Resolving Discrepancies in Calculations of Mechanical Properties of CH\textsubscript{3}NH\textsubscript{3}PbI\textsubscript{3} Perovskites

TL;DR

This study clarifies discrepancies in the reported mechanical properties of CH3NH3PbI3 perovskites by systematically analyzing various computational methods and providing accurate reference values for their elastic properties.

Contribution

The paper introduces a comprehensive DFT-based methodology for accurately calculating the elastic properties of all phases of CH3NH3PbI3 perovskites, resolving literature inconsistencies.

Findings

Identified key factors affecting DFT calculations of elastic properties.

Provided consistent reference values for all phases of CH3NH3PbI3.

Established a general methodology for elastic property calculations.

Abstract

The mechanical properties of hybrid perovskite materials are important for device flexibility, resistance to fracture, epitaxial growth, surface energetics of quantum dots, and induction or relief of stress in thin films due to thermal expansion and phase changes. These issues are particularly salient for solar cells in space applications. Nonetheless, few studies are available on the mechanical properties of the paradigmatic hybrid perovskite CH$_3$NH$_3$PbI$_3$ (MAPI). Experimental results are only available for the room-temperature tetragonal phase, and there are significant discrepancies among them. Results from density functional theory (DFT) are available for all three phases but have even larger discrepancies from each other and from experiments. To clarify the disorder in the literature, we have studied the elastic properties of all three phases in detail with DFT calculations. We have examined the effect of different aspects in calculation methodology such as use of energy or stress, the structure, exchange-correlation functionals, Van der Waals corrections, pseudopotentials, $k$-point sampling, and formulas for anisotropic elasticity and polycrystalline averages. Our results provide accurate reference values and an appropriate general methodology for elastic properties of metal halide perovskites.