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Hydroxide films on mica form charge-stabilized microphases that circumvent nucleation barriers

Legg, B.A.; Voïtchovsky, K.; De Yoreo, J.J.

Hydroxide films on mica form charge-stabilized microphases that circumvent nucleation barriers Thumbnail


Authors

B.A. Legg

J.J. De Yoreo



Abstract

Crystal nucleation is facilitated by transient, nanoscale fluctuations that are extraordinarily difficult to observe. Here, we use high-speed atomic force microscopy to directly observe the growth of an aluminum hydroxide film from an aqueous solution and characterize the dynamically fluctuating nanostructures that precede its formation. Nanoscale cluster distributions and fluctuation dynamics show many similarities to the predictions of classical nucleation theory, but the cluster energy landscape deviates from classical expectations. Kinetic Monte Carlo simulations show that these deviations can arise from electrostatic interactions between the clusters and the underlying substrate, which drive microphase separation to create a nanostructured surface phase. This phase can evolve seamlessly from a low-coverage state of fluctuating clusters into a high-coverage nanostructured network, allowing the film to grow without having to overcome classical nucleation barriers.

Citation

Legg, B., Voïtchovsky, K., & De Yoreo, J. (2022). Hydroxide films on mica form charge-stabilized microphases that circumvent nucleation barriers. Science Advances, 8(35), Article eabn7087. https://doi.org/10.1126/sciadv.abn7087

Journal Article Type Article
Acceptance Date Jun 30, 2022
Online Publication Date Sep 2, 2022
Publication Date Sep 2, 2022
Deposit Date Sep 14, 2022
Publicly Available Date Sep 15, 2022
Journal Science Advances
Publisher American Association for the Advancement of Science
Peer Reviewed Peer Reviewed
Volume 8
Issue 35
Article Number eabn7087
DOI https://doi.org/10.1126/sciadv.abn7087

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Publisher Licence URL
http://creativecommons.org/licenses/by/4.0/

Copyright Statement
Copyright © 2022
The Authors, some
rights reserved;
exclusive licensee
American Association
for the Advancement
of Science. No claim to
original U.S.Government
Works. Distributed
under a Creative
Commons Attribution
License 4.0 (CC BY).





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