Layer-controllable synthesis, lattice structural Determination, and fluorescence lifetime imaging of (HA)2(MA)n-1PbnI3n+1 Quasi-2D organic-inorganic perovskite microsheets

Hybrid quasi-two-dimensional (quasi-2D) perovskites have attracted great interest due to their excellent photovoltaic and light-emitting properties, which enable the rapid development of high-performance perovskite-based solar cells, light-emitting diodes, and lasers. Although many efforts have been made to improve the quality and stability of organic-inorganic perovskites, the controlled synthesis of high-quality layered perovskites remains challenging. Here, single-crystalline quasi-2D (HA)2(MA)n-1PbnI3n+1 perovskites with layer numbers of n from 1 to 3 have been synthesized in a controllable manner, exhibiting stable lattice structures and tunable optical emission. Structurally, hexylamine (HA) with longer alkyl chains was used as an organic spacer in Ruddlesden-Popper (RP) phase perovskites to improve the chemical stability of perovskites. Various ratios of precursor materials were adopted for separating pure and large-scale quasi-2D (HA)2(MA)n-1PbnI3n+1 perovskites, in which different layer-number perovskites with tunable band gaps were obtained with the modulated fluorescence lifetimes. Our lattice structural and fluorescence-lifetime characterizations of RP-phase perovskites provide critical information on the emerging quasi-2D perovskite-crystal systems and their fluorescence relaxation dynamics. The employed strategy to synthesize high-quality perovskites (HA)2(MA)n-1PbnI3n+1 is technically essential to develop the rising perovskite-based photovoltaic and light-emitting applications. [Display omitted] •Hybrid quasi-two-dimensional (quasi-2D) perovskites have attracted great interest due to their excellent photovoltaic and light-emitting properties, which enable the rapid development of high-performance perovskite-based solar cells, light-emitting diodes, and lasers. Although many efforts have been made to improve the quality and stability of organic-inorganic perovskites, the controlled synthesis of high-quality layered perovskites remains challenging. Here, single-crystalline quasi-2D (HA)2(MA)n-1PbnI3n+1 perovskites with layer numbers of n from 1 to 3 have been synthesized in a controllable manner, exhibiting stable lattice structures and tunable optical emission. Structurally, hexylamine (HA) with longer alkyl chains was used as an organic spacer in Ruddlesden-Popper (RP) phase perovskites to improve the chemical stability of perovskites. Various ratios of precursor materials were adopted for separating pure and large-scale quasi-2D (HA)2(MA)n-