Room-temperature dynamic correlation between methylammonium molecules in lead-iodine based perovskites: An ab initio molecular dynamics perspective

Jonathan Lahnsteiner, Georg Kresse, Abhinav Kumar, D. D. Sarma, Cesare Franchini, Menno Bokdam*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

46 Citations (Scopus)

Abstract

The high efficiency of lead organo-metal-halide perovskite solar cells has raised many questions about the role of the methylammonium (MA) molecules in the Pb-I framework. Experiments indicate that the MA molecules are able to "freely" spin around at room temperature even though they carry an intrinsic dipole moment. We have performed large supercell (2592 atoms) finite-temperature ab initio molecular dynamics calculations to study the correlation between the molecules in the framework. An underlying long-range antiferroelectric ordering of the molecular dipoles is observed. The dynamical correlation between neighboring molecules shows a maximum around room temperature in the mid-temperature phase. In this phase, the rotations are slow enough to (partially) couple to neighbors via the Pb-I cage. This results in a collective motion of neighboring molecules in which the cage acts as the mediator. At lower and higher temperatures, the motions are less correlated.

Original languageEnglish
Article number214114
JournalPhysical Review B
Volume94
Issue number21
DOIs
Publication statusPublished - 28 Dec 2016
Externally publishedYes

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