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

Ning Jing Hao, Rui Xue Ding, Chuan Jia Tong*, Keith P. McKenna

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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.

Original languageEnglish
Article number145002
Number of pages8
JournalJournal of Applied Physics
Volume133
Issue number14
DOIs
Publication statusPublished - 14 Apr 2023

Bibliographical note

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).

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