Optoelectronic performance of perovskite Cs 2 KMI 6 (M = Ga, In) based on high-throughput screening and first-principles calculations.

Developing novel lead-free perovskite materials with suitable bandgaps and superior thermal stability is crucial to boost their applications in next-generation photovoltaic technologies. High throughput screening combined with the first principles method can accurately and effectively screen out promising perovskites. Herein, we select two lead-free all-inorganic halide double perovskite materials Cs ₂ KMI ₆ (M = Ga, In) from 1026 compounds with the criteria including appropriate structure factors, positive decomposition energies, and suitable direct bandgaps. We investigated the thermal and mechanical stability, geometric and electronic structures, photoelectric properties, and defect formation energies for both perovskites Cs ₂ KMI ₆ (M = Ga, In). They can exhibit excellent structural formability and stability through the analysis of structure factors, elastic constants, and stable chemical potential regions. In addition, we investigate the defect effects of Cs ₂ KMI ₆ (M = Ga, In) on the photovoltaic performance by evaluating the defect formation energies and transition energy levels. Based on the HSE06 functional, we calculated the energy band structures of these two compounds and demonstrate the direct bandgaps of 1.69 eV (HSE06) and 2.16 eV (HSE06) for Cs ₂ KGaI ₆ and Cs ₂ KInI ₆ , respectively. Moreover, we predicted excellent spectroscopic limited maximum efficiencies (SLMEs) of these two perovskites with high light absorption coefficients (around 10 ⁵ cm ^-1 ), for instance, the SLME of Cs ₂ KGaI ₆ can reach as high as 28.39%.