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Title: Energy landscape of ZnO clusters and low-density polymorphs

Abstract

We report on an extensive study of ZnO materials with cagelike motifs in clusters and bulk phases through structural searches using the minima hopping method. A novel putative ground state was discovered for the (ZnO)32 cluster with a tubelike structure, closely related to the previously reported (ZnO)24 ground-state cage geometry. Furthermore, the effect of ionization on the geometries and energetic ordering of (ZnO)n clusters with n=3–10,12 was studied by directly sampling the energy landscape of the ionized system. Our results indicate that the transition from ring and planar structures to three-dimensional cages occurs at larger cluster sizes than in the neutral system. Inspired by the bottom-up design philosophy and the predominance of cagelike structures in medium-sized clusters, a search for crystalline ZnO was conducted aimed specifically at low-density polymorphs, resulting in the discovery of 57 novel metastable phases. The voids in these low-density materials closely resemble the hollow cage structures of small (ZnO)n/(ZnO)+n clusters with n<16. Analogous to clathrate materials, these voids could serve to accommodate guest atoms to tailor the materials properties for various applications.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2]
  1. Inst. for Advanced Studies in Basic Sciences (IASBS). Dept. of Physics
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1544374
DOE Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 96; Journal Issue: 6; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English

Citation Formats

Rasoulkhani, Robabe, Tahmasbi, Hossein, Ghasemi, S. Alireza, Faraji, Somayeh, Rostami, Samare, and Amsler, Maximilian. Energy landscape of ZnO clusters and low-density polymorphs. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.96.064108.
Rasoulkhani, Robabe, Tahmasbi, Hossein, Ghasemi, S. Alireza, Faraji, Somayeh, Rostami, Samare, & Amsler, Maximilian. Energy landscape of ZnO clusters and low-density polymorphs. United States. doi:10.1103/PhysRevB.96.064108.
Rasoulkhani, Robabe, Tahmasbi, Hossein, Ghasemi, S. Alireza, Faraji, Somayeh, Rostami, Samare, and Amsler, Maximilian. Tue . "Energy landscape of ZnO clusters and low-density polymorphs". United States. doi:10.1103/PhysRevB.96.064108.
@article{osti_1544374,
title = {Energy landscape of ZnO clusters and low-density polymorphs},
author = {Rasoulkhani, Robabe and Tahmasbi, Hossein and Ghasemi, S. Alireza and Faraji, Somayeh and Rostami, Samare and Amsler, Maximilian},
abstractNote = {We report on an extensive study of ZnO materials with cagelike motifs in clusters and bulk phases through structural searches using the minima hopping method. A novel putative ground state was discovered for the (ZnO)32 cluster with a tubelike structure, closely related to the previously reported (ZnO)24 ground-state cage geometry. Furthermore, the effect of ionization on the geometries and energetic ordering of (ZnO)n clusters with n=3–10,12 was studied by directly sampling the energy landscape of the ionized system. Our results indicate that the transition from ring and planar structures to three-dimensional cages occurs at larger cluster sizes than in the neutral system. Inspired by the bottom-up design philosophy and the predominance of cagelike structures in medium-sized clusters, a search for crystalline ZnO was conducted aimed specifically at low-density polymorphs, resulting in the discovery of 57 novel metastable phases. The voids in these low-density materials closely resemble the hollow cage structures of small (ZnO)n/(ZnO)+n clusters with n<16. Analogous to clathrate materials, these voids could serve to accommodate guest atoms to tailor the materials properties for various applications.},
doi = {10.1103/PhysRevB.96.064108},
journal = {Physical Review B},
issn = {2469-9950},
number = 6,
volume = 96,
place = {United States},
year = {2017},
month = {8}
}

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