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Title: Interplay between Composition, Electronic Structure, Disorder, and Doping due to Dual Sublattice Mixing in Nonequilibrium Synthesis of ZnSnN 2:O

Abstract

We report the opportunity for enhanced functional properties in semiconductor solid solutions has attracted vast scientific interest for a variety of novel applications. However, the functional versatility originating from the additional degrees of freedom due to atomic composition and ordering comes along with new challenges in characterization and modeling. Developing predictive synthesis-structure-property relationships is prerequisite for effective materials design strategies. Here, a first-principles based model for property prediction in such complex semiconductor materials is presented. This framework incorporates nonequilibrium synthesis, dopants and defects, and the change of the electronic structure with composition and short range order. This approach is applied to ZnSnN 2 (ZTN) which has attracted recent interest for photovoltaics. The unintentional oxygen incorporation and its correlation with the cation stoichiometry leads to the formation of a solid solution with dual sublattice mixing. A nonmonotonic doping behavior as a function of the composition is uncovered. Finally, the degenerate doping of near-stoichiometric ZTN, which is detrimental for potential applications, can be lowered into the 10 17 cm -3 range in highly off-stoichiometric material, in quantitative agreement with experiments.

Authors:
ORCiD logo [1];  [2];  [3];  [1];  [1];  [1]
  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. Colorado School of Mines, Golden, CO (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S)
OSTI Identifier:
1494598
Alternate Identifier(s):
OSTI ID: 1491922
Report Number(s):
NREL/JA-5K00-73055
Journal ID: ISSN 0935-9648
Grant/Contract Number:  
AC36-08GO28308; 30302
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 11; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; computational materials design; defects; disorder; electronic structure; multinary material; nonequilibrium synthesis; semiconductor solid solution

Citation Formats

Pan, Jie, Cordell, Jacob, Tucker, Garritt J., Tamboli, Adele C., Zakutayev, Andriy, and Lany, Stephan. Interplay between Composition, Electronic Structure, Disorder, and Doping due to Dual Sublattice Mixing in Nonequilibrium Synthesis of ZnSnN2:O. United States: N. p., 2019. Web. doi:10.1002/adma.201807406.
Pan, Jie, Cordell, Jacob, Tucker, Garritt J., Tamboli, Adele C., Zakutayev, Andriy, & Lany, Stephan. Interplay between Composition, Electronic Structure, Disorder, and Doping due to Dual Sublattice Mixing in Nonequilibrium Synthesis of ZnSnN2:O. United States. doi:10.1002/adma.201807406.
Pan, Jie, Cordell, Jacob, Tucker, Garritt J., Tamboli, Adele C., Zakutayev, Andriy, and Lany, Stephan. Tue . "Interplay between Composition, Electronic Structure, Disorder, and Doping due to Dual Sublattice Mixing in Nonequilibrium Synthesis of ZnSnN2:O". United States. doi:10.1002/adma.201807406.
@article{osti_1494598,
title = {Interplay between Composition, Electronic Structure, Disorder, and Doping due to Dual Sublattice Mixing in Nonequilibrium Synthesis of ZnSnN2:O},
author = {Pan, Jie and Cordell, Jacob and Tucker, Garritt J. and Tamboli, Adele C. and Zakutayev, Andriy and Lany, Stephan},
abstractNote = {We report the opportunity for enhanced functional properties in semiconductor solid solutions has attracted vast scientific interest for a variety of novel applications. However, the functional versatility originating from the additional degrees of freedom due to atomic composition and ordering comes along with new challenges in characterization and modeling. Developing predictive synthesis-structure-property relationships is prerequisite for effective materials design strategies. Here, a first-principles based model for property prediction in such complex semiconductor materials is presented. This framework incorporates nonequilibrium synthesis, dopants and defects, and the change of the electronic structure with composition and short range order. This approach is applied to ZnSnN2 (ZTN) which has attracted recent interest for photovoltaics. The unintentional oxygen incorporation and its correlation with the cation stoichiometry leads to the formation of a solid solution with dual sublattice mixing. A nonmonotonic doping behavior as a function of the composition is uncovered. Finally, the degenerate doping of near-stoichiometric ZTN, which is detrimental for potential applications, can be lowered into the 1017 cm-3 range in highly off-stoichiometric material, in quantitative agreement with experiments.},
doi = {10.1002/adma.201807406},
journal = {Advanced Materials},
number = 11,
volume = 31,
place = {United States},
year = {2019},
month = {1}
}

Journal Article:
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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Defect physics of the kesterite thin-film solar cell absorber Cu2ZnSnS4
journal, January 2010

  • Chen, Shiyou; Gong, X. G.; Walsh, Aron
  • Applied Physics Letters, Vol. 96, Issue 2, Article No. 021902
  • DOI: 10.1063/1.3275796

Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Convergence of electronic bands for high performance bulk thermoelectrics
journal, May 2011

  • Pei, Yanzhong; Shi, Xiaoya; LaLonde, Aaron
  • Nature, Vol. 473, Issue 7345, p. 66-69
  • DOI: 10.1038/nature09996