Exciton Regulation and Fluorescence Switching via Redox‐Responsive Heterojunction Interfaces

Redox-responsive fluorescence regulation at heterointerfaces remains a critically underdeveloped yet strategically significant domain in advanced chemical sensing. Herein, we present an exciton modulation strategy enabled by heterojunction engineering between electron-rich CdSe quantum dots and an electron-deficient covalent triazine framework (CTF). This type-I CdSe@CTF heterostructure achieves nanoscale electronic decoupling and directional charge redistribution, unveiling a previously unreported fluorescence-switching mechanism governed by redox-triggered interfacial reconfiguration. Beyond excitonic regulation, the heterostructure intrinsically mimics oxidase-like catalysis, enabling dual fluorescence-colorimetric readouts within a unified excitonic framework. When embedded into flexible electrospun membranes and combined with artificial neural network (ANN)-based image recognition, the system offers adaptive and intelligent detection under bio-relevant conditions. This study establishes a molecularly encoded design paradigm that bridges exciton dynamics, redox chemistry, and wearable photonic sensing, offering a blueprint for the development of multifunctional bioelectronic platforms.