Lone-pair effect on carrier capture in Cu2ZnSnS4 solar cells
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Published version
Author(s)
Kim, Sunghyun
Park, Ji-Sang
Hood, SamanthaN
Walsh, Aron
Type
Journal Article
Abstract
The performance of kesterite thin-film solar cells is limited by a low open-circuit voltage due to defect-mediated electron–hole recombination. We calculate the non-radiative carrier-capture cross sections and Shockley–Read–Hall recombination coefficients of deep-level point defects in Cu2ZnSnS4 (CZTS) from first-principles. While the oxidation state of Sn is +4 in stoichiometric CZTS, inert lone pair (5s2) formation lowers the oxidation state to +2. The stability of the lone pair suppresses the ionization of certain point defects, inducing charge transition levels deep in the band gap. We find large lattice distortions associated with the lone-pair defect centers due to the difference in ionic radii between Sn(II) and Sn(IV). The combination of a deep trap level and large lattice distortion facilitates efficient non-radiative carrier capture, with capture cross-sections exceeding 10−12 cm2. The results highlight a connection between redox active cations and ‘killer’ defect centres that form giant carrier traps. This lone pair effect will be relevant to other emerging photovoltaic materials containing ns2 cations.
Date Issued
2019-02-14
Date Acceptance
2019-01-05
Citation
Journal of Materials Chemistry A, 2019, 7 (6), pp.2686-2693
ISSN
2050-7496
Publisher
Royal Society of Chemistry
Start Page
2686
End Page
2693
Journal / Book Title
Journal of Materials Chemistry A
Volume
7
Issue
6
Copyright Statement
© The Royal Society of Chemistry 2019. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (https://creativecommons.org/licenses/by/3.0/)
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000457893400028&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Energy & Fuels
Materials Science, Multidisciplinary
Chemistry
Materials Science
POINT-DEFECTS
RECOMBINATION
EFFICIENCY
LIMIT
Publication Status
Published
Date Publish Online
2019-01-21