Photon-induced carrier recombination in the nonlayered-structured hybrid organic-inorganic perovskite nano-sheets

The hybrid organic-inorganic perovskites (HOIPs) have attracted much attention recently due to their preeminent efficiency in solar cells. According to the difference on the crystalline structure, the HOIPs could be classified into layered and non-layered perovskites. Very recently, it has been realized that the non-layered HOIPs with common-vertex structure possess even better opto-electrical performance. Yet the carrier recombination mechanism in perovskite remains not very clear, and a clear understanding of this mechanism is essential to pinpoint the working mechanism of photovoltaic and electroluminescent materials. Here we report the optical studies on the hybrid perovskite crystalline nano-sheet of CH₃NH₃PbBr₃ with common-vertex structure. It is shown that the non-layered perovskite crystalline nanosheets possess the exciton binding energy about two orders of magnitude smaller than that of the layered perovskite and the colloidal nanoplates, which is beneficial for the designing of the high-efficiency photovoltaic devices. By measuring the temperature-dependent photoluminescence (PL) spectra, the excitation-power-variant PL spectra, and the time-resolved PL spectra, we identify that both the free-carrier and the localized exciton recombination channels may coexist in the crystallites. Further, for the thin crystallite (∼60 nm), the free-carrier recombination channel dominates; whereas when the thickness increases beyond 200 nm, the localized exciton recombination channel plays the major role. We suggest these results are helpful to improve further the photovoltaic and electroluminescent performances of perovskite devices.