Atomistic insights into the order-disorder transition in Cu 2 ZnSnS 4 solar cells from Monte Carlo simulations

Suzanne K. Wallace, Jarvist Moore Frost, Aron Walsh

Research output: Contribution to journalArticle

1 Citations (Scopus)

Abstract

Kesterite-structured Cu 2 ZnSnS 4 (CZTS) is an earth-abundant and non-toxic semiconductor that is being studied for use as the absorber layer in thin-film solar cells. Currently, the power-conversion efficiencies of this technology fall short of the requirements for commercialisation. Disorder in the Cu-Zn sub-lattice has been observed and is proposed as one explanation for the shortcomings of CZTS solar cells. Cation site disorder averaged over a macroscopic sample does not provide insights into the microscopic cation distribution that will interact with photogenerated electrons and holes. To provide atomistic insight into Cu/Zn disorder, we have developed a Monte Carlo (MC) model based on pairwise electrostatic interactions. Substitutional disorder amongst Cu and Zn ions in Cu-Zn (001) planes on the 2c and 2d Wyckoff sites-2D disorder-has been proposed as the dominant form of Cu/Zn disorder in near-stoichiometric crystals. We use our model to study the Cu/Zn order-disorder transition in 2D but also allow Zn to substitute onto the Cu 2a site-3D disorder-including Cu-Sn (001) planes. We find that defects are less concentrated in Cu-Sn (001) planes but that Zn ions readily substitute onto the Cu 2a site and that the critical temperature is lowered for 3D disorder.

Original languageEnglish
Pages (from-to)312-321
Number of pages10
JournalJournal of Materials Chemistry A
Volume7
Issue number1
DOIs
Publication statusPublished - 2019 Jan 1

Fingerprint

Order disorder transitions
Cations
Solar cells
Positive ions
Ions
Coulomb interactions
Conversion efficiency
Earth (planet)
Semiconductor materials
Defects
Crystals
Electrons
Temperature
Monte Carlo simulation
Thin film solar cells

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

Cite this

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abstract = "Kesterite-structured Cu 2 ZnSnS 4 (CZTS) is an earth-abundant and non-toxic semiconductor that is being studied for use as the absorber layer in thin-film solar cells. Currently, the power-conversion efficiencies of this technology fall short of the requirements for commercialisation. Disorder in the Cu-Zn sub-lattice has been observed and is proposed as one explanation for the shortcomings of CZTS solar cells. Cation site disorder averaged over a macroscopic sample does not provide insights into the microscopic cation distribution that will interact with photogenerated electrons and holes. To provide atomistic insight into Cu/Zn disorder, we have developed a Monte Carlo (MC) model based on pairwise electrostatic interactions. Substitutional disorder amongst Cu and Zn ions in Cu-Zn (001) planes on the 2c and 2d Wyckoff sites-2D disorder-has been proposed as the dominant form of Cu/Zn disorder in near-stoichiometric crystals. We use our model to study the Cu/Zn order-disorder transition in 2D but also allow Zn to substitute onto the Cu 2a site-3D disorder-including Cu-Sn (001) planes. We find that defects are less concentrated in Cu-Sn (001) planes but that Zn ions readily substitute onto the Cu 2a site and that the critical temperature is lowered for 3D disorder.",
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Atomistic insights into the order-disorder transition in Cu 2 ZnSnS 4 solar cells from Monte Carlo simulations . / Wallace, Suzanne K.; Frost, Jarvist Moore; Walsh, Aron.

In: Journal of Materials Chemistry A, Vol. 7, No. 1, 01.01.2019, p. 312-321.

Research output: Contribution to journalArticle

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