Improved Ultrafast Carrier Relaxation and Charge Transfer Dynamics in CuI Films and Their Heterojunctions via Sn Doping

CuI is one of the promising hole transport materials for perovskite solar cells. However, its tendency to form defects is currently limiting its use for device applications. Here, we report the successful improvement of CuI through Sn doping and the direct measurement of the carrier relaxation and interfacial charge-transfer processes in Sn-doped CuI films and their heterostructures. Femtosecond-transient absorption (fs-TA) measurements reveal that Sn doping effectively passivates the trap states within the bandgap of CuI. The I-V characteristics of heterostructures demonstrate drastic improvement in transport characteristics upon Sn doping. Fs-TA measurements further confirm that the CuSnI/ZnO heterojunction has a type-II configuration with ultrafast charge transfer (<280 fs). The charge transfer time of a CuI/ZnO heterostructure is ∼2.8 times slower than that of the CuSnI/ZnO heterostructure, indicating that Sn doping suppresses the interfacial states that retard the charge transfer. These results elucidate the effect of Sn doping on the performance of CuI-based heterostructures.