High Efficiency Perovskite‐Silicon Tandem Solar Cells: Effect of Surface Coating versus Bulk Incorporation of 2D Perovskite

Mixed-dimensional perovskite solar cells combining 3D and 2D perovskites have recently attracted wide interest owing to improved device efficiency and stability. Yet, it remains unclear which method of combining 3D and 2D perovskites works best to obtain a mixed-dimensional system with the advantages of both types. To address this, different strategies of combining 2D perovskites with a 3D perovskite are investigated, namely surface coating and bulk incorporation. It is found that through surface coating with different aliphatic alkylammonium bulky cations, a Ruddlesden–Popper “quasi-2D” perovskite phase is formed on the surface of the 3D perovskite that passivates the surface defects and significantly improves the device performance. In contrast, incorporating those bulky cations into the bulk induces the formation of the pure 2D perovskite phase throughout the bulk of the 3D perovskite, which negatively affects the crystallinity and electronic structure of the 3D perovskite framework and reduces the device performance. Using the surface-coating strategy with n-butylammonium bromide to fabricate semitransparent perovskite cells and combining with silicon cells in four-terminal tandem configuration, 27.7% tandem efficiency with interdigitated back contact silicon bottom cells (size-unmatched) and 26.2% with passivated emitter with rear locally diffused silicon bottom cells is achieved in a 1 cm2 size-matched tandem.This work was supported by the Australian Government through the Australian Renewable Energy Agency (ARENA). T.D. acknowledges the financial support of a Postdoc Fellowship from the Australian Centre for Advanced Photovoltaics (ACAP). T.W. is the recipient of an Australian Research Council Future Fellowship (project number FT180100302) funded by the Australian Government. Furthermore, the authors would like to gratefully acknowledge the financial support by the Helmholtz Association through the HYIG of U.W.P. (FKZ VH-NG-1148), the project PEROSEED (FKZ ZT-0024), the Helmholtz Energy Materials Foundry (HEMF), the Recruitment Initiative of B.S.R. as well as the Karlsruhe School of Optics & Photonics (KSOP)