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The Journal of Physical Chemistry C
Article . 2023 . Peer-reviewed
License: CC BY
Data sources: Crossref
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https://dx.doi.org/10.48550/ar...
Article . 2023
License: arXiv Non-Exclusive Distribution
Data sources: Datacite
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Phase Transitions in Inorganic Halide Perovskites from Machine-Learned Potentials

Authors: Erik Fransson; Julia Wiktor; Paul Erhart;

Phase Transitions in Inorganic Halide Perovskites from Machine-Learned Potentials

Abstract

The atomic scale dynamics of halide perovskites have a direct impact not only on their thermal stability but their optoelectronic properties. Progress in machine learned potentials has only recently enabled modeling the finite temperature behavior of these material using fully atomistic methods with near first-principles accuracy. Here, we systematically analyze the impact of heating and cooling rate, simulation size, model uncertainty, and the role of the underlying exchange-correlation functional on the phase behavior of CsPbX3 with X=Cl, Br, and I, including both the perovskite and the delta-phases. We show that rates below approximately 30 K/ns and system sizes of at least a few ten thousand atoms are indicated to achieve convergence with regard to these parameters. By controlling these factors and constructing models that are specific for different exchange-correlation functionals we then show that the semi-local functionals considered in this work (SCAN, vdW-DF-cx, PBEsol, and PBE) systematically underestimate the transition temperatures separating the perovskite phases while overestimating the lattice parameters. Among the considered functionals the vdW-DF-cx functional yields the closest agreement with experiment, followed by SCAN, PBEsol, and PBE. Our work provides guidelines for the systematic analysis of dynamics and phase transitions in inorganic halide perovskites and similar systems. It also serves as a benchmark for the further development of machine-learned potentials as well as exchange-correlation functionals.

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Keywords

Condensed Matter - Materials Science, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences, Computational Physics (physics.comp-ph), Physics - Computational Physics

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selected citations
These citations are derived from selected sources.
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
46
Top 1%
Top 10%
Top 1%
Green
hybrid