Density-functional theory computer simulations of CZTS0.25Se0.75 alloy phase diagrams

Chagarov, E.; Sardashti, K.; Haight, R.; Mitzi, D. B.; Kummel, A. C.

doi:10.1063/1.4959591

Title: Density-functional theory computer simulations of CZTS_0.25Se_0.75 alloy phase diagrams

Journal Article · Tue Aug 09 00:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4959591· OSTI ID:1467855

Chagarov, E. ^[1]; Sardashti, K. ^[1]; Haight, R. ^[2]; Mitzi, D. B. ^[3]; Kummel, A. C. ^[1]

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

Here, density-functional theory simulations of CZTS, CZTSe, and CZTS_0.25Se_0.75 photovoltaic compounds have been performed to investigate the stability of the CZTS_0.25Se_0.75 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 CZTS_0.25Se_0.75 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 CZTS_0.25Se_0.75 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 CZTS_0.25Se_0.75 in a thermodynamically stable state to minimize phase decomposition.

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Research Organization:: International Business Machines Corp. (IBM), Yorktown Heights, NY (United States). Thomas J. Watson Research Center

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0006334

OSTI ID:: 1467855

Alternate ID(s):: OSTI ID: 1287751

Journal Information:: Journal of Chemical Physics, Vol. 145, Issue 6; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 10 works

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Title: Density-functional theory computer simulations of CZTS_0.25Se_0.75 alloy phase diagrams