Thermodynamic Origin of the Photostability of the Two-Dimensional Perovskite PEA2Pb(I1-xBrx)4

Zehua Chen; Haibo Xue; Geert Brocks; Peter A. Bobbert; Shuxia Tao

doi:10.1021/acsenergylett.2c02463

Thermodynamic Origin of the Photostability of the Two-Dimensional Perovskite PEA₂Pb(I_1-xBr_x)₄

Zehua Chen, Haibo Xue, Geert Brocks, Peter A. Bobbert^*, Shuxia Tao

^*Corresponding author for this work

Research output: Contribution to journal › Article › Academic › peer-review

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Abstract

The two-dimensional (2D) mixed halide perovskite PEA₂Pb(I_1-xBr_x)₄ exhibits high phase stability under illumination as compared to the three-dimensional (3D) counterpart MAPb(I_1-xBr_x)₃. We explain this difference using a thermodynamic theory that considers the sum of a compositional and a photocarrier free energy. Ab initio calculations show that the improved compositional phase stability of the 2D perovskite is caused by a preferred I-Br distribution, leading to a much lower critical temperature for halide segregation in the dark than for the 3D perovskite. Moreover, a smaller increase of the band gap with Br concentration x and a markedly shorter photocarrier lifetime in the 2D perovskite reduce the driving force for phase segregation under illumination, enhancing the photostability.

Original language	English
Pages (from-to)	943-949
Number of pages	7
Journal	ACS Energy Letters
Volume	8
Issue number	2
Early online date	12 Jan 2023
DOIs	https://doi.org/10.1021/acsenergylett.2c02463
Publication status	Published - 10 Feb 2023

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title = "Thermodynamic Origin of the Photostability of the Two-Dimensional Perovskite PEA2Pb(I1-xBrx)4",

abstract = "The two-dimensional (2D) mixed halide perovskite PEA2Pb(I1-xBrx)4 exhibits high phase stability under illumination as compared to the three-dimensional (3D) counterpart MAPb(I1-xBrx)3. We explain this difference using a thermodynamic theory that considers the sum of a compositional and a photocarrier free energy. Ab initio calculations show that the improved compositional phase stability of the 2D perovskite is caused by a preferred I-Br distribution, leading to a much lower critical temperature for halide segregation in the dark than for the 3D perovskite. Moreover, a smaller increase of the band gap with Br concentration x and a markedly shorter photocarrier lifetime in the 2D perovskite reduce the driving force for phase segregation under illumination, enhancing the photostability.",

author = "Zehua Chen and Haibo Xue and Geert Brocks and Bobbert, {Peter A.} and Shuxia Tao",

note = "Funding Information: Z.C. acknowledges funding from the Eindhoven University of Technology. H.X. acknowledges funding from the China Scholarship Council (CSC, No. 201806420038). S.T. acknowledges funding by the Computational Sciences for Energy Research (CSER) tenure track program of Shell and NWO (Project No. 15CST04-2) as well as NWO START-UP from The Netherlands. This work made use of the Dutch national e-infrastructure with the support of the SURF Cooperative (Grant No. EINF-2988). Publisher Copyright: {\textcopyright} 2023 The Authors. Published by American Chemical Society.",

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AU - Bobbert, Peter A.

AU - Tao, Shuxia

N1 - Funding Information: Z.C. acknowledges funding from the Eindhoven University of Technology. H.X. acknowledges funding from the China Scholarship Council (CSC, No. 201806420038). S.T. acknowledges funding by the Computational Sciences for Energy Research (CSER) tenure track program of Shell and NWO (Project No. 15CST04-2) as well as NWO START-UP from The Netherlands. This work made use of the Dutch national e-infrastructure with the support of the SURF Cooperative (Grant No. EINF-2988). Publisher Copyright: © 2023 The Authors. Published by American Chemical Society.

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N2 - The two-dimensional (2D) mixed halide perovskite PEA2Pb(I1-xBrx)4 exhibits high phase stability under illumination as compared to the three-dimensional (3D) counterpart MAPb(I1-xBrx)3. We explain this difference using a thermodynamic theory that considers the sum of a compositional and a photocarrier free energy. Ab initio calculations show that the improved compositional phase stability of the 2D perovskite is caused by a preferred I-Br distribution, leading to a much lower critical temperature for halide segregation in the dark than for the 3D perovskite. Moreover, a smaller increase of the band gap with Br concentration x and a markedly shorter photocarrier lifetime in the 2D perovskite reduce the driving force for phase segregation under illumination, enhancing the photostability.

AB - The two-dimensional (2D) mixed halide perovskite PEA2Pb(I1-xBrx)4 exhibits high phase stability under illumination as compared to the three-dimensional (3D) counterpart MAPb(I1-xBrx)3. We explain this difference using a thermodynamic theory that considers the sum of a compositional and a photocarrier free energy. Ab initio calculations show that the improved compositional phase stability of the 2D perovskite is caused by a preferred I-Br distribution, leading to a much lower critical temperature for halide segregation in the dark than for the 3D perovskite. Moreover, a smaller increase of the band gap with Br concentration x and a markedly shorter photocarrier lifetime in the 2D perovskite reduce the driving force for phase segregation under illumination, enhancing the photostability.

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Thermodynamic Origin of the Photostability of the Two-Dimensional Perovskite PEA₂Pb(I_1-xBr_x)₄

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