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Title: Condensation and dissociation rates for gas phase metal clusters from molecular dynamics trajectory calculations

Abstract

In gas phase synthesis systems, clusters form and grow via condensation, in which a monomer binds to an existing cluster. While a hard sphere equation is frequently used to predict the condensation rate coefficient, this equation neglects the influences of potential interactions and cluster internal energy on the condensation process. Here, we present a collision rate theory-Molecular Dynamics simulation approach to calculate condensation probabilities and condensation rate coefficients; we use this approach to examine atomic condensation onto 6-56 atom Au and Mg clusters. The probability of condensation depends upon the initial relative velocity (v) between atom and cluster and the initial impact parameter (b). In all cases there is a well-defined region of b-v space where condensation is highly probable, and outside of which the condensation probability drops to zero. For Au clusters with more than 10 atoms, we find that at gas temperatures in the 300-1200 K range, the condensation rate coefficient exceeds the hard sphere rate coefficient by a factor of 1.5-2.0. Conversely, for Au clusters with 10 or fewer atoms, and for 14 atom and 28 atom Mg clusters, as cluster equilibration temperature increases the condensation rate coefficient drops to values below the hard sphere rate coefficient.more » Calculations also yield the self-dissociation rate coefficient, which is found to vary considerably with gas temperature. Finally, calculations results reveal that grazing (high b) atom-cluster collisions at elevated velocity (> 1000 m s-1) can result in the colliding atom rebounding (bounce) from the cluster surface or binding while another atom dissociates (replacement). In conclusion, the presented method can be applied in developing rate equations to predict material formation and growth rates in vapor phase systems.« less

Authors:
 [1];  [1]; ORCiD logo [1]
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  1. Univ. of Minnesota, Minneapolis, MN (United States)
Publication Date:
Research Org.:
Univ. of Minnesota, Minneapolis, MN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1434278
Alternate Identifier(s):
OSTI ID: 1434402
Grant/Contract Number:  
SC0018202
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 148; Journal Issue: 16; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; Clusters; Gas Phase Synthesis; Condensation

Citation Formats

Yang, Huan, Goudeli, Eirini, and Hogan, Christopher J. Condensation and dissociation rates for gas phase metal clusters from molecular dynamics trajectory calculations. United States: N. p., 2018. Web. doi:10.1063/1.5026689.
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Yang, Huan, Goudeli, Eirini, & Hogan, Christopher J. Condensation and dissociation rates for gas phase metal clusters from molecular dynamics trajectory calculations. United States. doi:https://doi.org/10.1063/1.5026689
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Yang, Huan, Goudeli, Eirini, and Hogan, Christopher J. Tue . "Condensation and dissociation rates for gas phase metal clusters from molecular dynamics trajectory calculations". United States. doi:https://doi.org/10.1063/1.5026689. https://www.osti.gov/servlets/purl/1434278.
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@article{osti_1434278,
title = {Condensation and dissociation rates for gas phase metal clusters from molecular dynamics trajectory calculations},
author = {Yang, Huan and Goudeli, Eirini and Hogan, Christopher J.},
abstractNote = {In gas phase synthesis systems, clusters form and grow via condensation, in which a monomer binds to an existing cluster. While a hard sphere equation is frequently used to predict the condensation rate coefficient, this equation neglects the influences of potential interactions and cluster internal energy on the condensation process. Here, we present a collision rate theory-Molecular Dynamics simulation approach to calculate condensation probabilities and condensation rate coefficients; we use this approach to examine atomic condensation onto 6-56 atom Au and Mg clusters. The probability of condensation depends upon the initial relative velocity (v) between atom and cluster and the initial impact parameter (b). In all cases there is a well-defined region of b-v space where condensation is highly probable, and outside of which the condensation probability drops to zero. For Au clusters with more than 10 atoms, we find that at gas temperatures in the 300-1200 K range, the condensation rate coefficient exceeds the hard sphere rate coefficient by a factor of 1.5-2.0. Conversely, for Au clusters with 10 or fewer atoms, and for 14 atom and 28 atom Mg clusters, as cluster equilibration temperature increases the condensation rate coefficient drops to values below the hard sphere rate coefficient. Calculations also yield the self-dissociation rate coefficient, which is found to vary considerably with gas temperature. Finally, calculations results reveal that grazing (high b) atom-cluster collisions at elevated velocity (> 1000 m s-1) can result in the colliding atom rebounding (bounce) from the cluster surface or binding while another atom dissociates (replacement). In conclusion, the presented method can be applied in developing rate equations to predict material formation and growth rates in vapor phase systems.},
doi = {10.1063/1.5026689},
journal = {Journal of Chemical Physics},
number = 16,
volume = 148,
place = {United States},
year = {2018},
month = {4}
}
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DOI:  https://doi.org/10.1063/1.5026689
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Figures / Tables:

FIG. 1 FIG. 1: (a) A depiction of the distant atom and cluster in the collision framework employed for determination of PTc (b, v), probability of condensation for prescribed b and v at a given equilibration cluster temperature Tc. (b) Depictions of the four distinct types of events observed in molecular dynamicsmore » trajectory calculations. The type of event depends upon the initial cluster equilibration temperature and orientation, as well as the distant atom initial velocity and impact parameter.« less
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