LAUSR

Excitation-dependent (Ex-De) photoluminescence, characterized by distinct emission color changes under varying excitation wavelengths, has been extensively investigated in doped systems, where luminescence relies on a dopant-host synergy. However, Ex-De behavior achieved through two independent luminescent centers in undoped metal halide lattices has scarcely been reported. Herein, we synthesized two novel zero-dimensional (0D) bimetallic halides (BMHs), [Eu(UREA)7H2O][SbCl6] (Eu-U) and [Tb(UREA)7H2O][SbCl6] (Tb-U), via a cooling crystallization method. Structural analyses reveal that Eu3+/Tb3+ ions coordinate with UREA and water molecules to form cationic complexes [Eu(UREA)7(H2O)]3+/[Tb(UREA)7(H2O)]3+, which isolate [SbCl6]3- anions. Hirshfeld surface analysis further indicates substantial hydrogen bonding between the complex cations and [SbCl6]3- octahedra, leading to notable structural distortion. Spectroscopic studies confirm that both compounds can exhibit simultaneous broadband emission from Sb3+ and narrowband emission from Eu3+/Tb3+, with no energy transfer between the centers. Leveraging this unique Ex-De behavior, we fabricated anticounterfeiting patterns by embedding Eu-U and Tb-U in silicone, demonstrating effective information concealment and retrieval. This work not only enriches the family of BMHs but also realizes synergistic narrowband and broadband emission, offering new insights for designing Ex-De luminescent materials with independent dual emitting centers.