Kinetic-Programmed Hydrolysis Enables Intelligent Time-Evolving Phosphorescence in Water.

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.