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Unexpected bowing band evolution in an all-inorganic CsSn1−xPbxBr3 perovskite†
Yufan Xia,Tian Luo,Hongyao Liang,Yujia Gao,Xin Xu,Weiguang Xie,Pengyi Liu,Xin Wang,Yu-Jun Zhao,Tingting Shi
RSC Advances Pub Date : 07/14/2020 00:00:00 , DOI:10.1039/D0RA03709E
Abstract

We theoretically investigated the structural and electronic properties of the all-inorganic perovskite CsSn1−xPbxBr3, compared with the mixed perovskite compound MAyCs1−ySn1−xPbxBr3, based on first-principle calculations. It has been demonstrated that Pb and Sn atoms are inclined to occupy the lattice sites uniformly in the all-inorganic perovskite, and this is distinguished from the most stable configurations observed in the mixed Cs-MA system. It is interesting that small Sn atoms prefer to stay close to the large MA+ cations, leading to smaller local structural distortion. Through spin-orbital coupling calculations, we found non-linear bowing band evolution in the all-inorganic mixed Sn–Pb system with a small bowing parameter (b = 0.35), while the band gap of MAyCs1−ySn1−xPbxBr3 was clearly reduced as the ratio of MA was around 0.5 (y ≥ 0.25). We determined the bowing band evolution in the mixed cation perovskites and the intrinsic electronic deficiency of the all-inorganic perovskite to obtain the optimal band gap.

Graphical abstract: Unexpected bowing band evolution in an all-inorganic CsSn1−xPbxBr3 perovskite
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