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Liquid-Like Interfaces Mediate Structural Phase Transitions in Lead Halide Perovskites

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Title: Liquid-Like Interfaces Mediate Structural Phase Transitions in Lead Halide Perovskites
Authors: Bischak, Connor G., Lai, Minliang, Lu, Dylan, Fan, Zhaochuan, David, Philippe, Dong, Dengpan, Chen, Hong, Etman, Ahmed S., Lei, Teng, Sun, Junliang, Grünwald, Michael, Limmer, David T., Yang, Peidong, Ginsberg, Naomi S.
Publication Year: 2019
Collection: Condensed Matter
Physics (Other)
Subject Terms: Condensed Matter - Mesoscale and Nanoscale Physics, Condensed Matter - Materials Science, Condensed Matter - Statistical Mechanics, Physics - Applied Physics, Physics - Chemical Physics
More Details: Microscopic pathways of structural phase transitions are difficult to probe because they occur over multiple, disparate time and length scales. Using $in$ $situ$ nanoscale cathodoluminescence microscopy, we visualize the thermally-driven transition to the perovskite phase in hundreds of non-perovskite phase nanowires, resolving the initial nanoscale nucleation and subsequent mesoscale growth and quantifying the activation energy for phase propagation. In combination with molecular dynamics computer simulations, we reveal that the transformation does not follow a simple martensitic mechanism, and proceeds via ion diffusion through a liquid-like interface between the two structures. While cations are disordered in this liquid-like region, the halide ions retain substantial spatial correlations. We find that the anisotropic crystal structure translates to faster nucleation of the perovskite phase at nanowire ends and faster growth along the long nanowire axis. These results represent a significant step towards manipulating structural phases at the nanoscale for designer materials properties.
Comment: 8 pages, 3 figures, ancilliary supplementary information
Document Type: Working Paper
DOI: 10.1016/j.matt.2020.07.015
Access URL: http://arxiv.org/abs/1907.13509
Accession Number: edsarx.1907.13509
Database: arXiv
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  Data: Liquid-Like Interfaces Mediate Structural Phase Transitions in Lead Halide Perovskites
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  Data: <searchLink fieldCode="AR" term="%22Bischak%2C+Connor+G%2E%22">Bischak, Connor G.</searchLink><br /><searchLink fieldCode="AR" term="%22Lai%2C+Minliang%22">Lai, Minliang</searchLink><br /><searchLink fieldCode="AR" term="%22Lu%2C+Dylan%22">Lu, Dylan</searchLink><br /><searchLink fieldCode="AR" term="%22Fan%2C+Zhaochuan%22">Fan, Zhaochuan</searchLink><br /><searchLink fieldCode="AR" term="%22David%2C+Philippe%22">David, Philippe</searchLink><br /><searchLink fieldCode="AR" term="%22Dong%2C+Dengpan%22">Dong, Dengpan</searchLink><br /><searchLink fieldCode="AR" term="%22Chen%2C+Hong%22">Chen, Hong</searchLink><br /><searchLink fieldCode="AR" term="%22Etman%2C+Ahmed+S%2E%22">Etman, Ahmed S.</searchLink><br /><searchLink fieldCode="AR" term="%22Lei%2C+Teng%22">Lei, Teng</searchLink><br /><searchLink fieldCode="AR" term="%22Sun%2C+Junliang%22">Sun, Junliang</searchLink><br /><searchLink fieldCode="AR" term="%22Grünwald%2C+Michael%22">Grünwald, Michael</searchLink><br /><searchLink fieldCode="AR" term="%22Limmer%2C+David+T%2E%22">Limmer, David T.</searchLink><br /><searchLink fieldCode="AR" term="%22Yang%2C+Peidong%22">Yang, Peidong</searchLink><br /><searchLink fieldCode="AR" term="%22Ginsberg%2C+Naomi+S%2E%22">Ginsberg, Naomi S.</searchLink>
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  Data: Microscopic pathways of structural phase transitions are difficult to probe because they occur over multiple, disparate time and length scales. Using $in$ $situ$ nanoscale cathodoluminescence microscopy, we visualize the thermally-driven transition to the perovskite phase in hundreds of non-perovskite phase nanowires, resolving the initial nanoscale nucleation and subsequent mesoscale growth and quantifying the activation energy for phase propagation. In combination with molecular dynamics computer simulations, we reveal that the transformation does not follow a simple martensitic mechanism, and proceeds via ion diffusion through a liquid-like interface between the two structures. While cations are disordered in this liquid-like region, the halide ions retain substantial spatial correlations. We find that the anisotropic crystal structure translates to faster nucleation of the perovskite phase at nanowire ends and faster growth along the long nanowire axis. These results represent a significant step towards manipulating structural phases at the nanoscale for designer materials properties.<br />Comment: 8 pages, 3 figures, ancilliary supplementary information
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