Density-functional theory computer simulations of CZTS0.25Se0.75 alloy phase diagrams
Abstract
Here, density-functional theory simulations of CZTS, CZTSe, and CZTS0.25Se0.75 photovoltaic compounds have been performed to investigate the stability of the CZTS0.25Se0.75 alloy vs. decomposition into CZTS, CZTSe, and other secondary compounds. The Gibbs energy for vibrational contributions was estimated by calculating phonon spectra and thermodynamic properties at finite temperatures. It was demonstrated that the CZTS0.25Se0.75 alloy is stabilized not by enthalpy of formation but primarily by the mixing contributions to the Gibbs energy. The Gibbs energy gains/losses for several decomposition reactions were calculated as a function of temperature with/without intermixing and vibration contributions to the Gibbs energy. A set of phase diagrams was built in the multidimensional space of chemical potentials at 300 K and 900 K temperatures to demonstrate alloy stability and boundary compounds at various chemical conditions. It demonstrated for CZTS0.25Se0.75 that the chemical potentials for stability differ between typical processing temperature (~900 K) and operating temperature (300 K). This implies that as cooling progresses, the flux/concentration of S should be increased in MBE growth to maintain the CZTS0.25Se0.75 in a thermodynamically stable state to minimize phase decomposition.
- Authors:
-
- Univ. of California, San Diego, CA (United States). Dept. of Chemistry and Biochemistry
- International Business Machines Corp. (IBM), Yorktown Heights, NY (United States). Thomas J. Watson Research Center
- Duke Univ., Durham, NC (United States). Dept. of Mechanical Engineering and Materials Science
- Publication Date:
- Research Org.:
- International Business Machines Corp. (IBM), Yorktown Heights, NY (United States). Thomas J. Watson Research Center
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1467855
- Alternate Identifier(s):
- OSTI ID: 1287751
- Grant/Contract Number:
- EE0006334
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 145; Journal Issue: 6; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 14 SOLAR ENERGY; decomposition reactions; phonons; solar cells; density functional theory; zinc; entropy; Gibbs free energy; II-VI semiconductors; phase diagrams; chemical potential
Citation Formats
Chagarov, E., Sardashti, K., Haight, R., Mitzi, D. B., and Kummel, A. C. Density-functional theory computer simulations of CZTS0.25Se0.75 alloy phase diagrams. United States: N. p., 2016.
Web. doi:10.1063/1.4959591.
Chagarov, E., Sardashti, K., Haight, R., Mitzi, D. B., & Kummel, A. C. Density-functional theory computer simulations of CZTS0.25Se0.75 alloy phase diagrams. United States. https://doi.org/10.1063/1.4959591
Chagarov, E., Sardashti, K., Haight, R., Mitzi, D. B., and Kummel, A. C. Tue .
"Density-functional theory computer simulations of CZTS0.25Se0.75 alloy phase diagrams". United States. https://doi.org/10.1063/1.4959591. https://www.osti.gov/servlets/purl/1467855.
@article{osti_1467855,
title = {Density-functional theory computer simulations of CZTS0.25Se0.75 alloy phase diagrams},
author = {Chagarov, E. and Sardashti, K. and Haight, R. and Mitzi, D. B. and Kummel, A. C.},
abstractNote = {Here, density-functional theory simulations of CZTS, CZTSe, and CZTS0.25Se0.75 photovoltaic compounds have been performed to investigate the stability of the CZTS0.25Se0.75 alloy vs. decomposition into CZTS, CZTSe, and other secondary compounds. The Gibbs energy for vibrational contributions was estimated by calculating phonon spectra and thermodynamic properties at finite temperatures. It was demonstrated that the CZTS0.25Se0.75 alloy is stabilized not by enthalpy of formation but primarily by the mixing contributions to the Gibbs energy. The Gibbs energy gains/losses for several decomposition reactions were calculated as a function of temperature with/without intermixing and vibration contributions to the Gibbs energy. A set of phase diagrams was built in the multidimensional space of chemical potentials at 300 K and 900 K temperatures to demonstrate alloy stability and boundary compounds at various chemical conditions. It demonstrated for CZTS0.25Se0.75 that the chemical potentials for stability differ between typical processing temperature (~900 K) and operating temperature (300 K). This implies that as cooling progresses, the flux/concentration of S should be increased in MBE growth to maintain the CZTS0.25Se0.75 in a thermodynamically stable state to minimize phase decomposition.},
doi = {10.1063/1.4959591},
journal = {Journal of Chemical Physics},
number = 6,
volume = 145,
place = {United States},
year = {Tue Aug 09 00:00:00 EDT 2016},
month = {Tue Aug 09 00:00:00 EDT 2016}
}
Web of Science
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