Potassium doping for grain boundary passivation and defect suppression enables highly-efficient kesterite solar cells

The complicated and diverse deep defects, voids, and grain boundary in the CZTSSe absorber are the main reasons for carrier recombination and efficiency degradation. The further improvement of the open-circuit voltage and fill factor so as to increase the efficiency of CZTSSe device is urgent. In this work, we obtained K-doped CZTSSe absorber by a simple solution method. The medium-sized K atoms, which combine the advantages of light and heavy alkali metals, are able to enter the grain interior as well as segregate at grain boundary. The K-Se liquid phase can improve the absorber crystallinity. We find that the accumulation of the wide bandgap compound K2Sn2S5 at grain boundary can increase the contact potential difference of grain boundary, form more effective hole barriers, and enhance the charge separation ability. At the same time, K doping passivates the interface as well as bulk defects and suppresses the non-radiative recombination. The improved crystallinity, enhanced charge transport capability and reduced defect density due to K doping result in a significant enhancement of the carrier lifetime, leading to 13.04% device efficiency. This study provides a new idea for simultaneous realization of grain boundary passivation and defect suppression in inorganic kesterite solar cells.