Cross‐layer all‐interface defect passivation with pre‐buried additive toward efficient all‐inorganic perovskite solar cells.

The buried interface in the perovskite solar cell (PSC) has been regarded as a breakthrough to boost the power conversion efficiency and stability. However, a comprehensive manipulation of the buried interface in terms of the transport layer, buried interlayer, and perovskite layer has been largely overlooked. Herein, we propose the use of a volatile heterocyclic compound called 2‐thiopheneacetic acid (TPA) as a pre‐buried additive in the buried interface to achieve cross‐layer all‐interface defect passivation through an in situ bottom‐up infiltration diffusion strategy. TPA not only suppresses the serious interfacial nonradiative recombination losses by precisely healing the interfacial and underlying defects but also effectively enhances the quality of perovskite film and releases the residual strain of perovskite film. Owing to this versatility, TPA‐tailored CsPbBr3 PSCs deliver a record efficiency of 11.23% with enhanced long‐term stability. This breakthrough in manipulating the buried interface using TPA opens new avenues for further improving the performance and reliability of PSC. [ABSTRACT FROM AUTHOR]