Sequential Preparation of Dual-Layer Fluorine-Doped Tin Oxide Films for Highly Efficient Perovskite Solar Cells

A dual-layer fluorine-doped tin oxide (FTO) film has been fabricated by means of sequential spray pyrolysis for high-efficiency perovskite solar cells (PSCs). The H-FTO/L-FTO dual layer film consists of a H-FTO layer prepared at high deposition temperature (≈450 °C) and a L-FTO layer, fabricated at low deposition temperature (≈150 °C), which is used to replace the traditional compact TiO₂/FTO layer. The effects of F/Sn molar ratio, precursor solution concentration, and deposition temperature on the electrical, optical, surface morphological, and grain structural characteristics of H-FTO layers have been studied systematically. With an increase in precursor solution concentration, the mobility and carrier concentration of H-FTO increases; however, the grain size and sheet resistance decreases as the precursor solution concentration increases. A high deposition temperature results in a large grain size and enhanced haze value. The L-FTO layer expresses compact layer growth, inconsistent with the H-FTO surface structure, and possesses excellent electron collection and transport efficiency. The effect of the hole-blocking characteristics of L-FTO on the PSC performance is studied. This study provides a novel dual-layer FTO film to replace the traditional compact TiO₂/FTO layer, which is usually prepared by coating TiO₂ precursor on FTO following calcination at 450 °C. The H-FTO/L-FTO dual-layer film can simplify the fabrication process and maintain a high power conversion efficiency (PCE); this results in more efficient electron transportation and blocking of holes. The champion device of PSCs with H-FTO/L-FTO shows the highest PCE of 17.37 % under the illumination of 100 mW cm⁻² (AM1.5G).