Abstract
Wide-bandgap (WBG) perovskite solar cells (PSCs) are employed as top cells of tandem cells to break through the theoretical limits of single-junction photovoltaic devices. However, WBG PSCs exhibit severe open-circuit voltage (V(oc)) loss with increasing bromine content. Herein, inhomogeneous halogen-phase distribution is pointed out to be the reason, which hinders efficient extraction of carriers. We thus propose to form homogeneous halogen-phase distribution to address the issue. With the help of density functional theory, we construct a double-layer structure (D-2P) based on 2-(9H-Carbazol-9-yl)ethyl]phosphonic acid molecules to provide nucleation sites for perovskite crystallization. Homogeneous perovskite phase is achieved through bottom-up templated crystallization of halogen component. The efficient carrier extraction reduces the Shockley-Read-Hall recombination, resulting in a high V(oc) of 1.32 V. As a result, D-2P-treated device (1.75 eV) achieves a record power conversion efficiency of 20.80% (certified 20.70%), which is the highest value reported for WBG (more than 1.74 eV) PSCs.