From Photons to Persistent Memory: Optically Controlled Trap Engineering Enables Secure, Hierarchical Optical Storage

ABSTRACT Electron‐trapping materials offer immense promise for advanced optical data storage systems, yet achieving secure multi‐level information encoding and retrieval has remained an ongoing challenge. In this work, we present a materials‐centric solution that addresses this limitation by integrating up‐conversion charging (UCC) with photo‐stimulated trap manipulation (PSTM) within a tailored phosphor platform, MgGeO 3 triply doped with Mn 2+ , Yb 3+ , and Eu 3+ ions. Here, Mn 2+ serves as the emission center, whereas Yb 3+ and Eu 3+ cooperatively engineer a hierarchical multi‐trap landscape. UCC exploits a nonlinear two‐photon ionization process to write high‐resolution patterns. Concurrently, PSTM uses ambient visible light to transfer electrons from deep to shallower traps, unlocking concealed data layers on demand. By recording distinct patterns in specific traps and retrieving them via afterglow, infrared stimulation, or PSTM activation, we demonstrate multi‐channel storage validated by spectroscopic and imaging evidence. This strategy pioneers a secure, multidimensional, and cost‐effective optical storage paradigm, shifting emphasis from hardware complexity to intrinsic material functionality—toward a future where information endures as persistently as the light that preserves it.