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Title: First‐principles study in an inter‐granular glassy film model of silicon nitride

Journal Article · · Journal of the American Ceramic Society
DOI: https://doi.org/10.1111/jace.15538 · OSTI ID:1429527
ORCiD logo [1];  [2];  [1];  [1];  [3];  [4]
  1. Department of Physics and Astronomy University of Missouri‐Kansas City Kansas City Missouri
  2. Department of Adaptive Machine Systems Osaka University Suita Osaka Japan, Japan Fine Ceramics Center Atsuta Nagoya Japan
  3. Japan Fine Ceramics Center Atsuta Nagoya Japan, Institute of Engineering Innovation University of Tokyo Bunkyo Tokyo Japan
  4. Japan Fine Ceramics Center Atsuta Nagoya Japan, Department of Materials Science and Engineering Kyoto University Kyoto Japan
+ Show Author Affiliations

Abstract Based on a previously constructed intergranular glassy film ( IGF ) model for bulk silicon nitride, a large periodic model of 3864 atoms containing 2 grains of different orientations from the main bulk β‐Si 3 N 4 and 2 IGF s was fully relaxed using the ab initio density‐functional theory package VASP . The relaxed structure was then used to calculate the electronic structure, density of states, interatomic bonding, partial charge distribution, and electron localization using the OLCAO method. Analysis of the data focuses on the interfacial regions between bulk β‐Si 3 N 4 and the Si‐O‐N glass layer with different orientations. The total bond order density ( TBOD ) is evaluated in different interfacial and bulk regions. We show minor differences in the internal cohesion between crystalline grains of different facets. However, the overall charges in the bulk crystal grains and in the glassy regions are electropositive which are balanced by the negatively charged interfacial region between the two. The presence of a less rigid glassy layer is the reason for structural flexibility in ceramics without a huge penalty in the steric energy. The optimization of the interfacial structure and bonding via the creation of defective sites is the atomic origin for the existence of the IGF in silicon nitride. The insights obtained from this detailed quantum mechanical analysis of a realistic IGF model are discussed including implications on the strength, fracture toughness, and processing methods. We also discuss the potential applications of our method to other complex materials systems.

Sponsoring Organization:
USDOE
Grant/Contract Number:
AC03-76SF00098
OSTI ID:
1429527
Journal Information:
Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Journal Issue: 7 Vol. 101; ISSN 0002-7820
Publisher:
Wiley-BlackwellCopyright Statement
Country of Publication:
United States
Language:
English

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