RESUMEN
New perovskite materials of two-dimensional (2D) all-inorganic Ruddlesden-Popper (RP) perovskite Cs6Pb5I16 nanosheets were successfully obtained from the structural transformation of 2D PR-phase Cs7Pb6I19 nanosheets. The 2D RP-phase Cs6Pb5I16 perovskite nanosheets exhibited unique green emission with an emission wavelength of â¼500 nm. The crystal structure of the 2D RP-phase Cs6Pb5I16 perovskite nanosheets was determined by powder X-ray diffraction (XRD), high-resolution transmission electron microscopy, and atomic force microscopy. The time-dependent photoluminescence measurements and XRD spectra were used to observe the optical and structure transformations from 2D Cs7Pb6I19 (n = 6) to 2D Cs6Pb5I16 (n = 5) perovskites. The in situ XRD measurements confirmed that γ-phase CsPbI3 was released during the structural transformation. Moreover, temperature-dependent in situ XRD measurements were employed to examine the kinetic energy involved in the structural transformation from the n = 6 form to the n = 5 form. Specifically, an intermediate structure from n = 6 to n = 5 was also identified. Most importantly, 2D Cs6Pb5I16 (n = 5) was more structurally thermodynamically stable than 2D Cs7Pb6I19 (n = 6). This study provides an essential route for the discovery of new types of perovskite structures during structural transformation.
RESUMEN
Two-dimensional (2D) all-inorganic Ruddlesden-Popper (RP) perovskite Cs7Pb6I19 nanosheets (NSs) were successfully developed for the first time by employing a structural recrystallization process with additional passivation of small organic sulfide molecules. The structure of Cs7Pb6I19 NSs is confirmed by powder X-ray diffraction measurements, atomically-resolved STEM measurements and atomic force microscopy (AFM) studies. Cs7Pb6I19 NSs with a specific n value of 6 exhibits unique absorption and emission spectra with intense excitons at 560 nm due to quantum confinement effects in 2D perovskite slabs. The formation mechanisms of 2D Cs7Pb6I19 NSs and 3D γ-CsPbI3 phases were investigated by in situ photoluminescence (PL) spectroscopy and the activation energies of their formation reactions were calculated to be 151 kJ mol-1 and 95.3 kJ mol-1, respectively. The phase stability of 2D Cs7Pb6I19 NSs can be maintained at temperatures below 14 °C for more than 4 weeks. The overall results indicate that 2D Cs7Pb6I19 NSs demonstrate unique optical properties and structural stability compared with other 3D perovskite materials. We have opened a new path to the future discovery of 2D perovskite structures with metastable phases by using this recrystallization method and the assistance of sulfur-derived organic molecules.
RESUMEN
Various types of 2D organic-inorganic perovskite solar cells have been developed and investigated due to better electron transport behavior and environmental stability. Controlling the formation of phases in the 2D perovskite films has been considered to play an important role in influencing the stability of perovskite materials and their performance in optoelectronic applications. In this work, Lewis base urea was used as an effective additive for the formation of 2D Ruddlesden-Popper (RP) perovskite (BA)2(MA)n-1PbnI3n+1 thin film with mixed phases (n = 2~4). The detailed structural morphology of the 2D perovskite thin film was investigated by in situ X-ray diffraction (XRD), grazing-incidence small-angle X-ray scattering (GISAXS) and photoluminescence mapping. The results indicated that the urea additive could facilitate the formation of 2D RP perovskite thin film with larger grain size and high crystallinity. The 2D RP perovskite thin films for solar cells exhibited a power conversion efficiency (PCE) of 7.9% under AM 1.5G illumination at 100 mW/cm2.