Investigation of combinatorial coevaporated thin film Cu2ZnSnS4 (II): Beneficial cation arrangement in Cu-rich growth

Cu2ZnSn(S,Se)4 (CZTSSe) is an earth-abundant semiconductor with potential for economical photovoltaic power generation at terawatt scales. In this work, we use Raman scattering to investigate phase coexistence in combinatorial CZTS thin films grown at 325 or 470 °C. The surface of the samples grown...

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Bibliographic Details
Published in:Journal of applied physics 2014-05, Vol.115 (17)
Main Authors: Lund, E. A., Du, H., Hlaing OO, W. M., Teeter, G., Scarpulla, M. A.
Format: Article
Language:English
Subjects:
Antisite defects
Applied physics
Cations
Chemical potential
Combinatorial analysis
Copper
Copper sulfides
Copper zinc tin sulfide
Electric power generation
Organic chemistry
Phase diagrams
Raman spectra
Thin films
Tin
Tin disulfide
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Summary:Cu2ZnSn(S,Se)4 (CZTSSe) is an earth-abundant semiconductor with potential for economical photovoltaic power generation at terawatt scales. In this work, we use Raman scattering to investigate phase coexistence in combinatorial CZTS thin films grown at 325 or 470 °C. The surface of the samples grown at 325 °C is rough except for a prominent specularly reflective band near and along the ZnS-Cu2SnS3 (CTS) tie line in the Cu-Zn-Sn-S quaternary phase diagram. All structurally incoherent secondary phases (SnS2, CuS) exist only as surface phases or are embedded as separate grains, whereas the structurally coherent secondary phase CTS coexists with CZTS in the dense underlying film. In films grown at 325 °C, which are kinetically trapped by the low growth temperature, a change is observed in Cu and Sn site occupancy, evidenced by the shift from cubic-CTS in the Cu-rich region (Cu/Sn > 2) to more tetragonal-CTS in the Sn-rich region (Cu/Sn  2) results in higher cation ordering meaning fewer antisite defects.
ISSN:0021-8979
1089-7550
DOI:10.1063/1.4871665