Perovskite solar cells (PSCs) have gained tremendous research interest because of their tolerance of defects, low cost, and facile processing. In PSC devices, PbI2 has been utilized to passivate defects at perovskite film surfaces and GBs; however, a systematic mechanism of PbI2 in situ passivation for enhancing the solar cells efficiency has not been fully explored. Here, this work, we systematically studies the effect of the precise PbI2 ratio and the PbI2 in situ passivation mechanism based on trap density, carrier lifetime, Fermi level, and so forth. This study finds the appropriate ratio of I/Pb to be around 2.57:1 using energy-dispersive spectroscopy. After the moderate excess PbI2 in situ passivation, the trap density is reduced from 6.12 × 1016 to 3.38 × 1016 cm-3, and the carrier lifetime is extended from 168.35 to 368.77 ps by using fs-TA spectroscopy. This result indicates that the moderate excess PbI2 in situ passivation can reduce the trap density and suppress the nonradiative recombination. The efficiency of solar cell has shown a nearly 11.3% improvement of 19.55% for an I/Pb ratio of 2.57:1 compared with 2.69:1. It also demonstrates that the efficiency of PSCs can be enhanced effectively by PbI2 in situ passivation.
Keywords: EDS mapping; PbI2; SnO2; passivation mechanism; perovskite solar cells; transient absorption spectroscopy.