Boosted Structural Stability and Interfacial Charge Transfer in C_mO_nCl_k/[FA,MA]Pb_1+yI₃ Heterostructures

We reported the first-principles computational study of the atomic-scale mechanism underlying the properties of CmOnClk/[FA,MA]Pb1+yI3 heterostructures composed of graphene-related materials CmOnClk and formamidinium and methylammonium lead halide perovskites [FA,MA]Pb1+yI3 (denoting [CH(NH2)2, CH3NH3]Pb1+yI3) with a Pb-rich surface that accounts for the proportion factor “y” of Pb. By investigating the structural and electronic properties, the charge carrier transfer, and the quantum transport of electrons, we revealed that among those graphene-related materials, chlorinated graphene oxide (Cl-GO) has the greatest positive effect on both the charge transfer and extraction rates and the stability of perovskite-based photovoltaics. In addition, our study shows that there are intermediate bands generated near the interfaces in Cl-GO/[FA,MA]Pb1+yI3 heterostructures, which extend the light absorption from the visible light region to the infrared region, enhancing the capability of light absorption of perovskite solar cells.