Excitation-Dependent Emission in Sb3+-Doped All-Inorganic Rare-Earth Double Perovskites for Anticounterfeiting Applications.

ABSTRACT

Achieving high-efficiency tunable emission in a single phosphor remains a significant challenge. Herein, we report a series of Sb3+-doped all-inorganic double perovskites, Sb3+Cs2NaScCl6, with efficient excitation-dependent emission. In 0.5%Sb3+Cs2NaScCl6, strong blue emission with a high photoluminescence quantum yield (PLQY) of 85% is obtained under 265 nm light irradiation, which turns into bright neutral white light with a PLQY of 56% when excited at 303 nm. Spectroscopic and computational investigations were performed to reveal the mechanism of this excitation-dependent emission. Sb3+ doping induces two different excitation channels the internal transition of Sb3+ 5s2 → 5s5p and the electron transfer transition of Sb3+ 5s → Sc3+ 3d. The former one generates excited Sb3+ ions, which can undergo efficient energy transfer to populate the host self-trapped exciton (STE) state, yielding enhanced blue emission. The latter one leads to the formation of a new STE state with the hole localized on Sb3+ and the electron delocalized on the nearest Sc3+, which accounts for the newly exhibited low-energy emission. The difference in the excitation pathways of the two emitting STE states results in the highly efficient excitation-dependent emission, making the doped systems promising anticounterfeiting materials.