Optoelectronic functional surfaces/interfaces are a representative research direction in surface and interface chemistry, and their performance requires precise regulation at both the molecular and interfacial microstructural levels. To address this key scientific issue, the applicant proposes a strategy based on innovative preparation of optoelectronic molecules and multilevel synergistic regulation of interfacial microstructures. Grounded in the principles of colloid and interface chemistry, and integrating precise chemical synthesis, assembly, and theoretical calculations, the applicant has conducted systematic applied basic research. (1) At the molecular level, new synthetic methods have been developed for main-group-element-containing viologens and spatially conjugated viologen derivatives. These enhance spin–orbit coupling, reduce the bandgap and reduction potential, and enable precise, multi-pathway regulation of optoelectronic activity, thereby clarifying the molecular-level regulation mechanism of viologen derivatives. (2) At the interfacial level, viologen derivatives are used as building units. Through interfacial confinement assembly and component energy-level matching, optoelectronic functional surfaces/interfaces are constructed via electrostatic, hydrogen-bonding, and covalent assembly. This improves charge separation efficiency and elucidates the synergistic regulation mechanism at the molecular and heterogeneous interfacial microstructural levels. (3) At the application level, based on molecular innovation and interfacial assembly regulation, high-stability electrochromic smart camouflage devices have been developed and engineering-validated. This research establishes a distinctive viologen-based functional surface/interface system with original innovation, achieves full-chain exploration from fundamental research to application validation, and enriches physical chemistry, particularly colloid and interface chemistry.

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