Manipulation of X‐Ray Persistent Radioluminescence in Core–Shell–Shell Nanoparticles for Energy‐Discriminated Chromatic 3D Imaging

Lanthanide-doped fluoride nanoparticles with tunable persistent radioluminescence (persistent RL) have emerged as promising scintillators for 3D X-ray delay imaging. However, its core challenges persist in developing a highly-discriminative imaging detection technologies for complex structures composed of materials with similar density. Here, a persistent RL-assisted energy-discriminated approach is developed to realize high-resolution chromatic X-ray 3D imaging for visualizing material specificity in complex structures. We demonstrated highly differentiated, energy-dependent, precisely persistent RL multicolor tuning within a single Core-Shell-Shell (CSS) heterogeneous nanoparticles. We uncover the fundamental mechanism underlying persistent RL decay kinetics, establishing a mechanistic framework that links X-ray energy to color dynamics. This mechanistic insight enables to establish a general design principle for color-engineered persistent RL nanocrystals and achieving precise discrimination of energy through color-based information. Moreover, flexible imaging detector incorporating the CSS nanoparticles with the ability to self-repair, be recycled, and record images, and demonstrated chromatic 3D imaging capable of resolving complex objects with subtle distinctions at a low X-ray dose rate of 15.1 uGy/s. These findings not only elucidate the photophysical origins of color-tunable persistent RL, but also pave the way for next-generation efficient X-ray imaging systems with broad potential across medical, industrial, and scientific applications.