“…Significant efforts are being made to improve long-term stability in PSCs. The initial effort was to introduce alloying of A-site cations and halide ions in 3D perovskites. − Surface treatments have been widely employed to passivate surface defects and achieve long-term stability. ,− Another approach involves depositing a 2D perovskite phase on top of the 3D perovskite phase thus creating a 2D/3D architecture for solar cell operation. ,,− ,, In a 2D/3D architecture of perovskite solar cells, the 3D perovskite phase is responsible for efficient photon conversion, while the 2D perovskite phase provides stability against moisture due to the hydrophobic spacer cations. − This architecture has been shown to improve the long-term stability of PSCs at room temperature, and in some cases, even to improve the photon conversion efficiency. ,,− ,,,,, However, studies from several groups, as well as ours, have recently shown the dynamic nature of the 2D/3D interface, as it becomes unstable under thermal stress or light soaking. ,,− The 2D/3D interface undergoes a transformation because of slow cation exchange, thus replacing the sharp 2D/3D interface with a gradient structure of 2D phases (n = 1, 2, 3, ...). − , The cation exchange rate depends on the cation (both A-site and spacer cations), with alkylammonium ions such as butylammonium showing greater mobility under thermal and light stress compared to other more bulky spacer cations. ,− It has been shown that at elevated temperatures, for example at 50 °C, the deterioration of the 2D/3D interface results in the efficiency loss of perovskite solar cells . A r...…”