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Title: Ab Initio Predictions of Hexagonal Zr(B,C,N) Polymorphs for Coherent Interface Design

Abstract

Density functional theory calculations are used to explore hexagonal (HX) NiAs-like polymorphs of Zr(B,C,N) and compare with corresponding Zr(B,C,N) Hagg-like face-centered cubic rocksalt (B1) phases. While all predicted compounds are mechanically stable according to the Born-Huang criteria, only HX Zr(C,N) are found dynamically stable from ab initio molecular dynamics simulations and lattice dynamics calculations. HX ZrN emerges as a candidate structure with ground state energy, elastic constants, and extrinsic mechanical parameters comparable with those of B1 ZrN. Ab initio band structure and semi-classical Boltzmann transport calculations predict a metallic character and a monotonic increase in electrical conductivity with the number of valence electrons. Electronic structure calculations indicate that the HX phases gain their stability and mechanical attributes by Zr d- non-metal p hybridization and by broadening of Zr d bands. Furthermore, it is shown that the HX ZrN phase provides a low-energy coherent interface model for connecting B1 ZrN domains, with significant energetic advantage over an atomistic interface model derived from high resolution transmission electron microscopy images. The ab initio characterizations provided herein should aid the experimental identification of non-Hagg-like hard phases. Furthermore, the results can also enrich the variety of crystalline phases potentially available for designing coherent interfaces inmore » superhard nanostructured materials and in materials with multilayer characteristics.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2];  [3]; ORCiD logo [1]
  1. Univ. of Minnesota-Twin Cities, Minneapolis, MN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Texas at Arlington, Arlington, TX (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1410197
DOE Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Physical Chemistry. C; Journal Volume: 121; Journal Issue: 46
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Hu, Chongze, Huang, Jingsong, Sumpter, Bobby G., Meletis, Efstathios, and Dumitrica, Traian. Ab Initio Predictions of Hexagonal Zr(B,C,N) Polymorphs for Coherent Interface Design. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.7b09444.
Hu, Chongze, Huang, Jingsong, Sumpter, Bobby G., Meletis, Efstathios, & Dumitrica, Traian. Ab Initio Predictions of Hexagonal Zr(B,C,N) Polymorphs for Coherent Interface Design. United States. doi:10.1021/acs.jpcc.7b09444.
Hu, Chongze, Huang, Jingsong, Sumpter, Bobby G., Meletis, Efstathios, and Dumitrica, Traian. Fri . "Ab Initio Predictions of Hexagonal Zr(B,C,N) Polymorphs for Coherent Interface Design". United States. doi:10.1021/acs.jpcc.7b09444.
@article{osti_1410197,
title = {Ab Initio Predictions of Hexagonal Zr(B,C,N) Polymorphs for Coherent Interface Design},
author = {Hu, Chongze and Huang, Jingsong and Sumpter, Bobby G. and Meletis, Efstathios and Dumitrica, Traian},
abstractNote = {Density functional theory calculations are used to explore hexagonal (HX) NiAs-like polymorphs of Zr(B,C,N) and compare with corresponding Zr(B,C,N) Hagg-like face-centered cubic rocksalt (B1) phases. While all predicted compounds are mechanically stable according to the Born-Huang criteria, only HX Zr(C,N) are found dynamically stable from ab initio molecular dynamics simulations and lattice dynamics calculations. HX ZrN emerges as a candidate structure with ground state energy, elastic constants, and extrinsic mechanical parameters comparable with those of B1 ZrN. Ab initio band structure and semi-classical Boltzmann transport calculations predict a metallic character and a monotonic increase in electrical conductivity with the number of valence electrons. Electronic structure calculations indicate that the HX phases gain their stability and mechanical attributes by Zr d- non-metal p hybridization and by broadening of Zr d bands. Furthermore, it is shown that the HX ZrN phase provides a low-energy coherent interface model for connecting B1 ZrN domains, with significant energetic advantage over an atomistic interface model derived from high resolution transmission electron microscopy images. The ab initio characterizations provided herein should aid the experimental identification of non-Hagg-like hard phases. Furthermore, the results can also enrich the variety of crystalline phases potentially available for designing coherent interfaces in superhard nanostructured materials and in materials with multilayer characteristics.},
doi = {10.1021/acs.jpcc.7b09444},
journal = {Journal of Physical Chemistry. C},
number = 46,
volume = 121,
place = {United States},
year = {Fri Oct 27 00:00:00 EDT 2017},
month = {Fri Oct 27 00:00:00 EDT 2017}
}