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Title: Connecting energetics to dynamics in particle growth by oriented attachment using real-time observations

Abstract

The interplay between crystal and solvent structure, interparticle forces and ensemble particle response dynamics governs the process of crystallization by oriented attachment (OA), yet a quantitative understanding is lacking. Using as a model system ZnO, we combine in situ TEM observations of single particle and ensemble assembly dynamics with simulations of interparticle forces and responses to relate experimentally derived interparticle potentials to the underlying interactions. We show that OA is driven by forces and torques due to a combination of electrostatic ion-solvent correlations and dipolar interactions that act at separations well beyond 5 nm. Importantly, coalignment is achieved before particles reach separations at which strong attractions drive the final jump to contact. The observed barrier to attachment is negligible, while dissipative factors in the quasi-2D confinement of the TEM fluid cell lead to abnormal diffusivities with timescales for rotation much less than for translation, thus enabling OA to dominate.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1]
  1. BATTELLE (PACIFIC NW LAB)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1604768
Report Number(s):
[PNNL-SA-148131]
Grant/Contract Number:  
[AC05-76RL01830]
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
[ Journal Volume: 11; Journal Issue: 1]
Country of Publication:
United States
Language:
English

Citation Formats

Liu, Lili, Nakouzi, Elias, Sushko, Maria L., Schenter, Gregory K., Mundy, Christopher J., Chun, Jaehun, and De Yoreo, James J. Connecting energetics to dynamics in particle growth by oriented attachment using real-time observations. United States: N. p., 2020. Web. doi:10.1038/s41467-020-14719-w.
Liu, Lili, Nakouzi, Elias, Sushko, Maria L., Schenter, Gregory K., Mundy, Christopher J., Chun, Jaehun, & De Yoreo, James J. Connecting energetics to dynamics in particle growth by oriented attachment using real-time observations. United States. doi:10.1038/s41467-020-14719-w.
Liu, Lili, Nakouzi, Elias, Sushko, Maria L., Schenter, Gregory K., Mundy, Christopher J., Chun, Jaehun, and De Yoreo, James J. Tue . "Connecting energetics to dynamics in particle growth by oriented attachment using real-time observations". United States. doi:10.1038/s41467-020-14719-w.
@article{osti_1604768,
title = {Connecting energetics to dynamics in particle growth by oriented attachment using real-time observations},
author = {Liu, Lili and Nakouzi, Elias and Sushko, Maria L. and Schenter, Gregory K. and Mundy, Christopher J. and Chun, Jaehun and De Yoreo, James J.},
abstractNote = {The interplay between crystal and solvent structure, interparticle forces and ensemble particle response dynamics governs the process of crystallization by oriented attachment (OA), yet a quantitative understanding is lacking. Using as a model system ZnO, we combine in situ TEM observations of single particle and ensemble assembly dynamics with simulations of interparticle forces and responses to relate experimentally derived interparticle potentials to the underlying interactions. We show that OA is driven by forces and torques due to a combination of electrostatic ion-solvent correlations and dipolar interactions that act at separations well beyond 5 nm. Importantly, coalignment is achieved before particles reach separations at which strong attractions drive the final jump to contact. The observed barrier to attachment is negligible, while dissipative factors in the quasi-2D confinement of the TEM fluid cell lead to abnormal diffusivities with timescales for rotation much less than for translation, thus enabling OA to dominate.},
doi = {10.1038/s41467-020-14719-w},
journal = {Nature Communications},
number = [1],
volume = [11],
place = {United States},
year = {2020},
month = {12}
}

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