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Title: Combinatorial Synthesis of Magnesium Tin Nitride Semiconductors

Abstract

Nitride materials feature strong chemical bonding character that leads to unique crystal structures, but many ternary nitride chemical spaces remain experimentally unexplored. The search for previously undiscovered ternary nitrides is also an opportunity to explore unique materials properties, such as transitions between cation-ordered and -disordered structures, as well as to identify candidate materials for optoelectronic applications. Here, we present a comprehensive experimental study of MgSnN 2, an emerging II–IV–N 2 compound, for the first time mapping phase composition and crystal structure, and examining its optoelectronic properties computationally and experimentally. We demonstrate combinatorial cosputtering of cation-disordered, wurtzite-type MgSnN 2 across a range of cation compositions and temperatures, as well as the unexpected formation of a secondary, rocksalt-type phase of MgSnN 2 at Mg-rich compositions and low temperatures. Furthermore, a computational structure search shows that the rocksalt-type phase is substantially metastable (>70 meV/atom) compared to the wurtzite-type ground state. Spectroscopic ellipsometry reveals optical absorption onsets around 2 eV, consistent with band gap tuning via cation disorder. Finally, we demonstrate epitaxial growth of a mixed wurtzite-rocksalt MgSnN2 on GaN, highlighting an opportunity for polymorphic control via epitaxy. Collectively, these findings lay the groundwork for further exploration of MgSnN 2 as a model ternarymore » nitride, with controlled polymorphism, and for device applications, enabled by control of optoelectronic properties via cation ordering.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2];  [2]; ORCiD logo [1]; ORCiD logo [3];  [4];  [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [4]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Colorado School of Mines, Golden, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1659856
Report Number(s):
NREL/JA-5K00-76175
Journal ID: ISSN 0002-7863; MainId:6827;UUID:bca7f71d-d454-ea11-9c31-ac162d87dfe5;MainAdminID:13514
Grant/Contract Number:  
AC36-08GO28308; AC02-76SF00515; DGE 1106400; DGE 1752814; 1646713
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 142; Journal Issue: 18; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; nitride semiconductors; light-emitting diodes; combinatorial synthesis; RF co-sputtering

Citation Formats

Greenaway, Ann, Loutris, Amanda L., Heinselman, Karen, Melamed, Celeste, Schnepf, Rekha, Tellekamp, Brooks, Woods-Robinson, Rachel, Sherbondy, Rachel, Bardgett, Dylan, Bauers, Sage, Zakutayev, Andriy, Christensen, Steven, Lany, Stephan, and Tamboli, Adele. Combinatorial Synthesis of Magnesium Tin Nitride Semiconductors. United States: N. p., 2020. Web. doi:10.1021/jacs.0c02092.
Greenaway, Ann, Loutris, Amanda L., Heinselman, Karen, Melamed, Celeste, Schnepf, Rekha, Tellekamp, Brooks, Woods-Robinson, Rachel, Sherbondy, Rachel, Bardgett, Dylan, Bauers, Sage, Zakutayev, Andriy, Christensen, Steven, Lany, Stephan, & Tamboli, Adele. Combinatorial Synthesis of Magnesium Tin Nitride Semiconductors. United States. https://doi.org/10.1021/jacs.0c02092
Greenaway, Ann, Loutris, Amanda L., Heinselman, Karen, Melamed, Celeste, Schnepf, Rekha, Tellekamp, Brooks, Woods-Robinson, Rachel, Sherbondy, Rachel, Bardgett, Dylan, Bauers, Sage, Zakutayev, Andriy, Christensen, Steven, Lany, Stephan, and Tamboli, Adele. Sat . "Combinatorial Synthesis of Magnesium Tin Nitride Semiconductors". United States. https://doi.org/10.1021/jacs.0c02092.
@article{osti_1659856,
title = {Combinatorial Synthesis of Magnesium Tin Nitride Semiconductors},
author = {Greenaway, Ann and Loutris, Amanda L. and Heinselman, Karen and Melamed, Celeste and Schnepf, Rekha and Tellekamp, Brooks and Woods-Robinson, Rachel and Sherbondy, Rachel and Bardgett, Dylan and Bauers, Sage and Zakutayev, Andriy and Christensen, Steven and Lany, Stephan and Tamboli, Adele},
abstractNote = {Nitride materials feature strong chemical bonding character that leads to unique crystal structures, but many ternary nitride chemical spaces remain experimentally unexplored. The search for previously undiscovered ternary nitrides is also an opportunity to explore unique materials properties, such as transitions between cation-ordered and -disordered structures, as well as to identify candidate materials for optoelectronic applications. Here, we present a comprehensive experimental study of MgSnN2, an emerging II–IV–N2 compound, for the first time mapping phase composition and crystal structure, and examining its optoelectronic properties computationally and experimentally. We demonstrate combinatorial cosputtering of cation-disordered, wurtzite-type MgSnN2 across a range of cation compositions and temperatures, as well as the unexpected formation of a secondary, rocksalt-type phase of MgSnN2 at Mg-rich compositions and low temperatures. Furthermore, a computational structure search shows that the rocksalt-type phase is substantially metastable (>70 meV/atom) compared to the wurtzite-type ground state. Spectroscopic ellipsometry reveals optical absorption onsets around 2 eV, consistent with band gap tuning via cation disorder. Finally, we demonstrate epitaxial growth of a mixed wurtzite-rocksalt MgSnN2 on GaN, highlighting an opportunity for polymorphic control via epitaxy. Collectively, these findings lay the groundwork for further exploration of MgSnN2 as a model ternary nitride, with controlled polymorphism, and for device applications, enabled by control of optoelectronic properties via cation ordering.},
doi = {10.1021/jacs.0c02092},
url = {https://www.osti.gov/biblio/1659856}, journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 18,
volume = 142,
place = {United States},
year = {2020},
month = {4}
}

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