Nonequilibrium Lattice Dynamics in Photoexcited 2D Perovskites
© 2022 UChicago Argonne, LLC, Operation of Argonne National Laboratory and The Authors. Advanced Materials published by Wiley-VCH GmbH.
Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 44 vom: 03. Nov., Seite e2202709 |
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Weitere Verfasser: | , , , , , , , , , , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2022
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Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
Schlagworte: | Journal Article lead halide perovskites optical excitation transient structures |
Zusammenfassung: | © 2022 UChicago Argonne, LLC, Operation of Argonne National Laboratory and The Authors. Advanced Materials published by Wiley-VCH GmbH. Interplay between structural and photophysical properties of metal halide perovskites is critical to their utility in optoelectronics, but there is limited understanding of lattice response upon photoexcitation. Here, 2D perovskites butylammonium lead iodide, (BA)2 PbI4 , and phenethylammonium lead iodide, (PEA)2 PbI4 , are investigated using ultrafast transient X-ray diffraction as a function of optical excitation fluence to discern structural dynamics. Both powder X-ray diffraction and time-resolved photoluminescence linewidths narrow over 1 ns following optical excitation for the fluence range studied, concurrent with slight redshifting of the optical bandgaps. These observations are attributed to transient relaxation and ordering of distorted lead iodide octahedra stimulated mainly by electron-hole pair creation. The c axis expands up to 0.37% over hundreds of picoseconds; reflections sampling the a and b axes undergo one tenth of this expansion with the same timescale. Post-photoexcitation appearance of the (110) reflection in (BA)2 PbI4 would suggest a transient phase transition, however, through new single-crystal XRD, reflections are found that violate glide plane conditions in the reported Pbca structure. The static structure space group is reassigned as P21 21 21 . With this, a nonequilibrium phase transition is ruled out. These findings offer increased understanding of remarkable lattice response in 2D perovskites upon excitation |
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Beschreibung: | Date Revised 04.11.2022 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.202202709 |