Cu2ZnSnS4薄膜之硫化製程研究

李銘峰

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Cu2ZnSnS4薄膜之硫化製程研究

Preparation of Cu2ZnSnS4thin films by sulfurization

李銘峰 , Masters　　Advisor：曾百亨　　

繁體中文

薄膜太陽電池； Cu2ZnSnS4 ；前驅物；硫化；快速加熱製程； rapid thermal processing ； sulfurization ； Cu2ZnSnS4 ； precursor ； thin film solar cell

Abstract │ Reference (39) │ Altmetrics

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In this study, a sulfurization process was employed to synthesize Cu2ZnSnS4 (CZTS)
thin films. The process was conducted by the deposition of elemental precursor layers
with the stacking sequence of Zn/Sn/Cu by sputtering on soda glass (soda-lime glass SLG) substrate and followed by thermal annealing in an inert ambient to form the
CZTS film. Both conventional and repaid thermal sulfurization with heating rate of 30℃/min and 5-25℃/sec had been used, respectively, to raise the temperature to 570℃.The duration for annealing was 30 minutes for conventional sulfurization and 1 minute for rapid thermal sulfurization. The samples were then cooled to room temperature with a supply of sulfur vapor until the temperature reached 300℃.Our experimental results on conventional sulfurization showed that single phase of CZTS could be prepared with the preset composition using the Zn/Sn ratio fixed at 1.2 and the Cu/(Zn+Sn) ratio kept between 0.6 and 0.9. The film resistivity was related to chemical composition and  could be controlled between 0.2 and 800 Ω-cm. Optical bandgap of the films was measured to be about 1.5eV and optical absorptioncoefficients were determined to be 104~105cm-1.The film adhesion problem occurred for the films prepared by rapid thermal sulfurization and could be improved by using a heating rate below 5℃/sec. Single-phase CZTS films could be prepared with the preset composition of Zn/Sn = 1.2 and Cu/(Zn + Sn) = 0.75. Its resistivity was measured to be 3000Ω-cm. Optical transmission measurement of this film showed that the bandgap and optical absorption coefficients were 1.48 eV and 104~105cm-1, respectively.In order to improve grain structures and surface morphology of the films, a thin layer of Sb was added between Sn and Zn in the precursor for sulfurization. An Sb layer thickness of 100 nm was suitable for the above mentioned purposes but the reproducibility of this process was still a problem.To promote the formation of liquid phase during the sulfurization processes, Cu had been replaced with CuxSe as part of precursors. The result was not promising because CuxSe might be turned into CuxS and caused the film peeled off.

Reference ( 39 ) 〈TOP〉

1. Philip Jackson, Dimitrios Hariskos, Roland Wuerz, Wiltraud Wischmann, Michael Powalla, Compositional investigation of potassium doped Cu(In,Ga)Se2 solar cells with efficiencies up to 20.8%, physica status solidi (RRL) - Rapid Research Letters, Volume 8, Issue 3, pages 219–222,March 2014
連結：
3. HongxiaWang, Progress in Thin Film Solar Cells Based on Cu2ZnSnS4, Volume 2011, Article ID 801292, 10 pages
連結：
4. QijieGuo, Hugh W. Hillhouse, and Rakesh Agrawal, Synthesis of Cu2ZnSnS4 Nanocrystal Ink and Its Use for Solar Cells,J. AM. CHEM. SOC. 2009, 131, 11672–11673
連結：
7. S.Chen﹐X.G.Gong﹐A.Walsh﹐S.H.Wei﹐Crystal and electronic band structure of Cu2ZnSnX4 (X=Sand Se) photovoltaic absorbers: First-principles insights﹐Appl. Phys. Lett. 94, 041903 (2009)
連結：
8. V.Keraj﹐K.K.Patel﹐S.J.Patel﹐D.V.Shah﹐Synthesis and characterisation of Copper Zinc Tin Sulphide（CZTS）compound for absorber material in solar-cells﹐Journal of Crystal Growth 362（2013）174-177
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