Complex Surface Chemistry of Kesterites: Cu/Zn Reordering after Low Temperature Postdeposition Annealing and Its Role in High Performance Devices

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• 作者：Markus Neuschitzer ; Yudania Sanchez ; Tetiana Olar ; Thomas Thersleff ; Simon Lopez-Marino ; Florian Oliva ; Moises Espindola-Rodriguez ; Haibing Xie ; Marcel Placidi ; Victor Izquierdo-Roca ; Iver Lauermann ; Klaus Leifer ; Alejandro P茅rez-Rodriguez ; Edgardo Saucedo
• 刊名：Chemistry of Materials
• 出版年：2015
• 出版时间：August 11, 2015
• 年：2015
• 卷：27
• 期：15
• 页码：5279-5287
• 全文大小：526K
• ISSN：1520-5002

文摘

A detailed study explaining the beneficial effects of low temperature postdeposition annealing combined with selective surface etchings for Cu₂ZnSnSe₄ (CZTSe) based solar cells is presented. After performing a selective oxidizing surface etching to remove ZnSe secondary phases typically formed during the synthesis processes an additional 200 掳C annealing step is necessary to increase device performance from below 3% power conversion efficiency up to 8.3% for the best case. This significant increase in efficiency can be explained by changes in the surface chemistry which results in strong improvement of the CdS/CZTSe heterojunction commonly used in this kind of absorber/buffer/window heterojunction solar cells. XPS measurements reveal that the 200 掳C annealing promotes a Cu depletion and Zn enrichment of the etched CZTSe absorber surface relative to the CZTSe bulk. Raman measurements confirm a change in Cu/Zn ordering and an increase in defect density. Furthermore, TEM microstructural investigations indicate a change of grain boundaries composition by a reduction of their Cu content after the 200 掳C annealing treatment. Additionally, insights in the CdS/CZTSe interface are gained showing a significant amount of Cu in the CdS buffer layer which further helps the formation of a Cu-depleted surface and seems to play an important role in the formation of the pn-heterojunction.