L₂[GA_xFA_1–xPbI₃]PbI₄ (0 ≤ x ≤ 1) Ruddlesden–Popper Perovskite Nanocrystals for Solar Cells and Light-Emitting Diodes

The main challenges to overcome for colloidal 2D Ruddlesden–Popper (RP) organo-lead iodide perovskite nanocrystals (NCs) are phase instability and low photoluminescence quantum yield (PLQY). Herein, we demonstrate colloidal synthesis of guanidinium (GA)-L2[GAPbI3]PbI4, formamidinium (FA)-L2[FAPbI3]PbI4, and GA and FA alloyed L2[GA0.5FA0.5PbI3]PbI4 NCs without using polar or high boiling point nonpolar solvents. Importantly, we show that optical properties and phase stability of L2[APbI3]PbI4 NCs can be affectively tuned by alloying with guanidinium and formamidinium cations. Additionally, the band gap of NCs can be rapidly engineered by bromide ion exchange in L2[GAxFA1–xPbI3]PbI4 (0 ≤ x ≤ 1) NCs. Our approach produces a stable dispersion of L2[FAPbI3]PbI4 NCs with 12.6% PLQY that is at least three times higher than the previously reported PLQY in the nanocrystals. Furthermore, L2[GAPbI3]PbI4 and L2[GA0.5FA0.5PbI3]PbI4 NC films exhibit improved ambient stability over 10 days, which is significantly higher than L2[FAPbI3]PbI4 NC films, which transform to an undesired 1D phase within 6 days. The colloidally synthesized guanidinium- and formamidinium-based 2D RP organo-lead iodide perovskite NCs with improved stability and high PLQY demonstrated in this study may find applications in solar cells and light-emitting diodes. Therefore, large A-site cation-alloyed 2D RP perovskite NCs may provide a new way to rationalize high-performance and stable perovskite solar cells and light-emitting diodes.