Wetting-induced formation of void-free metal halide perovskite films by green ultrasonic spray coating for large-area mesoscopic perovskite solar cells

A void-free metal halide perovskite (MHP) layer on a mesoscopic TiO2 (m-TiO2) film was formed via the wetting-induced infiltration of MHP solution in the m-TiO2 film via a green ultrasonic spray coating process using a non-hazardous solvent. The systematic investigation of the behavior of ultrasonic-sprayed MHP micro-drops on the m-TiO2 film disclosed that the void-free MHP layer on the m-TiO2 film can be formed if the following conditions are satisfied: (1) the sprayed micro-drops are merged and wetted in the mesoscopic scaffold of the m-TiO2 film, (2) the MHP solution infiltrated into the m-TiO2 film by wetting is leveled to make a smooth wet MHP film, and (3) the smooth wet MHP film is promptly heat treated to eliminate dewetting and the coffee ring effect by convective flow in order to form a uniform void-free MHP layer. A void-free MHP layer on the m-TiO2 film was formed under optimal ultrasonic spray coating conditions of substrate temperature of ∼30 °C, spray flow rate of ∼11 mL h-1, nozzle to substrate distance of ∼8 cm, and MHP solution-concentration of ∼0.6 M under a fixed scan speed of 30 mm s-1 and purged N2 carrier gas pressure of 0.02 MPa. The mesoscopic MHP solar cells with an aperture area of 0.096, 1, 25, and 100 cm2 exhibited 17.14%, 16.03%, 12.93%, and 10.67% power conversion efficiency at 1 sun condition, respectively.