Accurate and efficient band gap predictions of metal halide perovskites using the DFT-1/2 method: GW accuracy with DFT expense

Abstract

The outstanding optoelectronics and photovoltaic properties of metal halide perovskites, including high carrier motilities, low carrier recombination rates, and the tunable spectral absorption range are attributed to the unique electronic properties of these materials. While DFT provides reliable structures and stabilities of perovskites, it performs poorly in electronic structure prediction. The relativistic GW approximation has been demonstrated to be able to capture electronic structure accurately, but at an extremely high computational cost. Here we report efficient and accurate band gap calculations of halide metal perovskites by using the approximate quasiparticle DFT-1/2 method. Using AMX3 (A = CH3NH3, CH2NHCH2, Cs; M = Pb, Sn, X=I, Br, Cl) as demonstration, the influence of the crystal structure (cubic, tetragonal or orthorhombic), variation of ions (different A, M and X) and relativistic effects on the electronic structure are systematically studied and compared with experimental results. Our results show that the DFT-1/2 method yields accurate band gaps with the precision of the GW method with no more computational cost than standard DFT. This opens the possibility of accurate electronic structure prediction of sophisticated halide perovskite structures and new materials design for lead-free materials.

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• Relativistic Solar Cells
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• Revealing the role of organic cations in hybrid halide perovskites CH3NH3PbI3
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Cited by in corpus (14)

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• Limitations of the DFT-1/2 method for covalent semiconductors and transition-metal oxides
• Excitonic States in Semiconducting Two-dimensional Perovskites
• Transferable classical force field for pure and mixed metal halide perovskites parameterized from first principles
• Defining the Topological Influencers and Predictive Principles to Engineer Band Structure of Halide Perovskites
• Graph Neural Network Architecture Search for Molecular Property Prediction
• Versatile Top-Down Patterning Technique for Perovskite On-Chip Integration
• Effect of the structure of lead iodine perovskites on the photovoltaic efficiencies
• Efficient Computation of Metal Halide Perovskites Properties using the Extended Density Functional Tight Binding: GFN1-xTB Method
• Material gain and eight-band k.p description for selected perovskites
• Theoretical investigation of the role of the organic cation in methylammonium lead iodide perovskite