Polyfluorinated-Regulator-Assisted Scaffold-Directed Tilted 1D/3D Heterointerfaces for High-Voltage and Stable Perovskite Solar Cells.

Protective low-dimensional interphases can improve perovskite solar-cell stability, but they often compromise charge extraction because of unfavorable interfacial packing and transport barriers. Herein, we report a scaffold-directed strategy to construct an interwoven tilted 1D/3D heterointerface on inverted perovskite absorbers. By depositing PbI2 onto a tilt-oriented 3D perovskite scaffold and inducing solvent-assisted reconstruction, a compact near-surface interphase composed of edge-sharing 1D PbI2 and face-sharing 1D δ-FAPbI3 is formed with an oblique orientation guided by the crystallographic texture of the underlying 3D framework. Unlike conventional laterally aligned low-dimensional overlayers, this tilted 1D interphase preserves out-of-plane interfacial connectivity while providing a robust barrier against defect propagation and ion migration. We further identify 7F-EA-HI, a flexible polyfluorinated ammonium iodide, as an effective crystallization regulator that suppresses reconstruction-induced defects and favorably modulates interfacial energetics through its large molecular dipole. As a result, the optimized inverted PSCs deliver a power conversion efficiency (PCE) of 24.94%, with an open-circuit voltage (VOC) of 1.188 V, a short-circuit current density (JSC) of 24.67 mA cm-2, and a fill factor (FF) of 85.11%, along with markedly improved ambient and thermal stability. This work demonstrates tilted 1D/3D interfacial engineering as a viable route toward high-voltage and durable perovskite optoelectronics.