Correlating Carrier Dynamics with Performance in Perovskite Solar Cells

Advancing the efficiency of perovskite solar cells (PSCs) critically depends on suppressing non‐radiative recombination at perovskite‐related interfaces and within the perovskite layer. A comprehensive understanding of carrier dynamic within PSCs is pivotal for promoting their efficiencies and facilitating more flexible design options for both perovskite and transport layers. Herein, the intrinsic mechanisms and device physics of PSCs are delved into, with a specific focus on investigating the variation of electron and hole mobilities and their effects on device performance. Through a rigorous photoelectric simulation, it is confirmed that the impact of performance of PSCs on electron or hole mobility primarily depends on the direction of illumination. For n–i–p PSCs, high hole mobility is favorable for the device performance, whereas for p–i–n PSCs, elevated electron mobility proves advantageous. Notably, these findings remain applicable across a large range of transport layers and perovskite bandgaps, although exceptions may arise when the perovskite layer undergoes specific doping. Additionally, it is discovered that high carrier mobility contributes to the reduction of both carrier and ion accumulation, thereby effectively suppressing hysteresis behavior. In this work, valuable insights into the significance and mechanisms of carrier mobility in PSCs are provided, offering essential guidance for fabricating high‐efficiency PSCs.