While operational stability has evolved to be the primary issue for the practical applications of perovskite solar cells (PSCs), the understanding of the origins of device degradation is still limited. Hysteresis is known as a unique and significant feature of PSCs. The hysteresis behavior of the current density-voltage (J–V) curves, governed by the interaction between the evolving ion-induced electric field and the carrier transport/recombination, offers rich and important information about the physical properties of the device. Herein, we propose to establish hysteresis as a diagnostic key to unveil and remedy degradation issues with device physics. With a custom-made ion-incorporated drift-diffusion simulator, we comprehensively investigate the relations between characteristic J–V hysteresis features and critical device issues such as bulk and surface defects, and low mobility of each layer in the PSCs. Ultimately, we derive a fundamental understanding and unveil the origins of the device degradation during the continuous operation of PSCs. This work therefore offers a new way to address and optimize PSC operational stability.
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