Structural Dimensionality Modulation toward Enhanced Photoluminescence Efficiencies of Hybrid Lead-Free Antimony Halides

Rationally optimizing the photoluminescence performance via accurate structural modulation is one of most important and challenging issues for hybrid halides. Herein, a viable crystal dimensional reduction strategy is proposed to reasonably enhance the photoluminescence quantum yield (PLQY) of hybrid antimony halide. Specifically, a synthetic technique is developed and new 1D [DMPZ]SbCl5 center dot H2O (DP-SbCl5) is sliced to 0D [DMPZ](2)SbCl6 center dot Cl center dot (H2O)(2) (DP-SbCl6) with crystal dimensional reduction from infinite [SbCl5](2-) chain to discrete [SbCl6](3-) octahedron. Comparing with nonluminescent 1D DP-SbCl5, 0D DP-SbCl6 displays highly efficient broadband yellow light emission with enhanced PLQY up to 75.94%. First-principles calculation demonstrates that 0D DP-SbCl6 features more flat and narrow band structure, which promotes the photoelectron localization and increases the quantum confinement, and finally boosts the luminescence efficiency. Together highly efficient and ultra-stable luminescence performance enable DP-SbCl6 as excellent down-conversion broadband yellow phosphor to successfully fabricate white light emitting diodes with a high color rendering index of 92. This work provides a novel structural modulation strategy of crystal dimensional reduction to rationally optimize the PL performance of hybrid metal halides.

Automated summary

This study introduces a crystal dimensional reduction strategy to enhance the photoluminescence quantum yield of hybrid antimony halide, resulting in efficient broadband yellow light emission and the development of white light-emitting diodes with a high color rendering index. The reduction in crystal dimensions creates a more flat and narrow band structure which improves photoelectron localization and increases luminescence efficiency. Such structural modulation strategy provides a novel approach to optimize the photoluminescence performance of hybrid metal halides.