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Atomistic insights into the order-disorder transition in Cu2ZnSnS4 solar cells from Monte Carlo simulations

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Title: Atomistic insights into the order-disorder transition in Cu<inf>2</inf>ZnSnS<inf>4</inf> solar cells from Monte Carlo simulations
Authors: Wallace, SK
Frost, JM
Walsh, A
Item Type: Journal Article
Abstract: Kesterite-structured Cu2ZnSnS4 (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.
Issue Date: 7-Jan-2019
Date of Acceptance: 23-Nov-2018
URI: http://hdl.handle.net/10044/1/65431
DOI: https://dx.doi.org/10.1039/c8ta04812f
ISSN: 2050-7488
Publisher: Royal Society of Chemistry
Start Page: 312
End Page: 321
Journal / Book Title: Journal of Materials Chemistry A
Volume: 7
Issue: 1
Copyright Statement: © 2019 Royal Society of Chemistry.
Publication Status: Published
Online Publication Date: 2018-11-23
Appears in Collections:Faculty of Engineering
Materials