Buried Interface Regulation with a Supramolecular Assembled Template Enables High-Performance Perovskite Solar Cells for Minimizing the V(OC) Deficit.

Despite the rapid development of perovskite solar cells (PSCs) in the past decade, the open-circuit voltage (V(OC)) of PSCs still lags behind the theoretical Shockley-Queisser limit. Energy-level mismatch and unwanted nonradiative recombination at key interfaces are the main factors detrimental to V(OC). Herein, a perovskite crystallization-driven template is constructed at the SnO(2)/perovskite buried interface through a self-assembled amphiphilic phosphonate derivative. The highly oriented supramolecular template grows from an evolutionary selection growth via solid-solid phase transition. This strategy induces perovskite crystallization into a highly preferred (100) orientation toward out-of-plane direction and facilitated carrier extraction and transfer due to the elimination of energy barrier. This self-assembly process positively passivates the intrinsic surface defects at the SnO(2)/perovskite interface through the functionalized moieties, a marked contrast to the passive effect achieved via incidental contacts in conventional passivation methods. As a result, PSCs with buried interface modification exhibit a promising PCE of 25.34%, with a maximum V(OC) of 1.23 V, corresponding to a mere 0.306 V deficit (for perovskite bandgap of 1.536 eV), reaching 97.2% of the theoretical V(OC) limit. This strategy spontaneously improves the long-term operational stability of PSCs under thermal and moisture stress (ISOS-L-3: MPP, 65 °C, 50% RH, T(92) lifetime exceeding 1200 h).