Heterogeneity of grain boundary properties in Cu2ZnSnS4:A first-principles study

Abstract

Using first-principles density functional calculations, we investigate the structure and properties of previously unstudied grain boundaries (GBs) in the solar absorber material copper-zinc-tin-sulfide (CZTS). We identify four stable low-ς value symmetric tilt GBs with low formation energies: ς3 (111) and ς5 (201), each with two different GB terminations. Compared to CdTe and CuInSe, GBs in the quaternary semiconductor CZTS exhibit a wider variety of electronic states due to the more complex chemical environment near the GB, including under-coordinated atoms and dangling bonds. Further analysis confirms that strong dangling bonds introduce deep gap states in all GBs studied. We also investigate segregation and electronic properties of intrinsic point defects to GBs and find that one of the ς3 (111) GBs exhibits an abnormal defect segregation behavior that favors Cu-poor (Zn-rich) GB composition, which is beneficial for its overall performance.

Metadata

Item Type:	Article
Authors/Creators:	Hao, Ning Jing Ding, Rui Xue Tong, Chuan Jia McKenna, Keith P. https://orcid.org/0000-0003-0975-3626
Copyright, Publisher and Additional Information:	Funding Information: C.-J.T. acknowledges support by the National Natural Science Foundation (No. 12104515). N.-J.H. and R.-X.D. acknowledge support from National College Students' innovation and entrepreneurship training program (No. 2022105330185). K.P.M. acknowledges support from EPSRC (Nos. EP/K003151/1, EP/P006051/1, and EP/P023843/1). This work made use of the facilities of Archer, the United Kingdom's national high-performance computing service, via our membership in the UK HPC Materials Chemistry Consortium, which is funded by EPSRC (Nos. EP/L000202/1 and EP/R029431/1). This project also made use of the Viking Cluster, which is a high-performance computation facility provided by the University of York. We are grateful for resources from the High-Performance Computing Center of Central South University and Hefei Advanced Computing Center. All data created during this research are available by request from the University of York Research database at https://doi.org/10.15124/32bf9075-80ee-4f08-b93c-53f2398d7c84 . Publisher Copyright: © 2023 Author(s).
Dates:	Published: 14 April 2023 Accepted: 25 March 2023
Institution:	The University of York
Academic Units:	The University of York > Faculty of Sciences (York) > Physics (York)
Depositing User:	Pure (York)
Date Deposited:	01 Jun 2023 09:20
Last Modified:	27 Nov 2024 00:46
Published Version:	https://doi.org/10.1063/5.0147435
Status:	Published
Refereed:	Yes
Identification Number:	10.1063/5.0147435
Related URLs:	http://www.scopus.com/inward/record.url?...
Open Archives Initiative ID (OAI ID):	oai:eprints.whiterose.ac.uk:199838

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Heterogeneity of grain boundary properties in Cu2ZnSnS4:A first-principles study

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