Aggregation-induced delayed electrochemiluminescence of organic dots in aqueous media

Abstract

Full utilization of the excited species at both singlet states (¹R*) and triplet states (³R*) is crucial to improving electrochemiluminescence (ECL) efficiency but is challenging for organic luminescent materials. Here, an aggregation-induced delayed ECL (AIDECL) active organic dot (OD) containing a benzophenone acceptor and dimethylacridine donor is reported, which shows high ECL efficiency via reverse intersystem crossing (RISC) of non-emissive ³R* to emissive ¹R*, overcoming the spin-forbidden radiative decay from ³R*. By introducing dual donor-acceptor pairs into luminophores, it is found that nonradiative pathway could be further suppressed via enhanced intermolecular weak interactions, and multiple spin-up conversion channels could be activated. As a consequence, the obtained OD enjoys a 6.8-fold higher ECL efficiency relative to the control AIDECL-active OD. Single-crystal studies and theoretical calculations reveal that the enhanced AIDECL behaviors come from the acceleration of both radiative transition and RISC. This work represents a major step towards purely organic, high-efficiency ECL dyes and a direction for the design of next-generation ECL dyes at the molecular level.

Keywords

aggregation-induced delayed electrochemiluminescence / benzophenone / dimethylacridine / organic dots / reverse intersystem crossing

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