Dynamical evolution of the 2D/3D interface: a hidden driver behind perovskite solar cell instability

Engineering two-/three-dimensional (2D/3D) perovskite solar cells is nowadays a popular strategy for efficient and stable devices. However, the exact function of the 2D/3D interface in controlling the long-term device behavior is still obscure. Here, we reveal a dynamical structural mutation of the 2D/3D interface: the small cations in the 3D cage move towards the 2D layer, which acts as an ion scavenger. If structurally stable, the 2D layer physically blocks the ion movement at the interface boosting the device stability. Otherwise, the 2D layer embeds them, dynamically self-transforming into a quasi-2D structure. The judicious choice of the 2D constituent is decisive in controlling the 2D/3D kinetics and improving the device lifetime, opening a new avenue for perovskite interface design.