Kinetic‐Programmed Hydrolysis Enables Intelligent Time‐Evolving Phosphorescence in Water

Abstract

ABSTRACT The development of aqueous room‐temperature phosphorescent (RTP) materials with dynamically programmable afterglow remains a significant challenge. Herein, we report a universal and programmable synthesis paradigm that overcomes this limitation by orchestrating the hydrolysis kinetics of aminosilanes. This approach constructs silylated carbon dots (Si‐CDs) with dual‐emission centers covalently locked within a rigid silica matrix. The aminosilane precursor serves as a multifunctional building block, simultaneously acting as the carbon source, electron donor, and molecular bridge, which synergistically enhances intersystem crossing while effectively suppressing non‐radiative decay. The resulting ultra‐small nanoparticles (7–9 nm) exhibit exceptional aqueous RTP performance, including a long lifetime of 859 ms and a high quantum yield of 29.3%. More importantly, we pioneer the concept of programmable time‐dependent phosphorescence (TDP), enabling on‐demand, dynamic color evolution (e.g., from red to blue) through precise kinetic control. This intelligent temporal color coding, attributed to the synergy between charge‐transfer modulation and matrix confinement, opens a new dimension for optical information security. We further demonstrate its transformative potential in autofluorescence‐free in vivo bioimaging, advanced anti‐counterfeiting, and dynamic 3D data encryption. This work provides a versatile platform for the rational design of next‐generation intelligent photonic nanomaterials.