Boosting the Self-Trapped Exciton Emission in Cs2NaYCl6 Double Perovskite Single Crystals and Nanocrystals

Halide double perovskites have aroused substantial research interest because of their unique optical properties and intriguing flexibility for various compositional adjustments. Herein, we report the synthesis and photophysics of rare-earth element yttrium (Y)-based double perovskite single crystals (SCs) and nanocrystals (NCs). The pristine Cs2NaYCl6 bulk SCs exhibit a weak sky-blue emission with a low photoluminescence quantum yield (PLQY) of 7.68% based on the self-trapped exciton (STE), while no PL emission was observed for NCs. Excitingly, the STE emission of SCs and NCs is greatly enhanced via Sb3+ doping. The optimized Cs2NaYCl6:Sb3+ SCs and NCs exhibit high PLQYs up to 82.5% and 51.8%, respectively. Theoretical calculations and charge-carrier dynamic studies demonstrate that the giant emission enhancement after Sb3+ doping is related with the enhancement of the sensitization of the emissive STE states, the passivating of the nonradiative carrier trapping processes, and the regulation of carrier-phonon coupling.