Intermediate-phase-assisted low-temperature formation of γ-CsPbI3 films for high-efficiency deep-red light-emitting devices

Black phase CsPbI3 is attractive for optoelectronic devices, while usually it has a high formation energy and requires an annealing temperature of above 300 degrees C. The formation energy can be significantly reduced by adding HI in the precursor. However, the resulting films are not suitable for light-emitting applications due to the high trap densities and low photoluminescence quantum efficiencies, and the low temperature formation mechanism is not well understood yet. Here, we demonstrate a general approach for deposition of gamma -CsPbI3 films at 100 degrees C with high photoluminescence quantum efficiencies by adding organic ammonium cations, and the resulting light-emitting diode exhibits an external quantum efficiency of 10.4% with suppressed efficiency roll-off. We reveal that the low-temperature crystallization process is due to the formation of low-dimensional intermediate states, and followed by interionic exchange. This work provides perspectives to tune phase transition pathway at low temperature for CsPbI3 device applications. Exploiting low-temperature formed black phase CsPbI3 for light-emitting applications remains a challenge. Here, the authors propose a method to enable the deposition of gamma -CsPbI3 films at 100C and demonstrate a light-emitting diode with an external quantum efficiency of 10.4% with suppressed efficiency roll-off.