Defect Engineering in Earth-Abundant Cu_(2)ZnSnSe_(4) Absorber Using Efficient Alkali Doping for Flexible and Tandem Solar Cell Applications

To demonstrate flexible and tandem device applications,a low-temperature Cu_(2)ZnSnSe_(4)(CZTSe)deposition process,combined with efficient alkali doping,was developed.First,high-quality CZTSe films were grown at 480℃by a single co-evaporation,which is applicable to polyimide(PI)substrate.Because of the alkali-free substrate,Na and K alkali doping were systematically studied and optimized to precisely control the alkali distribution in CZTSe.The bulk defect density was significantly reduced by suppression of deep acceptor states after the(NaF+KF)PDTs.Through the low-temperature deposition with(NaF+KF)PDTs,the CZTSe device on glass yields the best efficiency of 8.1%with an improved Voc deficit of 646 mV.The developed deposition technologies have been applied to PI.For the first time,we report the highest efficiency of 6.92%for flexible CZTSe solar cells on PI.Additionally,CZTSe devices were utilized as bottom cells to fabricate four-terminal CZTSe/perovskite tandem cells because of a low bandgap of CZTSe(~1.0 eV)so that the tandem cell yielded an efficiency of 20%.The obtained results show that CZTSe solar cells prepared by a low-temperature process with in-situ alkali doping can be utilized for flexible thin-film solar cells as well as tandem device applications.