Atomistic insights into the order-disorder transition in Cu<inf>2</inf>ZnSnS<inf>4</inf> solar cells from Monte Carlo simulations
File(s)Accepted.pdf (2.64 MB)
Accepted version
Author(s)
Wallace, SK
Frost, JM
Walsh, A
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.
Date Issued
2019-01-07
Date Acceptance
2018-11-23
Citation
Journal of Materials Chemistry A, 2019, 7 (1), pp.312-321
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
Date Publish Online
2018-11-23