Temperature and volumetric effects on structural and dielectric properties of hybrid perovskites

Andrzej Nowok (), Szymon Sobczak, Kinga Roszak, Anna Z. Szeremeta, Mirosław Mączka, Andrzej Katrusiak (), Sebastian Pawlus, Filip Formalik, Antonio José Barros dos Santos, Waldeci Paraguassu and Adam Sieradzki ()
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Andrzej Nowok: Université Toulouse, INSA-T
Szymon Sobczak: Adam Mickiewicz University, Poznań
Kinga Roszak: Adam Mickiewicz University, Poznań
Anna Z. Szeremeta: University of Silesia in Katowice
Mirosław Mączka: Polish Academy of Sciences
Andrzej Katrusiak: Adam Mickiewicz University, Poznań
Sebastian Pawlus: University of Silesia in Katowice
Filip Formalik: Northwestern University
Antonio José Barros dos Santos: Universidade Federal do Para
Waldeci Paraguassu: Universidade Federal do Para
Adam Sieradzki: Wrocław University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Three-dimensional organic-inorganic perovskites are rapidly evolving materials with diverse applications. This study focuses on their two representatives - acetamidinium manganese(II) formate (AceMn) and formamidinium manganese(II) formate (FMDMn) – subjected to varying temperature and pressure. We show that AceMn undergoes atypical pressure-induced structural transformations at room temperature, increasing the symmetry from ambient-pressure P21/n phase II to the high-pressure Pbca phase III. In turn, FMDMn in its C2/c phase II displays temperature- and pressure-induced ordering of cage cations that proceeds without changing the phase symmetry or energy barriers. The FMD+ cations do not order under constant volume across the pressure-temperature plane, despite similar pressure and temperature evolution of the unit-cell parameters. Temperature and pressure affect the cage cations differently, which is particularly pronounced in their relaxation dynamics seen by dielectric spectroscopy. Their motion require a rearrangement of the metal-formate framework, resulting in the energy and volumetric barriers defined by temperature-independent activation energy and activation volume parameters. As this process is phonon-assisted, the relaxation time is strongly temperature-dependent. Consequently, relaxation times do not scale with unit-cell volume nor H-bond lengths in formates, offering the possibility of tuning their electronic properties by external stimuli (like temperature or pressure) even without any structural changes.

Date: 2024
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DOI: 10.1038/s41467-024-51396-5

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