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Designing Photochromic Materials with Large Luminescence Modulation and Strong Photochromic Efficiency for Dual‐Mode Rewritable Optical Storage

Inorganic materials combining photochromism and luminescence modulation characteristics have great potential in dual‐mode rewritable optical storage due to their unique optical features and excellent thermal stability. However, the failure of achieving a large luminescence modulation and a strong photochromic efficiency in photostimulated inorganic photochromic materials limits their applications. Herein, a new strategy for realizing an overlap between the photochromic absorption peak and the photoluminescent emission/excitation peak is proposed for designing high‐performance photochromic materials. The obtained BaMgSiO4: M (M = Ce3+, Mn2+, or Nd3+) ceramics exhibit a reversible white‐pink color change upon alternate 310 nm and 590 nm illumination (or thermal stimulus) accompanied by a high photochromic efficiency (>50%). Benefiting from a perfectly matched photochromic absorption peak and Mn2+ emission peak, a record luminescence modulation of 96.3% with excellent fatigue resistance is obtained in BaMgSiO4: Mn2+ ceramics. These properties are superior to all photochromic materials reported to date, demonstrating great potential in optical information storage applications. The trap‐related photochromic and regulated luminescence behavior is investigated together with a prototype of a dual‐mode information display. This work is expected to promote the practical application of photochromic materials in various optical devices and provides an effective strategy to develop other photochromic materials.