Finite-temperature structure of the MAPbI3 perovskite: Comparing density functional approximations and force fields to experiment

Jonathan Lahnsteiner*, Georg Kresse, Jurn Heinen, Menno Bokdam*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

20 Citations (Scopus)

Abstract

Determining the finite-temperature structure of the hybrid perovskite MAPbI3 is a challenge for both experimental and theoretical methods. A very powerful computational method that can resolve the atomic structure is molecular dynamics (MD). The resulting structure depends on the density functional approximation (DFA) in the case of ab initio MD and the force field in classical MD. We compare the structure between 250 and 400 K obtained with different DFAs and force fields in one consistent manner. The symmetry of the PbI3 framework is analyzed as well as the relative ordering of the neighboring organic molecules inside the framework. The distribution function of the molecules is used to map out an effective energy surface for the rotation of a single molecule. This surface is accurately modeled by a pair of cubic harmonics. Available experimental data in literature are discussed and compared to the structure obtained with the different methods. The spread in these data is still too large to uniquely determine the method that "best" describes the perovskite, however, promising candidates and outliers have been identified.

Original languageEnglish
Article number073604
JournalPhysical Review Materials
Volume2
Issue number7
DOIs
Publication statusPublished - 16 Jul 2018
Externally publishedYes

Fingerprint

Dive into the research topics of 'Finite-temperature structure of the MAPbI3 perovskite: Comparing density functional approximations and force fields to experiment'. Together they form a unique fingerprint.

Cite this