A Molecular Descriptor Guided Asymmetric Strategy for High Carrier-Mobility Light-Emitting Organic Semiconductors

Abstract

Combining high mobility and high-efficiency luminescence in one material is challenging because of their contradictory design principles. Here, under the three-state exciton model, a molecular descriptor O = (|t_h + t_e| - |t_h - t_e|)/2J is proposed to quantitatively design materials with balanced luminescence and mobility in aggregated states, where a large O would promise high crystalline photoluminescence quantum yield (PLQY) with small J (excitonic coupling) and significant t_h and t_e (hole and electron transfer integrals) would indicate high mobility. Through theoretical calculation and experimental validation, it is found that the asymmetric anthracene derivatives are quite effective in simultaneously achieving high mobility and high PLQY. Following the asymmetric guideline, the newly developed compounds, 2-phenyl vinyl anthracene (2-PhVA) and 6-(2-(anthracene-2-yl)vinyl)benzo[b]thiophene (6-BTVA) demonstrate high O values alongside excellent performance: 2-PhVA exhibits a PLQY of 81.5% and a maximum hole mobility of 10.0 cm² V^-1 s^-1, and 6-BTVA shows a PLQY of 30.9% with a maximum mobility of 9.3 cm² V^-1 s^-1. The above results demonstrate the validation of the descriptor and the asymmetric strategy in further developing high-mobility light-emitting aggregated materials.

Keywords

aggregated states / asymmetric strategy / carrier mobility / molecular descriptor / photoluminescence quantum yield (PLQY)

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