Publication date: 16th July 2025
State-of-the-art perovskite/silicon tandem solar cells rely on alkyl-chain-based self-assembled molecules (SAMs) as hole-selective contacts in p-i-n structured perovskite top cells. However, these SAMs tend to aggregate into multilayered stacks on micrometer-scale pyramidal textured silicon interfaces, introducing charge transport losses and degrading device performance. To address this, we synthesized a conjugated linker-based SAM, (4-(7H-dibenzo[c,g]carbazol-7-yl)phenyl)phosphonic acid (Bz-PhpPACz), and compared it with its alkyl-chain counterpart, (4-(7H-dibenzo[c,g]carbazol-7-yl)butyl)phosphonic acid (4PADCB). Surprisingly, the incorporation of Bz-PhpPACz led to reduced tandem cell performance. Chemical analysis revealed that commercially sourced 4PADCB contains a bromine-substituted impurity, which introduces interfacial passivation and enhances hole transport. By separately synthesizing bromine-substituted Bz-PhpPACz (namely, Bz-PhpPABrCz) and blending it with Bz-PhpPACz in controlled ratios, we demonstrate that combining conjugated linkers with bromine substitution synergistically improves tandem cells efficiency. The optimized SAMs enable perovskite/silicon tandem cells fabricated on Czochralski (CZ)-grown silicon bottom cells with a power conversion efficiency of 31.4%, marking a significant advancement in molecular interface engineering for commercially viable c-Si-based tandem photovoltaics. This work highlights the critical role of molecular design and impurity engineering in overcoming interfacial challenges in perovskite solar cells.
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