Cation disorder regulation by microstate configurational entropy in photovoltaic absorber materials Cu2ZnSn(S,Se)4

Shunli Shang, Yi Wang, Greta Lindwall, Neal R. Kelly, Tim J. Anderson, Zi-kui Liu

Research output: Contribution to journalArticle

13 Citations (Scopus)

Abstract

Cation disorder plays a major role in the performance deterioration of Cu2ZnSn(S,Se)4 (CZTSSe) photovoltaic (PV) absorbers. Unfortunately the quantitative impact of cation disorder in this material is not well understood. Here, we show that changes in microstate configurational entropy (SMCE), predicted by a combination of statistical mechanics, density functional theory, and phonon calculations, can quantitatively describe cation disorder and the associated properties in CZTSSe. For example, the predicted critical temperature of the second-order phase transition and the thermal expansion anomaly of CZTS based on SMCE are in good agreement with experiments. We further reveal that the more separated is the same kind of cations (Cu, Zn, or Sn), the lower the energy of the corresponding microstate will be, implying the maximum entropy probability distribution of cations at high temperatures. It is suggested that the introduction of SMCE can serve as a framework to quantitatively understand and tailor cation disorder and associated properties for synthesis of the high-quality CZTS-based solar cells.

Original languageEnglish (US)
Pages (from-to)24884-24889
Number of pages6
JournalJournal of Physical Chemistry C
Volume118
Issue number43
DOIs
StatePublished - Oct 30 2014

Fingerprint

absorbers (materials)
Cations
Entropy
Positive ions
disorders
entropy
cations
Statistical mechanics
deterioration
statistical mechanics
Probability distributions
Thermal expansion
Density functional theory
Deterioration
thermal expansion
absorbers
critical temperature
Solar cells
solar cells
Phase transitions

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

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abstract = "Cation disorder plays a major role in the performance deterioration of Cu2ZnSn(S,Se)4 (CZTSSe) photovoltaic (PV) absorbers. Unfortunately the quantitative impact of cation disorder in this material is not well understood. Here, we show that changes in microstate configurational entropy (SMCE), predicted by a combination of statistical mechanics, density functional theory, and phonon calculations, can quantitatively describe cation disorder and the associated properties in CZTSSe. For example, the predicted critical temperature of the second-order phase transition and the thermal expansion anomaly of CZTS based on SMCE are in good agreement with experiments. We further reveal that the more separated is the same kind of cations (Cu, Zn, or Sn), the lower the energy of the corresponding microstate will be, implying the maximum entropy probability distribution of cations at high temperatures. It is suggested that the introduction of SMCE can serve as a framework to quantitatively understand and tailor cation disorder and associated properties for synthesis of the high-quality CZTS-based solar cells.",
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Cation disorder regulation by microstate configurational entropy in photovoltaic absorber materials Cu2ZnSn(S,Se)4. / Shang, Shunli; Wang, Yi; Lindwall, Greta; Kelly, Neal R.; Anderson, Tim J.; Liu, Zi-kui.

In: Journal of Physical Chemistry C, Vol. 118, No. 43, 30.10.2014, p. 24884-24889.

Research output: Contribution to journalArticle

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AU - Wang, Yi

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AU - Kelly, Neal R.

AU - Anderson, Tim J.

AU - Liu, Zi-kui

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