晶体质量是决定铜锌锡硫硒(Cu2ZnSn(S,Se)4, CZTSSe)吸收层薄膜吸收效率的关键, 旋涂是溶液法制备CZTSSe吸收层的第一步, 因此旋涂方式的选择至关重要。为了探究不同旋涂方式对CZTSSe吸收层薄膜质量和相应器件性能的影响, 分别采用三组不同的旋涂方式制备铜锌锡硫(Cu2ZnSnS4, CZTS)前驱体薄膜及CZTSSe吸收层薄膜, 并利用X射线衍射仪(XRD)、能谱仪(EDS)、显微拉曼光谱仪(Raman)、场发射扫描电子显微镜(FE-SEM)分析了不同旋涂方式对所制备的CZTSSe吸收层薄膜晶体结构、元素成分、相纯度、表面形貌的影响。同时, 采用电流密度-电压(J-V)测试和外量子效率(EQE)测试对CZTSSe吸收层薄膜太阳电池的光电特性进行了表征。结果表明: 旋涂7周期, 且第一周期烘烤之前旋涂2次的效果最好, 所制备的CZTS前驱体薄膜均匀, 无裂纹, CZTSSe吸收层薄膜结晶度更高, 薄膜表面更平整致密, 晶粒大小更均匀, 实现了9.63%的光电转换效率。通过对采用不同旋涂方式制备的器件的性能参数进行统计分析, 得出新的旋涂方式可以提高CZTSSe薄膜太阳电池的可重复性, 为将来可能的大规模商业化应用做铺垫。

The crystal quality is the key to determining the absorption efficiency of the copper-zinc-tin-sulfur-selenium (Cu2ZnSn(S,Se)4, CZTSSe) absorber layer thin film, and spin coating is the first step in the preparation of the CZTSSe absorber layer by solution method, therefore, the choice of the spin coating method is crucial. To explore the effects of different spin coating modes on the quality of CZTSSe absorber layer thin film and the performance of corresponding devices, three groups of copper-zinc-tin-sulfur (Cu2ZnSnS4, CZTS) precursor thin films were prepared by different spin coating modes and the effects of different spin coating modes on the crystal structure, element composition, phase purity and surface morphology of CZTSSe absorber layer thin films were analyzed by X-ray diffractometer (XRD), energy dispersive spectrometer (EDS), Renishaw Raman system (Raman), and field emission scanning electron microscope (FE-SEM), separately. At the same time, the photoelectric characteristics of the CZTSSe thin film solar cell were characterized by current density-voltage (J-V) characteristic and external quantum efficiency (EQE) tests. The results show that the spin coating mode with 7 cycles and 2 times spin coatings before each baking in the first cycle result in uniform CZTS precursor thin films without cracks, higher crystallinity of CZTSSe absorber layer thin films, flatter, and denser film surface, and more uniform grain size. As a result, the CZTSSe thin film solar cell with a photoelectric conversion efficiency of 9.63% is realized. Through the statistical analysis of the performance parameters of devices based on different spin coating modes, it concludes that the new spin coating modes can improve the repeatability of CZTSSe thin film solar cells and pave the way for possible large-scale commercial applications in the future.