Nonstoichiometry Tailored Energy Flow Pathway Toward Multicolor Dynamic Thermo‐Stimulated Luminescence (DTSL) and Smart Optical Information Storage

Luminescent materials, with their multidimensional photon modulation and sensitivity to intrinsic/extrinsic stimuli, underpin emerging technologies spanning ultrahigh‐density data storage, high‐power lighting, and ultra‐sensitive detection. While static luminescence dominates conventional applications, dynamic luminescent systems offer superior information capacity through spatiotemporal light evolution and multiplexing. However, this paradigm shift is hindered by activator paucity and similar luminescence kinetics that confine most systems to monochromatic intensity variations. Here, this chromatic stagnation is broken through a dynamic thermo‐stimulated luminescence (DTSL) platform exhibiting temperature‐gated temporal evolution of dual‐emission intensity ratios, enabling quantized and visible chromatic transitions from green→cyan→blue. It originates from the dynamic interplay between blue emission (derived from deep‐level oxygen vacancy centers) and green luminescence (generated by Eu2⁺ activators) and thus tunable relative intensity, under the premise of the concerted modulation of defect concentration and energy level positioning. Mechanism studies reveal that nonstoichiometric doping creates a hierarchical defect architecture, where controlled energy partitioning between deep and shallow defects governs the time‐resolved chromatic trajectory. Beyond establishing a general framework for dynamic luminescence design, the work rationally manipulates the fundamental relationship between defect architecture and photonic information, opening previously unfeasible multicolor DTSL avenues for optical multiplexing.