Single-Crystal-Assisted In Situ Phase Reconstruction Enables Efficient and Stable 2D/3D Perovskite Solar Cells

Perovskite solar cells (PSCs) that incorporate both two-dimensional (2D) and three-dimensional (3D) phases possess the potential to combine the high stability of 2D PSCs with the superior efficiency of 3D PSCs. Here, we demonstrated in situ phase reconstruction of 2D/3D perovskites using a 2D perovskite single-crystal-assisted method. A gradient phase distribution of 2D RP perovskites was formed after spin-coating a solution of the 2D Ruddlesden–Popper (RP) perovskite single crystal, (DFP)2PbI4, onto the 3D perovskite surface, followed by thermal annealing. The resulting film exhibits much reduced trap density, increased carrier mobility, and superior water resistance. As a result, the optimized 2D/3D PSCs achieved a champion efficiency of 24.87% with a high open-circuit voltage (VOC) of 1.185 V. This performance surpasses the control 3D perovskite device, which achieved an efficiency of 22.43% and a VOC of 1.129 V. Importantly, the unencapsulated device demonstrates significantly enhanced operational stability, preserving over 97% of its original efficiency after continuous light irradiation for 1500 h. Moreover, the extrapolated T80 lifetimes surpass 5700 h. These findings pave the way for rational regulation of the gradient phase distribution at the interface between 2D and 3D perovskites by employing 2D RP perovskite crystals to achieve stable and efficient PSCs.