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Title: A map of the inorganic ternary metal nitrides

Abstract

Exploratory synthesis in new chemical spaces is the essence of solid-state chemistry. However, uncharted chemical spaces can be difficult to navigate, especially when materials synthesis is challenging. Nitrides represent one such space, where stringent synthesis constraints have limited the exploration of this important class of functional materials. Here, we employ a suite of computational materials discovery and informatics tools to construct a large stability map of the inorganic ternary metal nitrides. Our map clusters the ternary nitrides into chemical families with distinct stability and metastability, and highlights hundreds of promising new ternary nitride spaces for experimental investigation - from which we experimentally realized seven new Zn- and Mg-based ternary nitrides. As a result, by extracting the mixed metallicity, ionicity and covalency of solid-state bonding from the density functional theory (DFT)-computed electron density, we reveal the complex interplay between chemistry, composition and electronic structure in governing large-scale stability trends in ternary nitride materials.

Authors:
ORCiD logo [1];  [2];  [3];  [3];  [4];  [5];  [6]; ORCiD logo [6]; ORCiD logo [6];  [3]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [7];  [8]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of Colorado, Boulder, CO (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  4. Oregon State Univ., Corvallis, OR (United States)
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  7. Univ. of Colorado, Boulder, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1574332
Alternate Identifier(s):
OSTI ID: 1542766
Report Number(s):
NREL/JA-5K00-72591
Journal ID: ISSN 1476-1122
Grant/Contract Number:  
AC36-08GO28308; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 18; Journal Issue: 7; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; chemical bonding; density functional theory; solid-state chemistry; structure prediction; thermodynamics

Citation Formats

Sun, Wenhao, Bartel, Christopher J., Arca, Elisabetta, Bauers, Sage R., Matthews, Bethany, Orvañanos, Bernardo, Chen, Bor -Rong, Toney, Michael F., Schelhas, Laura T., Tumas, William, Tate, Janet, Zakutayev, Andriy, Lany, Stephan, Holder, Aaron M., and Ceder, Gerbrand. A map of the inorganic ternary metal nitrides. United States: N. p., 2019. Web. doi:10.1038/s41563-019-0396-2.
Sun, Wenhao, Bartel, Christopher J., Arca, Elisabetta, Bauers, Sage R., Matthews, Bethany, Orvañanos, Bernardo, Chen, Bor -Rong, Toney, Michael F., Schelhas, Laura T., Tumas, William, Tate, Janet, Zakutayev, Andriy, Lany, Stephan, Holder, Aaron M., & Ceder, Gerbrand. A map of the inorganic ternary metal nitrides. United States. doi:10.1038/s41563-019-0396-2.
Sun, Wenhao, Bartel, Christopher J., Arca, Elisabetta, Bauers, Sage R., Matthews, Bethany, Orvañanos, Bernardo, Chen, Bor -Rong, Toney, Michael F., Schelhas, Laura T., Tumas, William, Tate, Janet, Zakutayev, Andriy, Lany, Stephan, Holder, Aaron M., and Ceder, Gerbrand. Mon . "A map of the inorganic ternary metal nitrides". United States. doi:10.1038/s41563-019-0396-2.
@article{osti_1574332,
title = {A map of the inorganic ternary metal nitrides},
author = {Sun, Wenhao and Bartel, Christopher J. and Arca, Elisabetta and Bauers, Sage R. and Matthews, Bethany and Orvañanos, Bernardo and Chen, Bor -Rong and Toney, Michael F. and Schelhas, Laura T. and Tumas, William and Tate, Janet and Zakutayev, Andriy and Lany, Stephan and Holder, Aaron M. and Ceder, Gerbrand},
abstractNote = {Exploratory synthesis in new chemical spaces is the essence of solid-state chemistry. However, uncharted chemical spaces can be difficult to navigate, especially when materials synthesis is challenging. Nitrides represent one such space, where stringent synthesis constraints have limited the exploration of this important class of functional materials. Here, we employ a suite of computational materials discovery and informatics tools to construct a large stability map of the inorganic ternary metal nitrides. Our map clusters the ternary nitrides into chemical families with distinct stability and metastability, and highlights hundreds of promising new ternary nitride spaces for experimental investigation - from which we experimentally realized seven new Zn- and Mg-based ternary nitrides. As a result, by extracting the mixed metallicity, ionicity and covalency of solid-state bonding from the density functional theory (DFT)-computed electron density, we reveal the complex interplay between chemistry, composition and electronic structure in governing large-scale stability trends in ternary nitride materials.},
doi = {10.1038/s41563-019-0396-2},
journal = {Nature Materials},
number = 7,
volume = 18,
place = {United States},
year = {2019},
month = {6}
}

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