Methylammonium Lead Iodide across Physical Space: Phase Boundaries and Structural Collapse

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL
Pelayo Marin-Villa, Mattia Gaboardi, Boby Joseph, Frederico Alabarse, Jeff Armstrong, Kacper Drużbicki, Felix Fernandez-Alonso
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引用次数: 0

Abstract

Hybrid perovskites exhibit complex structures and phase behavior under different thermodynamic conditions and chemical environments, the understanding of which continues to be pivotally important for tailoring their properties toward improved operational stability. To this end, we present for the first time a comprehensive neutron and synchrotron diffraction investigation over the pressure–temperature phase diagram of the paradigmatic hybrid organic–inorganic perovskite methylammonium lead iodide (MAPbI3). This ambitious experimental campaign down to cryogenic temperatures and tens of kilobars was supported by extensive ab initio molecular dynamics simulations validated by the experimental data, to track the structural evolution of MAPbI3 under external physical stimuli at the atomic and molecular levels. These combined efforts enable us to identify the mechanisms underpinning structural phase transitions, including those exhibiting negative thermal expansion across the boundary between the cation-ordered low-temperature phase and the dynamically disordered high-pressure cubic phase. Our results bring to the fore how pronounced octahedral distortions at high pressures ultimately drive the structural collapse and amorphization of this material.

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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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