Control of Surface Defects in ZnO Nanorod Arrays with Thermally Deposited Au Nanoparticles for Perovskite Photovoltaics

In this work, we employ vacuum deposited Au nanoparticles (-4 nm) to control the defect density on the surface of hydrothermally synthesized ZnO nanorod arrays (ZnO-NR), which are of interest for electron-transport layers in perovskite solar cells. Using a combination of photoluminescence spectroscopy, X-ray photoelectron spectroscopy, and ultraviolet photoelectron spectroscopy, we show that the Au particles reduce the presence of defects in the ZnO-NR. We discuss this in terms of trap filling due to band bending at the ZnO-NR surface. As a proof-of-concept, we apply the Au-decorated ZnO-NR as electron-transport layers in mixed-cation and mixed-halide lead perovskite solar cells (Cs_0.15FA_0.85PbI_2.75Br_0.25). Devices prepared with the Au-decorated ZnO-NR electron-transport layers demonstrate higher open-circuit voltages and fill factors compared to solar cells prepared with pristine ZnO-NR, resulting in an increase in the power-conversion efficiency from 11.7 to 13.7%. However, the operational stability of the solar cells is not improved by the Au nanoparticles, indicating that bulk properties of the perovskite may limit device lifetime.