Electrochemiluminescence of hot exciton nanomaterial with boosted efficiency for visual bioanalysis

Abstract

The electrochemiluminescence (ECL) efficiency (ΦECL) of organic ECL emitters is greatly influenced by the excited state property and component. Here we design a hot exciton molecule (BCzP-BT) with hybridized local and charge-transfer (HLCT) excited state property to prepare the first hot exciton organic nanorods (BB NRs). The BB NRs exhibit both sensitive annihilation and intense coreactant ECL emissions with a band gap emission model. Due to the reverse intersystem crossing among high-lying excited states (hRISC), the HLCT excited state property leads to highly efficient utilization of triplet excitons and thus high photoluminescence quantum yields (ΦPL) of more than 80% at 554 nm, which is demonstrated by solvatochromic experiments and quantum chemical calculations. The high ΦPL endows BB NRs with superior ΦECL over other nanoemitters, even the thermally activated delayed fluorescence materials, and thus offers highly-efficient nanoemitters for the design of ECL imaging strategy. As a proof of concept, an ECL probe is constructed by assembling BHQ2-ssDNA on BB NRs to integrate CRISPR/Cas12a system for target recognition, which produces a rapid and high-throughput ECL imaging platform. The proposed imaging method for HPV16 DNA detection shows excellent performance with a detection limit of 0.6 fM. This work broadens the application of hot exciton materials in ECL field, and opens a new avenue for developing next-generation ECL devices.