Elucidating the role of Sn-substitution and Pb-$\square$ in regulating stability and carrier concentration in CH${}_3$NH${}_3$Pb${}_{1-X-Y}$Sn${}_X$${\square }_Y$I${}_3$

Abstract

We address the role of Sn-substitution and Pb-vacancy (Pb-$\square$) in regulating stability and carrier concentration of CH${}_3$NH${}_3$Pb${}_{1-X-Y}$Sn${}_X$${\square }_Y$I${}_3$ perovskite using density functional theory, where the performance of the exchange-correlation functional is carefully analyzed, and validated w.r.t. available experimental results. We find the most stable configuration does not prefer any Pb at 50\% concentration of Sn. However, the Pb-$\square$s become unfavourable above 250K due to the reduced linearity of Sn-I bonds. For n-type host the Sn substitution is more preferable than Pb-$\square$ formation, while for p-type host the trend is exactly opposite. The charge states of both Sn and Pb-$\square$ are found to be dependent on the Sn concentration, which in turn alters the perovskite from n-type to p-type with increasing $X$ ($>$0.5).

5 pages, 4 figures

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