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

Chongze Hu, Jingsong Huang, Bobby G. Sumpter, Efstathios Meletis, Traian Dumitricǎ

Research output: Contribution to journalArticle

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Abstract

Density functional theory calculations are used herein to explore the hexagonal (HX) NiAs-like polymorphs of Zr(B,C,N) and compare them with the corresponding Zr(B,C,N) Hagg-like face-centered-cubic rocksalt (B1) phases. Although all predicted compounds are mechanically stable according to the Born-Huang criteria, only HX Zr(C,N) are dynamically stable according to ab initio molecular dynamics simulations and lattice dynamics calculations. HX ZrN emerges as a candidate structure with a ground-state energy, elastic constants, and extrinsic mechanical parameters comparable with those of B1 ZrN. Ab initio band structure and semiclassical 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 through Zr d-nonmetal p hybridization and broadening of the 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 (HRTEM) images. The ab initio characterizations provided herein should aid the experimental identification of non-Hagg-like hard phases. 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.

Original languageEnglish (US)
Pages (from-to)26007-26018
Number of pages12
JournalJournal of Physical Chemistry C
Volume121
Issue number46
DOIs
StatePublished - Nov 22 2017

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Polymorphism
predictions
Nonmetals
Lattice vibrations
Elastic constants
High resolution transmission electron microscopy
Nanostructured materials
Band structure
Ground state
Electronic structure
Density functional theory
Molecular dynamics
Multilayers
elastic properties
molecular dynamics
density functional theory
electronic structure
Crystalline materials
valence
transmission electron microscopy

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Ab Initio Predictions of Hexagonal Zr(B,C,N) Polymorphs for Coherent Interface Design. / Hu, Chongze; Huang, Jingsong; Sumpter, Bobby G.; Meletis, Efstathios; Dumitricǎ, Traian.

In: Journal of Physical Chemistry C, Vol. 121, No. 46, 22.11.2017, p. 26007-26018.

Research output: Contribution to journalArticle

Hu, Chongze ; Huang, Jingsong ; Sumpter, Bobby G. ; Meletis, Efstathios ; Dumitricǎ, Traian. / Ab Initio Predictions of Hexagonal Zr(B,C,N) Polymorphs for Coherent Interface Design. In: Journal of Physical Chemistry C. 2017 ; Vol. 121, No. 46. pp. 26007-26018.
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