked charge-transfer (CT) cocrystal comprising isometrically structured dicyanodistyrylbenzene-based D and A molecules is designed and synthesized. Uniform 2D-type morphology is manifested by the exquisite interplay of intermolecular interactions. In addition to its appealing structural features, unique optoelectronic properties are unveiled. Exceptionally high photoluminescence quantum yield (Φ_F ≈ 60%) is realized by non-negligible oscillator strength of the S₁ transition, and rigidified 2D-type structure. Moreover, this luminescent 2D-type CT crystal exhibits balanced ambipolar transport (µ_h and µ_e of ≈10⁻⁴ cm² V⁻¹ s⁻¹). As a consequence of such unique optoelectronic characteristics, the first CT electroluminescence is demonstrated in a single active-layered organic light-emitting transistor (OLET) device. The external quantum efficiency of this OLET is as high as 1.5% to suggest a promising potential of luminescent mixed-stacked CT cocrystals in OLET applications.

A novel 2D-type slab crystal based on 2:1 donor:acceptor mixed-stacked charge-transfer (CT) complex is developed. Unique optoelectronic properties: balanced ambipolar transport (µ_e, µ_h ≈ 10⁻⁴ cm² V⁻¹ s⁻¹) and bright luminescence (Φ_F ≈ 60%) are successfully bridged in organic field-effect transistor (OFET) devices, demonstrating the first CT organic light-emitting transistors with high external quantum efficiency up to 1.5%.

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