Abnormal spatial heterogeneity governing the charge-carrier mechanism in efficient Ruddlesden-Popper perovskite solar cells

Layered Ruddlesden-Popper perovskite (RPP) photovoltaics have gained substantial attention owing to their excellent air stability. However, their photovoltaic performance is still limited by the unclear real-time charge-carrier mechanism of operating devices. Herein, we report the correlation between the charge-carrier mechanism and the spatially heterogeneous RPP bulks induced by distinct sublattice cations in the state-of-the-art antisolvent-driven RPP devices. In particular, abnormal heterogeneities ranging from the lateral long-range to local sub-grain scale and corresponding charge-carrier behaviours are visualized for triple-cation RPPs. We discovered that such heterogeneities with a unitary 2D/3D hybrid suppress lattice vibrations and reduce Fröhlich interactions by about 2 times, significantly promoting charge-carrier dynamics. Consequently, optimized triple-cation RPP solar cells greatly outperform their mono-cation counterparts. Furthermore, this principle can be applicable irrespective of 2D layer thickness (n > 2) and substrate type. This work provides a rationale for leveraging a disordered structure to stimulate charge-carrier motion and suggests the design principle of low-dimensional perovskites.