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Title: Synthesis of Lanthanum Tungsten Oxynitride Perovskite Thin Films

Abstract

Ternary metal-oxide material systems commonly crystallize in the perovskite crystal structure, which is utilized in numerous electronic applications. In contrast to oxides, there are no known nitride perovskites, likely due to the competition with oxidation, which makes the formation of pure nitride materials difficult and synthesis of oxynitride materials more common. While deposition of oxynitride perovskite thin films is important for many electronic applications, it is difficult to control oxygen and nitrogen stoichiometry. Lanthanum tungsten oxynitride (LaWN3-..delta..O..delta..) thin films with varying La:W ratio are synthesized by combinatorial sputtering and characterized for their chemical composition, crystal structure, and microstructure. A three-step synthesis method, which involves co-sputtering, capping layer deposition, and rapid thermal annealing, is established for producing crystalline thin films while minimizing the oxygen content. Elemental depth profiling results show that the cation-stoichiometric films contain approximately one oxygen for every five nitrogen (..delta.. = 0.5). Synchrotron-based diffraction indicates a tetragonal perovskite crystal structure. These results are discussed in terms of the perovskite tolerance factors, octahedral tilting, and bond valence. Overall, this synthesis and characterization is expected to pave the way toward future thin film property measurements of lanthanum tungsten oxynitrides and eventual synthesis of oxygen-free nitride perovskites.

Authors:
 [1];  [1];  [1];  [2];  [3];  [4];  [4]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Univ. of California, Berkeley, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Colorado School of Mines, Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1526455
Alternate Identifier(s):
OSTI ID: 1524106
Report Number(s):
NREL/JA-5K00-71392
Journal ID: ISSN 2199-160X
Grant/Contract Number:  
AC36-08GO28308; DE‐AC36‐08GO28308; DE‐AC02‐76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Electronic Materials
Additional Journal Information:
Journal Volume: 5; Journal Issue: 7; Journal ID: ISSN 2199-160X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; LaWON; oxynitride; perovskites; sputtering; thin films

Citation Formats

Talley, Kevin, Mangum, John, Perkins, Craig, Woods-Robinson, Rachel, Mehta, Apurva, Gorman, Brian, Brennecka, Geoff, and Zakutayev, Andriy A. Synthesis of Lanthanum Tungsten Oxynitride Perovskite Thin Films. United States: N. p., 2019. Web. doi:10.1002/aelm.201900214.
Talley, Kevin, Mangum, John, Perkins, Craig, Woods-Robinson, Rachel, Mehta, Apurva, Gorman, Brian, Brennecka, Geoff, & Zakutayev, Andriy A. Synthesis of Lanthanum Tungsten Oxynitride Perovskite Thin Films. United States. doi:10.1002/aelm.201900214.
Talley, Kevin, Mangum, John, Perkins, Craig, Woods-Robinson, Rachel, Mehta, Apurva, Gorman, Brian, Brennecka, Geoff, and Zakutayev, Andriy A. Mon . "Synthesis of Lanthanum Tungsten Oxynitride Perovskite Thin Films". United States. doi:10.1002/aelm.201900214. https://www.osti.gov/servlets/purl/1526455.
@article{osti_1526455,
title = {Synthesis of Lanthanum Tungsten Oxynitride Perovskite Thin Films},
author = {Talley, Kevin and Mangum, John and Perkins, Craig and Woods-Robinson, Rachel and Mehta, Apurva and Gorman, Brian and Brennecka, Geoff and Zakutayev, Andriy A.},
abstractNote = {Ternary metal-oxide material systems commonly crystallize in the perovskite crystal structure, which is utilized in numerous electronic applications. In contrast to oxides, there are no known nitride perovskites, likely due to the competition with oxidation, which makes the formation of pure nitride materials difficult and synthesis of oxynitride materials more common. While deposition of oxynitride perovskite thin films is important for many electronic applications, it is difficult to control oxygen and nitrogen stoichiometry. Lanthanum tungsten oxynitride (LaWN3-..delta..O..delta..) thin films with varying La:W ratio are synthesized by combinatorial sputtering and characterized for their chemical composition, crystal structure, and microstructure. A three-step synthesis method, which involves co-sputtering, capping layer deposition, and rapid thermal annealing, is established for producing crystalline thin films while minimizing the oxygen content. Elemental depth profiling results show that the cation-stoichiometric films contain approximately one oxygen for every five nitrogen (..delta.. = 0.5). Synchrotron-based diffraction indicates a tetragonal perovskite crystal structure. These results are discussed in terms of the perovskite tolerance factors, octahedral tilting, and bond valence. Overall, this synthesis and characterization is expected to pave the way toward future thin film property measurements of lanthanum tungsten oxynitrides and eventual synthesis of oxygen-free nitride perovskites.},
doi = {10.1002/aelm.201900214},
journal = {Advanced Electronic Materials},
number = 7,
volume = 5,
place = {United States},
year = {2019},
month = {6}
}

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