“…Among the substitutes to traditional energy, economic and environmental-friendly solar energy has the most extensive development prospect because of its great potential in meeting the supply of large-scale low-carbon electricity in the future. − In the numerous photovoltaic (PV) devices, crystalline silicon (c-Si), which occupies a very important position in the PV field, is gradually being replaced by metal chalcogenide-based thin-film PV technology due to c-Si’s high processing cost and complex manufacturing process . Among the different chalcogenide PV devices, only Cu(In,Ga)Se 2 (CIGSe) and CdTe devices have met efficiency requirements for commercial production. − However, the disadvantages of In, Ga, Te, and Cd, such as toxic properties, high cost, and shortage of element reserves, limit their large-scale development. , Cu 2 ZnSn(S,Se) 4 (CZTSSe) is a derivative of commercialized CIGSe devices with similar structure and optoelectronic properties, which is rich in earth resources, low in production cost, and friendly for environmental protection. − Furthermore, the theoretical Shockley–Queisser limits for CZTS, CZTSe, and CZTSSe solar cells are 32.4, 31.6, and 31.0%, respectively, which are higher than that for CIGSe of 31.0%. − Due to the similar properties, the development experience of CIGSe solar cells can provide great technical support for CZTSSe solar cells . Thus, CZTSSe is considered as an absorber layer material with bright prospect in the field of PV devices.…”