期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 31, 页码 12369-12379出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c06403
关键词
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资金
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy [EXC 2089/1-390776260]
- Leibniz Supercomputing Centre of the Bavarian Academy of Sciences and Humanities
- Solar Technologies go Hybrid (SolTech) - Bavarian Ministry of Science and Art
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division
- China Scholarship Council
- Consortium des Equipements de Calcul Intensif (CECI) - Fonds de la Recherche Scientifique de Belgique (F.R.S.-FNRS) [2.5020.11]
- Walloon Region
The emergence of halide double perovskites has opened up new possibilities for lead-free and stable photovoltaic absorbers. However, most halide double perovskites possess large band gaps or transitions that are not ideal for solar cell applications. By designing and screening pnictogen-based quaternary antiperovskites, researchers have identified five stable compounds with promising properties for photovoltaic applications, showing potential for efficiencies exceeding 29%, comparable to or higher than lead-based perovskites.
The emergence of halide double perovskites significantly increases the compositional space for lead-free and air-stable photovoltaic absorbers compared to halide perovskites. Nevertheless, most halide double perovskites exhibit oversized band gaps (>1.9 eV) or dipole-forbidden optical transition, which are unfavorable for efficient single-junction solar cell applications. The current device performance of halide double perovskite is still inferior to that of lead-based halide perovskites, such as CH3NH3PbI3 (MAPbI(3)). Here, by ion type inversion and anion ordering on perovskite lattice sites, two new classes of pnictogen-based quaternary antiperovskites with the formula of X(6)B(2)AA' and X6BB'A(2) are designed. Phase stability and tunable band gaps in these quaternary antiperovskites are demonstrated based on first-principles calculations. Further photovoltaic-functionality-directed screening of these materials leads to the discovery of 5 stable compounds (Ca6N2AsSb, Ca6N2PSb, Sr6N2AsSb, Sr6N2PSb, and Ca6NPSb2) with suitable direct band gaps, small carrier effective masses and low exciton binding energies, and dipole-allowed strong optical absorption, which are favorable properties for a photovoltaic absorber material. The calculated theoretical maximum solar cell efficiencies based on these five compounds are all larger than 29%, comparable to or even higher than that of the MAPbI(3) based solar cell. Our work reveals the huge potential of quaternary antiperovskites in the optoelectronic field and provides a new strategy to design lead-free and air-stable perovskite-based photovoltaic absorber materials.
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