Revealing the stability and efficiency enhancement in mixed halide perovskites MAPb(I${}_{1-x}$Cl${}_x$)${}_3$ with ab initio calculations

Abstract

A little addition of Cl to \ce{MAPbI3} has been reported to improve the material stability as well as light harvesting and carrier conducting properties of organometal trihalide perovskites, the key component of perovskite solar cell (PSC). However, the mechanism of performance enhancement of PSC by Cl addition is still unclear. Here, we apply the efficient virtual crystal approximation method to revealing the effects of Cl addition on the structural, electronic, optical properties and material stability of \ce{MAPb(I_{1-x}Cl_x)3}. Our {\it ab initio} calculations present that as the increase of Cl content cubic lattice constants and static dielectric constants decrease linearly, while band gaps and exciton binding energies increase quadratically. Moreover, we find the minimum of exciton binding energy at the Cl content of 7\%, at which the chemical decomposition reaction changes coincidentally to be from exothermic to endothermic. Interactions among constituents of compound and electronic charge transferring during formation are carefully discussed. This reveals new prospects for understanding and designing of stable, high efficiency PSCs.

References in corpus (5)

• Direct Measurement of the Exciton Binding Energy and Effective Masses for Charge carriers in an Organic-Inorganic Tri-halide Perovskite
• Revealing the role of organic cations in hybrid halide perovskites CH3NH3PbI3
• Intrinsic Instability of the Hybrid Halide Perovskite Semiconductor CH3NH3PbI3
• Influence of halide composition on the structural, electronic, and optical properties of mixed CH${}_3$NH${}_3$Pb(I${}_{1-x}$Br${}_x$)${}_3$ perovskites calculated using the virtual crystal approximation method
• Electronic structure and photo absorption property of pseudo-cubic perovskites CH${}_3$NH${}_3$PbX${}_3$ (X=I, Br) including van der Waals interaction

Cited by in corpus (4)

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• First-Principles Study on Material Properties and Stability of Inorganic Halide Perovskite Solid Solutions CsPb(I${}_{1-x}$Br${}_x$)${}_3$ towards High Performance Perovskite Solar Cells
• Determining Exciton Binding Energy and Reduced Effective Mass in Metal Tri-Halide Perovskites from Optical and Impedance Spectroscopy Measurements
• Computational Prediction of Structural, Electronic, Optical Properties and Phase Stability of Double Perovskites K2SnX6 (X = I, Br, Cl)