Halogen Content Tunes the Color Temperature of White Light and Afterglow in Zero-Dimensional Hybrid Indium Halides

Zero-dimensional (0D) organic–inorganic hybrid metal halides (OIMHs) have been a category of non-negligible candidates with potential application in light-emitting diodes (LEDs), optical information storage, and anticounterfeiting. Herein, we first obtained two 0D isomorphic indium-based OIHMs, namely, IBPAInCl 6 ·H 2 O and IBPAInBr 6 ·H 2 O (IBPA 3+ = bis(3-aminopropyl)amine cation), and further prepared a family of crystal samples of mixed-halogen IBPAIn(Cl 1– x Br x ) 6 ·H 2 O ( x = 0.25, 0.5, and 0.75) with the strategy of halogen substitution, which integrated the bluish-white photoluminescence (PL) emission of IBPAInCl 6 ·H 2 O and the orange PL emission of IBPAInBr 6 ·H 2 O as a perfect pair of complementary colors affording white-light emission. Interestingly, the cold-warm-tunable white-light emission in single-metal-templated In-based OIMHs was realized for the first time via continuous halogen content control. Mechanistic studies disclose that the ratios of the emission intensities at higher energies and lower energies present a gradual variation tendency, resulting in cold-warm-tunable white-light emissions. Moreover, the ultralong afterglow of IBPAInCl 6 ·H 2 O (1.1 s) that can be identified by the naked eyes was found to be facilely tuned by regulating the content of Br – anions. Hence, the crystal samples of halogen substitution in In-based halides were applied as anticounterfeiting/information storage materials to fabricate a time-resolved encryption system with high performance.