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Methylammonium chloride (MACl) additive is almost irreplaceable in high‐performance formamidine perovskite photovoltaics. Nevertheless, Some of the problems that can arise from adding MACl are rarely mentioned. Herein, it is proposed for the first time that the addition of MACl would cause the non‐stoichiometric ratio in the perovskite film, resulting in the halogen vacancy. It is demonstrated that the non‐synchronous volatilization of methylamine cations and chloride ions leads to the formation of halogen vacancy defects. To solve this problem, the NH4HCOO is introduced into the perovskite precursor solution to passivate the halogen vacancy. The HCOO− ions have a strong force with lead ions and can fill the halogen vacancy defects. Consequently, the champion devices' power conversion efficiency (PCE) can be improved from 21.23% to 23.72% with negligible hysteresis. And the unencapsulated device can still retain >90% of the initial PCE even operating in N2 atmosphere for over 1200 h. This work illustrates another halogen defect source in the MACl‐assisted formamidine perovskite photovoltaics and provides a new route to obtain high‐performance perovskite solar cells. [ABSTRACT FROM AUTHOR]

The perovskite photovoltaic field has developed rapidly within a decade. In particular, formamidinium (FA)‐rich perovskite allows a broad absorption spectrum, and is considered to be one of the most promising perovskite materials. Great progress has been achieved, and most recorded high‐efficient perovskite solar cells (PSCs) used the FA‐rich perovskite light absorption layer. However, the black α‐phase formamidinium lead iodide (FAPbI3) perovskite easily transforms into an undesirable δ‐phase at a low temperature. Thus, researchers have put a lot of effort into deeply understanding the phase transformation and stabilization mechanism of FA‐rich perovskite. Herein, the fundamental physical properties of FAPbI3 materials, including crystal structure, phase‐transition temperature, charge‐carrier dynamics, etc. are summarized, and establish a complete phase evolution with temperature by reviewing previous reports. The intrinsic and external factors are subsequently discussed for influencing the stability of FAPbI3 perovskite and the remarkable breakthroughs of FA‐rich PSCs in recent years are reviewed. Moreover, a series of strategies to stabilize FA‐rich perovskite is summarized, including but not limited to compositional engineering, passivating engineering, processing engineering, and strain engineering. Finally, several new viewpoints are provided for improving the efficiency and stability of PSCs. This review may be regarded as a reference project for preparing high‐efficient and stable perovskite photovoltaic devices. [ABSTRACT FROM AUTHOR]

Wide‐bandgap CsPbCl3 perovskite has fueled studies on applications in a variety of newly developing optoelectronic devices, including solar cells, lasers, light‐emitting diodes, and photodetectors. Most of them are now focused on film fabrication and device performance optimization, technology transfer of these proof‐of‐concept devices to the market will necessitate optimization of the device structure to minimize the optical loss and fabrication cost. While device model‐based electro‐optics simulations are considered a powerful method to attain the purpose, during which accurate optical constants are preconditions. Herein, for the first time, the optical constants of CsPbCl3 film through Mueller matrix spectroscopic ellipsometry (SE) are reported. Taking optoelectronic devices in vertical structure as a demonstration, simulations on the distributions of 2D electromagnetic field and photo‐generated electron field are arranged, successfully demonstrating the profile of the photons and electrons inside the devices. The evolution trend of device performance in the experiments matched with the simulations, for device performance is closely related to the photons and photo‐generated electrons. Benefitting from the simulations and experiments, general design criteria of the CsPbCl3‐based optoelectronic and photonic devices are posed, inevitably accelerating their development and commercialization. [ABSTRACT FROM AUTHOR]