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

• Published in: Advanced optical materials Vol. 9; no. 19
• Main Authors: Zhao, Jian‐Qiang, Han, Meng‐Fei, Zhao, Xue‐Jie, Ma, Yue‐Yu, Jing, Chang‐Qing, Pan, Hong‐Mei, Li, Dong‐Yang, Yue, Cheng‐Yang, Lei, Xiao‐Wu
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 01-10-2021
• Subjects: 0D hybrid metal halides; Antimony; Broadband; crystal dimensionality; Crystal structure; Halides; Light emission; Light emitting diodes; low‐dimensional halide perovskites; Luminescence; Materials science; Metal halides; Modulation; Optics; Optimization; Phosphors; Photoelectrons; Photoluminescence; photoluminescence efficiency; Quantum confinement; structural design; White light; white light emitting diodes
• ISSN: 2195-1071; 2195-1071
• DOI: 10.1002/adom.202100556

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 ∙ H2O (DP‐SbCl5) is sliced to 0D [DMPZ]2SbCl6 ∙ Cl ∙ (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.
With controllable structural evolution from 1D to 0D hybrid antimony halides, the photoluminescence quantum yield (PLQY) realizes a notable enhancement from <1% to 75.94% in yellow spectral region benefitting from more localized photoelectrons and increased quantum confinement. This work provides a structural platform to verify the feasibility of crystal dimensionality reduction strategy to rationally improve the PLQY of metal halides.