Sequential Cesium Incorporation for Highly Efficient Formamidinium-Cesium Perovskite Solar Cells

Although pure formamidinium iodide perovskite (FAPbI3) possesses an optimal gap for photovoltaics, their poor phase stability limits the long-term operational stability of the devices. A promising approach to enhance their phase stability is to incorporate cesium into FAPbI3. However, state-of-the-art formamidinium-cesium (FA-Cs) iodide perovskites demonstrate much worse efficiency compared with FAPbI3, limited by different crystallization dynamics of formamidinium and cesium, which result in poor composition homogeneity and high trap densities. We develop a novel strategy of crystallization decoupling processes of formamidinium and cesium via a sequential cesium incorporation approach. As such, we obtain highly reproducible and highly efficient solar cells based on FA1-xCsxPbI3 films, with uniform composition distribution and low defect densities. In addition, our cesium-incorporated perovskites demonstrate much enhanced stability compared with FAPbI3, as a result of suppressed ionic migration due to reduced electron-phonon coupling.

Regulating crystallization dynamics and crystal orientation of methylammonium tin iodide enables high-efficiency lead-free perovskite solar cells

Tin (Sn)-based perovskite solar cells (PSCs) have attracted much attention because they are more environmentally friendly than lead-based PSCs. However, the fast crystallization of Sn-based perovskite film and the easy...

Manipulating crystallization dynamics through chelating molecules for bright perovskite emitters

Molecular additives are widely utilized to minimize non-radiative recombination in metal halide perovskite emitters due to their passivation effects from chemical bonds with ionic defects. However, a general and puzzling observation that can hardly be rationalized by passivation alone is that most of the molecular additives enabling high-efficiency perovskite light-emitting diodes (PeLEDs) are chelating (multidentate) molecules, while their respective monodentate counterparts receive limited attention. Here, we reveal the largely ignored yet critical role of the chelate effect on governing crystallization dynamics of perovskite emitters and mitigating trap-mediated non-radiative losses. Specifically, we discover that the chelate effect enhances lead-additive coordination affinity, enabling the formation of thermodynamically stable intermediate phases and inhibiting halide coordination-driven perovskite nucleation. The retarded perovskite nucleation and crystal growth are key to high crystal quality and thus efficient electroluminescence. Our work elucidates the full effects of molecular additives on PeLEDs by uncovering the chelate effect as an important feature within perovskite crystallization. As such, we open new prospects for the rationalized screening of highly effective molecular additives.

Real-time monitoring of crystallization from solution by using an interdigitated array electrode sensor

An Interdigitated array Electrode sensor (IES) is used for real-time monitoring of the crystallization dynamics of organic molecules, achieving a temporal resolution of 15 ms.

Visualization of halide perovskite crystal growth processes by in situ heating WAXS measurements

We observed the crystallization dynamics of halide perovskite crystals (CH3NH3PbI3) by in situ heating WAXS measurements.