title: Cu2ZnSnSe4 nanocrystals capped with S(2-) by ligand exchange: utilizing energy level alignment for efficiently reducing carrier rec ombination.
abstract: In this work, we employed a convenient one-step synthesis method for synthesizing Cu2ZnSnSe4 (CZTSe) nanocrystals (NCs) in an excess selenium environment. This excess selenium situation enhanced the reaction of metal acetylacetonates with selenium, resulting in the burst nucleation of NCs at relatively low temperatures. The phase morphology and surface and optoelectronic properties of NCs before and after ligand exchange were discussed in depth. It was found that pure tetragonal-phase structure CZTSe NCs with approximately 1.7-eV bandgap could be synthesized. The removal of large organic molecules on CZTSe NCs after ligand exchange by S(2-) decreased the resistivity. The bandgap of the films after ligand exchange by 550°C selenization was also decreased due to better crystallinity. For potential application in CZTSe solar cells, we constructed an energy level diagram to explain the mutual effect between the absorption layer and CdS layer. Using cyclic voltammetry (CV) measurement, we found that the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energy levels of CZTSe films shifted down after ligand exchange. After energy level alignment at the CdS/CZTSe interface, a type I band alignment structure was more conveniently formed after ligand exchange. This structure acted as the barrier against injection electrons from ZnO to the CZTSe layer, and recombination would subsequently be depressed.
authors.affiliation: The Key Laboratory for Special Functional Materials of MOE, Henan University, Kaifeng 475004, China.
authors.forename: Xia
authors.initials: X
authors.lastname: Wang
authors.affiliation: The Key Laboratory for Special Functional Materials of MOE, Henan University, Kaifeng 475004, China.
authors.forename: Dong-Xing
authors.initials: DX
authors.lastname: Kou
authors.affiliation: The Key Laboratory for Special Functional Materials of MOE, Henan University, Kaifeng 475004, China.
authors.forename: Wen-Hui
authors.initials: WH
authors.lastname: Zhou
authors.affiliation: The Key Laboratory for Special Functional Materials of MOE, Henan University, Kaifeng 475004, China.
authors.forename: Zheng-Ji
authors.initials: ZJ
authors.lastname: Zhou
authors.affiliation: The Key Laboratory for Special Functional Materials of MOE, Henan University, Kaifeng 475004, China.
authors.forename: Si-Xin
authors.initials: SX
authors.lastname: Wu
authors.affiliation: Institute of Oceanographic Instrumentation, Shandong Academy of Sciences, Qingdao 266061, China.
authors.forename: Xuan
authors.initials: X
authors.lastname: Cao
keywords: CZTSe NCs; Energy level alignment; Ligand exchange; One-step synthesis