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The development of efficient all perovskite tandem solar cells has faced challenges related to current matching and optical losses. In this work, a design of a non‐coplanar three‐terminal (3T) all perovskite tandem solar cell is presented, which consists of a p‐i‐n inverted NiOX‐based CsPbI2Br perovskite top cell, and a FA0.6MA0.4Sn0.5Pb0.5I3 perovskite bottom cell with back‐contact (BC) device structure. It effectively mitigated the optical losses introduced in non‐absorbing layers and resulted in a 2.9% absolute efficiency improvement compared to that of planar sandwich‐type 3T tandems. Both optical and electrical characteristics of the multi‐terminal tandem cells are investigated. Then, it is focused on understanding the impact of top cell thickness on overall non‐coplanar BC 3T‐tandem performance, considering low‐energy photon optical reflection and carrier transport distance. Following optimizations of energy level and device structure, an efficiency of 32.16% is achieved, with non‐coplanar BC 3T device architecture: top cell consisting of hole extraction layer (ITO/NiOx), CsPbI2Br absorber layer, and electron extraction layer (ZnO/FA0.6MA0.4Sn0.5Pb0.5I3/SnO2/Ag); and bottom cell (Ni/NiOx/FA0.6MA0.4Sn0.5Pb0.5I3/SnO2/Ag); bottom perovskite layer has two functions, one is electron transport layer for top cell, and the other is low‐energy photon absorption layer in bottom cell. It provides insight and a promising pathway for manufacturing high‐efficient all perovskite tandem solar cells. [ABSTRACT FROM AUTHOR]

Nickel oxide (NiOX) has a crucial role in enhancing the efficiency and stability of p‐i‐n inverted perovskite solar cells (PSCs), which hold great potential for commercialization. However, improving contact passivation between perovskites and NiOX is a challenge due to a hindered buried interface. In order to address this issue, self‐assembled monolayers (SAMs) are introduced as a buffer layer to prevent direct contact and non‐radiative recombination. While, the large dipole moment of SAMs increases the work function of NiOX, which is crucial for enhancing hole transport performance, given the low interfacial potential barrier for hole transfer. By a combination of the first‐principles calculations, drive‐level capacitance profiling, and transient absorption spectrum characterization, the understanding of the ion‐dipole interactions and interface passivation mechanism of potassium fluoride (KF) ultra‐thin buffer layer between SAMs and perovskites is provided. The efficiency of inverted PSCs as high as 23.25% is obtained, and the unencapsulated devices kept 90% of initial efficiency following 1400 h aging under nitrogen, which demonstrate remarkable long‐term stability as well. This novel strategy highlights the significance of SAMs dipole moment at the NiOX/perovskites interface and provides a new approach to address buried interfaces for high‐efficiency and long‐term stability in inverted PSCs. [ABSTRACT FROM AUTHOR]