Top-Down Dual-Interface Carrier Management for Highly Efficient and Stable Perovskite/Silicon Tandem Solar Cells

Abstract

Despite significant advancements in the power conversion efficiency (PCE) of perovskite/silicon tandem solar cells, improving carrier management in top cells remains challenging due to the defective dual interfaces of wide-bandgap perovskite, particularly on textured silicon surfaces. Herein, a series of halide ions (Cl⁻, Br⁻, I⁻) substituted piperazinium salts are designed and synthesized as post-treatment modifiers for perovskite surfaces. Notably, piperazinium chloride induces an asymmetric bidirectional ions distribution from the top to the bottom surface, with large piperazinium cations concentrating at the perovskite surface and small chloride anions migrating downward to accumulate at the buried interface. This results in effective dual-interface defect passivation and energy band modulation, enabling wide-bandgap (1.68 eV) perovskite solar cells to achieve a PCE of 22.3% and a record product of open-circuit voltage × fill factor (84.4% relative to the Shockley–Queisser limit). Furthermore, the device retains 91.3% of its initial efficiency after 1200 h of maximum power point tracking without encapsulation. When integrated with double-textured silicon heterojunction solar cells, a remarkable PCE of 31.5% is achieved for a 1.04 cm² monolithic perovskite/silicon tandem solar cell, exhibiting excellent long-term operational stability (T₈₀ = 755 h) without encapsulation in ambient air. This work provides a convenient strategy on dual-interface engineering for making high-efficiency and stable perovskite platforms.