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Unraveling the Ordered Phase of the Quintessential Hybrid Perovskite MAPbI(3)—Thermophysics to the Rescue

[Image: see text] Hybrid perovskites continue to attract an enormous amount of attention, yet a robust microscopic picture of their different phases as well as the extent and nature of the disorder present remains elusive. Using specific-heat data along with high-resolution inelastic neutron scatter...

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Autores principales: Marín-Villa, Pelayo, Arauzo, Ana, Drużbicki, Kacper, Fernandez-Alonso, Felix
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9486940/
https://www.ncbi.nlm.nih.gov/pubmed/36069450
http://dx.doi.org/10.1021/acs.jpclett.2c02208
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author Marín-Villa, Pelayo
Arauzo, Ana
Drużbicki, Kacper
Fernandez-Alonso, Felix
author_facet Marín-Villa, Pelayo
Arauzo, Ana
Drużbicki, Kacper
Fernandez-Alonso, Felix
author_sort Marín-Villa, Pelayo
collection PubMed
description [Image: see text] Hybrid perovskites continue to attract an enormous amount of attention, yet a robust microscopic picture of their different phases as well as the extent and nature of the disorder present remains elusive. Using specific-heat data along with high-resolution inelastic neutron scattering and ab initio modeling, we address this ongoing challenge for the case of the ordered phase of the quintessential hybrid-perovskite MAPbI(3). At low temperatures, the specific heat of MAPbI(3) reveals strong deviations from the Debye limit, a common feature of pure hybrid perovskites and their mixtures. Our thermophysical analysis demonstrates that the (otherwise ordered) structure around the organic moiety is characterized by a substantial lowering of the local symmetry relative to what can be inferred from crystallographic studies. The physical origin of the observed thermophysical anomalies is unequivocally linked to excitations of sub-terahertz optical phonons responsible for translational–librational distortions of the octahedral units.
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spelling pubmed-94869402022-09-21 Unraveling the Ordered Phase of the Quintessential Hybrid Perovskite MAPbI(3)—Thermophysics to the Rescue Marín-Villa, Pelayo Arauzo, Ana Drużbicki, Kacper Fernandez-Alonso, Felix J Phys Chem Lett [Image: see text] Hybrid perovskites continue to attract an enormous amount of attention, yet a robust microscopic picture of their different phases as well as the extent and nature of the disorder present remains elusive. Using specific-heat data along with high-resolution inelastic neutron scattering and ab initio modeling, we address this ongoing challenge for the case of the ordered phase of the quintessential hybrid-perovskite MAPbI(3). At low temperatures, the specific heat of MAPbI(3) reveals strong deviations from the Debye limit, a common feature of pure hybrid perovskites and their mixtures. Our thermophysical analysis demonstrates that the (otherwise ordered) structure around the organic moiety is characterized by a substantial lowering of the local symmetry relative to what can be inferred from crystallographic studies. The physical origin of the observed thermophysical anomalies is unequivocally linked to excitations of sub-terahertz optical phonons responsible for translational–librational distortions of the octahedral units. American Chemical Society 2022-09-07 2022-09-15 /pmc/articles/PMC9486940/ /pubmed/36069450 http://dx.doi.org/10.1021/acs.jpclett.2c02208 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Marín-Villa, Pelayo
Arauzo, Ana
Drużbicki, Kacper
Fernandez-Alonso, Felix
Unraveling the Ordered Phase of the Quintessential Hybrid Perovskite MAPbI(3)—Thermophysics to the Rescue
title Unraveling the Ordered Phase of the Quintessential Hybrid Perovskite MAPbI(3)—Thermophysics to the Rescue
title_full Unraveling the Ordered Phase of the Quintessential Hybrid Perovskite MAPbI(3)—Thermophysics to the Rescue
title_fullStr Unraveling the Ordered Phase of the Quintessential Hybrid Perovskite MAPbI(3)—Thermophysics to the Rescue
title_full_unstemmed Unraveling the Ordered Phase of the Quintessential Hybrid Perovskite MAPbI(3)—Thermophysics to the Rescue
title_short Unraveling the Ordered Phase of the Quintessential Hybrid Perovskite MAPbI(3)—Thermophysics to the Rescue
title_sort unraveling the ordered phase of the quintessential hybrid perovskite mapbi(3)—thermophysics to the rescue
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9486940/
https://www.ncbi.nlm.nih.gov/pubmed/36069450
http://dx.doi.org/10.1021/acs.jpclett.2c02208
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