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Gradient Luminescence Enhancement in Organic Metal Halide Perovskites via the Suppression of SbCln3-n Unit Distortion

Intrinsic stereochemical activity of the 5s2 electron configuration in Sb3+ leads to structural distortion within [SbCln]3-n units, which, while stabilizing the material, paradoxically diminishes luminescence intensity due to induced asymmetry. To address this issue, a strategy, which encompasses in...

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Bibliographic Details
Published in:Inorganic chemistry 2024-12
Main Authors: Zeng, Zixun, Zhang, Guodong, Wang, Yingsheng, Zhang, Min, Tian, Long, Cheng, Ziyong, Lian, Hongzhou, Lin, Jun
Format: Article
Language:English
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Summary:Intrinsic stereochemical activity of the 5s2 electron configuration in Sb3+ leads to structural distortion within [SbCln]3-n units, which, while stabilizing the material, paradoxically diminishes luminescence intensity due to induced asymmetry. To address this issue, a strategy, which encompasses increasing the structural dimensions and introducing In3+ doping, was developed to mitigate the geometrical distortion in the [SbCln]3-n units within the metal-organic perovskite (DABCO)2Sb2Cl10·H2O and (DABCO)2SbCdCl9·2H2O (DABCO = triethylenediamine). This dimensional augmentation confines lattice distortion effectively, and the In3+ doping modifies the 5s2 electron configuration of Sb3+, thereby reducing the distortion at its origin. The unique suitability of indium-based halides as a matrix for Sb3+ doping is underscored by our approach, which capitalizes on their ability to regulate the electron configuration of Sb3+. This strategy has been validated through crystallographic data from single-crystal X-ray diffraction. By effectively reducing the adverse effects of geometric distortion, several hundred-fold enhancements in the luminescent intensity of the material have been achieved by our methodology, leading to potential applications in white-light LEDs. This advancement not only highlights the pivotal role of structural symmetry in the optical properties of materials but also exemplifies the power of material engineering to optimize the optical performance.Intrinsic stereochemical activity of the 5s2 electron configuration in Sb3+ leads to structural distortion within [SbCln]3-n units, which, while stabilizing the material, paradoxically diminishes luminescence intensity due to induced asymmetry. To address this issue, a strategy, which encompasses increasing the structural dimensions and introducing In3+ doping, was developed to mitigate the geometrical distortion in the [SbCln]3-n units within the metal-organic perovskite (DABCO)2Sb2Cl10·H2O and (DABCO)2SbCdCl9·2H2O (DABCO = triethylenediamine). This dimensional augmentation confines lattice distortion effectively, and the In3+ doping modifies the 5s2 electron configuration of Sb3+, thereby reducing the distortion at its origin. The unique suitability of indium-based halides as a matrix for Sb3+ doping is underscored by our approach, which capitalizes on their ability to regulate the electron configuration of Sb3+. This strategy has been validated through crystallographic data from single-crystal X-ray di
ISSN:1520-510X
1520-510X
DOI:10.1021/acs.inorgchem.4c04270