Issue 1, 2023

Experimental absence of the non-perovskite ground state phases of MaPbI3 explained by a Funnel Hopping Monte Carlo study based on a neural network potential

Abstract

Methylammonium lead iodide is a material known for its exceptional opto-electronic properties that make it a promising candidate for many high performance applications, such as light emitting diodes or solar cells. A recent computational structure search revealed two previously unknown non-perovskite polymorphs, that are lower in energy than the experimentally observed perovskite phases. To investigate the elusiveness of the non-perovskite phases in experimental studies, we extended our Funnel Hopping Monte Carlo (FHMC) method to periodic systems and performed extensive MC simulations driven by a machine learned potential. FHMC simulations that also include these newly discovered non-perovskite phases show that above temperatures of 200 K the perovskite phases are thermodynamically preferred. A comparison with the quasi-harmonic approximation highlights the importance of anharmonic effects captured by FHMC.

Graphical abstract: Experimental absence of the non-perovskite ground state phases of MaPbI3 explained by a Funnel Hopping Monte Carlo study based on a neural network potential

Supplementary files

Article information

Article type
Paper
Submitted
07 Oct 2022
Accepted
11 Nov 2022
First published
17 Nov 2022
This article is Open Access
Creative Commons BY-NC license

Mater. Adv., 2023,4, 184-194

Experimental absence of the non-perovskite ground state phases of MaPbI3 explained by a Funnel Hopping Monte Carlo study based on a neural network potential

J. A. Finkler and S. Goedecker, Mater. Adv., 2023, 4, 184 DOI: 10.1039/D2MA00958G

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