Versatile and High‐Performance LiTaO3:Tb3+, Gd3+ Perovskite for Multimode Anti‐counterfeiting, Flexible X‐Ray Imaging, Continuous Stress Sensing, and Non‐Real‐Time Recording.

Multimode luminescence relates to how charge carriers are transported and recombined in response to various physical excitations. It shows promising applications in many fields like advanced anti‐counterfeiting, information storage and encryption. Enabling a stable single compound with multimode luminescence is a unique technology but still remains a challenge. Herein, a versatile and high‐performance energy storage LiTaO3:0.01Tb3+,xGd3+ perovskite is discovered by utilizing the interplay of electron‐trapping defect levels and hole‐trapping Tb3+. It combines an excellent charge carrier storage capacity (≈7 and 12 times higher than state‐of‐the‐art BaFBr(I):Eu2+ and Al2O3:C), >1200 h storage duration, >40 h afterglow, efficient optically stimulated luminescence, persistent mechanoluminescence, and force‐induced charge carrier storage features. Particularly, it well responds to various stimuli channels, i.e., wide‐range X‐rays to 850 nm infrared photons, thermal activation, mechanical force grinding, or compression. To elucidate this multimode luminescence, charge carrier trapping and release processes in LiTaO3:0.01Tb3+,xGd3+ with various physical stimulations will be unraveled by combining the vacuum‐referred binding diagram construction, spectroscopy, thermoluminescence, and mechanoluminescence techniques. The versatile and high‐performance LiTaO3:0.01Tb3+,xGd3+ enables promising proof‐of‐concept multimode luminescence applications in advanced anti‐counterfeiting, flexible X‐ray imaging, continuous compression force sensing, and non‐real‐time recording. [ABSTRACT FROM AUTHOR]