Interface Molecular Engineering for Laminated Monolithic Perovskite/Silicon Tandem Solar Cells with 80.4% Fill Factor

A multipurpose interconnection layer based on poly(3,4-ethylenedioxythiophene) doped with poly(styrene sulfonate) (PEDOT:PSS), and d-sorbitol for monolithic perovskite/silicon tandem solar cells is introduced. The interconnection of independently processed silicon and perovskite subcells is a simple add-on lamination step, alleviating common fabrication complexities of tandem devices. It is demonstrated experimentally and theoretically that PEDOT:PSS is an ideal building block for manipulating the mechanical and electrical functionality of the charge recombination layer by controlling the microstructure on the nano- and mesoscale. It is elucidated that the optimal functionality of the recombination layer relies on a gradient in the d-sorbitol dopant distribution that modulates the orientation of PEDOT across the PEDOT:PSS film. Using this modified PEDOT:PSS composite, a monolithic two-terminal perovskite/silicon tandem solar cell with a steady-state efficiency of 21.0%, a fill factor of 80.4%, and negligible open circuit voltage losses compared to single-junction devices is shown. The versatility of this approach is further validated by presenting a laminated two-terminal monolithic perovskite/organic tandem solar cell with 11.7% power conversion efficiency. It is envisioned that this lamination concept can be applied for the pairing of multiple photovoltaic and other thin film technologies, creating a universal platform that facilitates mass production of tandem devices with high efficiency.