Methylammonium Governs Structural and Optical Properties of Hybrid Lead Halide Perovskites through Dynamic Hydrogen Bonding

Gabriele Saleh, Giulia Biffi, Francesco Di Stasio, Beatriz Martín-Garciá, Ahmed L. Abdelhady, Liberato Manna, Roman Krahne, Sergey Artyukhin

Research output: Contribution to journalArticlepeer-review

14 Scopus citations

Abstract

Methylammonium lead halide perovskites have emerged as ideal materials for photovoltaics and other optoelectronic applications. Their optimal properties stem from complex mechanisms at an atomic level. In these structures, methylammonium molecules undergo continuous temperature-induced reorientations. The underlying atomistic mechanism of this phenomenon and its effect on the material properties are unexplored in many aspects. Here, we address this issue through extensive first-principles and force-field calculations. We show that the interplay between thermal energy and the energetics of molecular orientations fully explains the orthorhombic-tetragonal-cubic phase transitions of the material. The close links among methylammonium orientations, electronic structures, and optical properties are identified. Hydrogen bonding between organic and inorganic sublattices is demonstrated to be the key player in these relationships. We validate our findings against temperature-dependent one-photon and two-photon photoluminescence spectra of CH3NH3PbBr3 and results from the literature. The gained insights can explain the diversity of spectral features observed in the experimental data.

Original languageBritish English
Pages (from-to)8524-8533
Number of pages10
JournalChemistry of Materials
Volume33
Issue number21
DOIs
StatePublished - 9 Nov 2021

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