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2D Ruddlesden–Popper perovskites (RPPs) are emerging as potential challengers to their 3D counterpart due to superior stability and competitive efficiency. However, the fundamental questions on energetics of the 2D RPPs are not well understood. Here, the energetics at (PEA)2(MA)n−1PbnI3n+1/[6,6]‐phenyl‐C61‐butyric acid methyl ester (PCBM) interfaces with varying n values of 1, 3, 5, 40, and ∞ are systematically investigated. It is found that n–n junctions form at the 2D RPP interfaces (n = 3, 5, and 40), instead of p–n junctions in the pure 2D and 3D scenarios (n = 1 and ∞). The potential gradient across phenethylammonium iodide ligands that significantly decreases surface work function, promotes separation of the photogenerated charge carriers with electron transferring from perovskite crystal to ligand at the interface, reducing charge recombination, which contributes to the smallest energy loss and the highest open‐circuit voltage (Voc) in the perovskite solar cells (PSCs) based on the 2D RPP (n = 5)/PCBM. The mechanism is further verified by inserting a thin 2D RPP capping layer between pure 3D perovskite and PCBM in PSCs, causing the Voc to evidently increase by 94 mV. Capacitance–voltage measurements with Mott–Schottky analysis demonstrate that such Voc improvement is attributed to the enhanced potential at the interface.

Organometal halide perovskites exhibit a bright future for applications in solar cells, as efficiency has achieved over 22%. The long‐term stability remains a major obstacle for commercialization. Here, it is found that three cationic compositional engineered perovskites, MAPb(I0.83Br0.17)3, FA0.83MA0.17Pb(I0.83Br0.17)3, and Cs0.1(FA0.83MA0.17)0.9Pb(I0.83Br0.17)3, undergo severe degradation under white‐light illumination in ultrahigh vacuum (UHV) environment, but the rate of degradation is significantly lower for the mixed cation perovskites. This is attributed to the defect‐induced trap states that trigger the strong coupling between the photoexcited carriers and the crystal lattice. The observed behavior supports the view of the mixed cations suppressing the photoinduced degradation. It is further demonstrated that UHV environment remarkably accelerates the degradation of the perovskite films under illumination, which delivers a very important message that the current hybrid perovskite materials and their optoelectronic devices are not suitable for application in outer space. Moreover, the applied UHV environment can be an accelerated test method to estimate the photostability of the perovskites.

The fast evolution of metal halide perovskite solar cells has opened a new chapter in the field of renewable energy. High-quality perovskite films as the active layers are essential for both high efficiency and long-term stability. Here, the perovskite films with enlarged crystal grain size and decreased defect density are fabricated by introducing the extremely low-cost and green polymer, ethyl cellulose (EC), into the perovskite layer. The addition of EC triggers hydrogen bonding interactions between EC and the perovskite, passivating the charge defect traps at the grain boundaries. The long chain of EC further acts as a scaffold for the perovskite structure, eliminating the annealing-induced lattice strain during the film fabrication process. The resulting devices with the EC additive exhibit a remarkably enhanced average power conversion efficiency from 17.11 to 19.27% and an improvement of all device parameters. The hysteresis index is found to decrease by three times from 0.081 to 0.027, which is attributed to suppressed ion migration and surface charge trapping. In addition, the defect passivation by EC significantly improves the environmental stability of the perovskite films, yielding devices that retain 80% of their initial efficiency after 30 days in ambient air at 45% relative humidity, whereas the pristine devices without EC fully degrade. This work provides a low-cost and green avenue for passivating defects that improves both the efficiency and operational stability of perovskite solar cells.