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The effect of organic cation dynamics on the optical properties in (PEA)2(MA)[Pb2I7] perovskite dimorphs
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Lekina, Yulia, Dintakurti, Sai S. H., Febriansyah, Benny, Bradley, D., Yan, Jiaxu, Shi, Xiangyan, England, Jason, White, Tim, Hanna, John V. and Shen, Ze Xiang (2021) The effect of organic cation dynamics on the optical properties in (PEA)2(MA)[Pb2I7] perovskite dimorphs. Journal of Materials Chemistry C, 9 (47). pp. 17050-17060. doi:10.1039/d1tc04181a ISSN 2050-7526.
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WRAP-Effect-organic-cation-dynamics-optical-properties-perovskite-dimorphs-2021.pdf - Accepted Version - Requires a PDF viewer. Download (2378Kb) | Preview |
Official URL: https://doi.org/10.1039/d1tc04181a
Abstract
Two-dimensional (2D) phenylethyl ammonium (PEA+)-methyl ammonium (MA+) lead iodide ((PEA)2(MA)[Pb2I7]) hybrid perovskite exists as temperature-dependent dimorphs exhibiting an ill-defined phase transition occurring over the 150–200 K range. Raman scattering, photoluminescence, optical absorbance and solid state MAS NMR spectroscopic methods are employed to investigate the structural complexity, disorder and structure/function of this system. The Raman and 1H MAS NMR data indicate that the lower bounds of the phase transition at ∼150 K are characterised by attenuated rotational modes and slower motional dynamics throughout the disordered MA+ organic sublattice, inducing a strengthening of the MA+⋯I hydrogen bonds and a 5 meV increase in the excitonic and photoluminescence energies. It is evident that different recombination mechanisms are dominant for the room temperature and low temperature phases reflecting the importance of MA+ dynamics in the optical properties of the material. Single crystal X-ray studies are unable to position the organic cations within the Pb2I7 framework; however, 1H/13C MAS NMR measurements describe elements of local structural disorder based on conformational isomerism within the PEA+ sublattice. Concomitant I− and Pb2+ migration and [Pb2I7]3− framework defects create stacking disorder, dislocations and dispersed octahedral tilting leading to additional disorder and distributed MA+ and PEA+ cation dynamics.
| Item Type: | Journal Article | ||||||||||||
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| Subjects: | Q Science > QC Physics Q Science > QD Chemistry Q Science > QE Geology |
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| Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||||||||||
| SWORD Depositor: | Library Publications Router | ||||||||||||
| Library of Congress Subject Headings (LCSH): | Perovskite (Mineral), Perovskite (Mineral) -- Optical properties, Raman effect, Photoluminescence , Light absorption , Nuclear magnetic resonance spectroscopy | ||||||||||||
| Journal or Publication Title: | Journal of Materials Chemistry C | ||||||||||||
| Publisher: | Royal Society of Chemistry | ||||||||||||
| ISSN: | 2050-7526 | ||||||||||||
| Official Date: | 21 December 2021 | ||||||||||||
| Dates: |
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| Volume: | 9 | ||||||||||||
| Number: | 47 | ||||||||||||
| Page Range: | pp. 17050-17060 | ||||||||||||
| DOI: | 10.1039/d1tc04181a | ||||||||||||
| Status: | Peer Reviewed | ||||||||||||
| Publication Status: | Published | ||||||||||||
| Access rights to Published version: | Restricted or Subscription Access | ||||||||||||
| Date of first compliant deposit: | 18 January 2022 | ||||||||||||
| Date of first compliant Open Access: | 12 November 2022 | ||||||||||||
| RIOXX Funder/Project Grant: |
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