[2205.10545] What Happens at Surfaces and Grain Boundaries of Halide Perovskites: Insights from Reactive Molecular Dynamics Simulations of CsPbI$_{3}$ Skip to main content Search Submit Donate Log in Search arXiv Press Enter to search · Advanced search Condensed Matter > Materials Science arXiv:2205.10545 (cond-mat) [Submitted on 21 May 2022 ( v1 ), last revised 29 Aug 2022 (this version, v2)] Title: What Happens at Surfaces and Grain Boundaries of Halide Perovskites: Insights from Reactive Molecular Dynamics Simulations of CsPbI$_{3}$ Authors: Mike Pols , Tobias Hilpert , Ivo Filot , Adri C.T. van Duin , Sofía Calero , Shuxia Tao View a PDF of the paper titled What Happens at Surfaces and Grain Boundaries of Halide Perovskites: Insights from Reactive Molecular Dynamics Simulations of CsPbI$_{3}$, by Mike Pols and 4 other authors View PDF HTML (experimental) Abstract: The commercialization of perovskite solar cells is hindered by the poor long-term stability of the metal halide perovskite (MHP) light absorbing layer. Solution processing, the common fabrication method for MHPs, produces polycrystalline films with a wide variety of defects, such as point defects, surfaces, and grain boundaries. Although the optoelectronic effects of such defects have been widely studied, the evaluation of their impact on the long-term stability remains challenging. In particular, an understanding of the dynamics of degradation reactions at the atomistic scale is lacking. In this work, using reactive force field (ReaxFF) molecular dynamics simulations, we investigate the effects of defects, in the forms of surfaces, surface defects and grain boundaries, on the stability of the inorganic halide perovskite CsPbI$_{3}$. Our simulations establish a stability trend for a variety of surfaces, which correlates well with the occurrence of these surfaces in experiments. We find that a perovskite surface degrades by progressively changing the local geometry of PbI$_{\mathrm{x}}$ octahedra from corner- to edge- to face-sharing. Importantly, we find that Pb dangling bonds and the lack of steric hindrance of I species are two crucial factors that induce degradation reactions. Finally, we show that the stability of these surfaces can be modulated by adjusting their atomistic details, either by creating additional point defects or merging them to form grain boundaries. While in general additional defects, particularly when clustered, have a negative impact on the material stability, some grain boundaries have a stabilizing effect, primarily because of the additional steric hindrance. Comments: 29 pages, 7 figures Subjects: Materials Science (cond-mat.mtrl-sci) Cite as: arXiv:2205.10545 [cond-mat.mtrl-sci] (or arXiv:2205.10545v2 [cond-mat.mtrl-sci] for this version) https://doi.org/10.48550/arXiv.2205.10545 Focus to learn more arXiv-issued DOI via DataCite Journal reference: ACS Appl. Mater. Interfaces 2022, 14, 36, 40841-40850 Related DOI : https://doi.org/10.1021/acsami.2c09239 Focus to learn more DOI(s) linking to related resources Submission history From: Mike Pols [ view email ] [v1] Sat, 21 May 2022 09:43:40 UTC (32,965 KB) [v2] Mon, 29 Aug 2022 22:17:33 UTC (40,207 KB) Full-text links: Access Paper: View a PDF of the paper titled What Happens at Surfaces and Grain Boundaries of Halide Perovskites: Insights from Reactive Molecular Dynamics Simulations of CsPbI$_{3}$, by Mike Pols and 4 other authors View PDF HTML (experimental) TeX Source view license Current browse context: cond-mat.mtrl-sci < prev | next > new | recent | 2022-05 Change to browse by: cond-mat References & Citations NASA ADS Google Scholar Semantic Scholar export BibTeX citation Loading... BibTeX formatted citation × loading... 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