期刊
CHEMISTRY OF MATERIALS
卷 32, 期 19, 页码 8129-8138出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.0c01255
关键词
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资金
- European Union's Horizon 2020 Research and Innovation Programme under the Marie Skl.odowska-Curie grant [841136]
- HOMING programme of the Foundation for Polish Science - European Union under the European Regional Development Fund [POIR.04.04.00-00-5EE7/18-00]
- Tata Group [UF150033]
- European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (HYPERION) [756962]
- Engineering and Physical Sciences Research Council (EPSRC)
- EPSRC [EP/R023980/1]
- Polish Ministry of Science and Higher Education within the Mobilnosc Plus Program [1603/MOB/V/2017/0]
- National Science Centre [2019/34/A/ST5/00416]
- EPSRC [EP/R023980/1] Funding Source: UKRI
- Marie Curie Actions (MSCA) [841136] Funding Source: Marie Curie Actions (MSCA)
All-inorganic double perovskites (elpasolites) are a promising potential alternatives to lead halide perovskites in optoelectronic applications. Although halide mixing is a well-established strategy for band gap tuning, little is known about halide mixing and phase segregation phenomena in double perovskites. Here, we synthesize a wide range of single- and mixed-halide Cs2AgBiX6 (X = Cl, Br, and I) double perovskites using mechanosynthesis and probe their atomic-level microstructure using Cs-133 solid-state MAS NMR. We show that mixed Cl/Br materials form pure phases for any Cl/Br ratio while Cl/I and Br/I mixing is only possible within a narrow range of halide ratios (<3 mol % I) and leads to a complex mixture of products for higher ratios. We characterize the optical properties of the resulting materials and show that halide mixing does not lead to an appreciable tunability of the PL emission. We find that iodide incorporation is particularly pernicious in that it quenches the PL emission intensity and radiative charge carrier lifetimes for iodide ratios as low as 0.3 mol %. Our study shows that solid-state NMR, in conjunction with optical spectroscopies, provides a comprehensive understanding of the structure-activity relationships, halide mixing, and phase segregation phenomena in Cs2AgBiX6 (X = Cl, Br, and I) double perovskites.
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