Interaction of C60 with Methylammonium Lead Iodide Perovskite Surfaces: Unveiling the Role of C60 in Surface Engineering

Abstract Understanding the interaction between fullerene (C 60 ) and perovskite surfaces is pivotal for advancing the efficiency and stability of perovskite solar cells. In this study, we investigate the adsorption behavior of C 60 on methylammonium lead iodide (MAPbI 3 ) surfaces using periodic density functional theory calculations. We explore various surface terminations and defect configurations to elucidate the influence of surface morphology on the C 60 ‐perovskite interaction, computing the adsorption energy and transfer of charge. Our results reveal distinct adsorption energies and charge transfer mechanisms for different surface terminations, shedding light on the role of surface defects in modifying the electronic structure and stability of perovskite materials. Furthermore, we provide insights into the potential of C 60 to passivate surface defects, playing a relevant role in the surface reconstruction after the formation of defects. This comprehensive understanding of C 60 ‐perovskite interactions offers valuable guidelines about the role of fullerenes on surface structure and reconstruction.