Optimizing Molecular Packing and Interfacial Contact via Halogenated N-Glycidyl Carbazole Small Molecules for Low Energy Loss and Highly Efficient Inverted Perovskite Solar Cells

Nonideal interfacial contact and non-radiative voltage loss in self-assembled monolayers (SAMs)-based inverted perovskite solar cells (PSCs) limit their further development. Herein, two carbazole-based molecules with different halogen atoms (X-OCZ, X = Cl or Br) are developed as efficient interfacial regulators. The halogen effect not only finely modulates the molecular packing, crystallinity, and surface contact potential of the MeO-2PACz analogue via self-induced intermolecular interactions but also significantly influences the subsequent crystal growth of perovskite, thus resulting in the formation of high-quality films with enhanced crystallinity, improved energy level alignment, and depressed non-radiative recombination. Importantly, the Cl-OCZ-mediated device exhibits a minimal interfacial carrier transport energy barrier of 0.10 eV and an impressive charge collection efficiency of 93.6%. Moreover, the target device (aperture area: 0.09 cm²) shows an exceptional efficiency of 26.57% (certified 26.4%) along with enhanced thermal and operational stability. The strategy is also extended to large area devices, delivering efficiencies of 25.0% for a 1 cm² device and 22.9% for a 12.96 cm² minimodule. This study highlights the halogen role of interfacial small molecules in optimizing molecular packing and interfacial contact toward highly efficient PSCs with minimized energy loss and non-radiative recombination.