Preparation of high-performance large-area perovskite solar cells by atomic layer deposition of metal oxide buffer layer

Perovskite solar cells have been widely recognized as the most promising new-type photovoltaic device due to its power conversion efficiency rapidly increasing from 3.8% to over 26% in merely fifteen years. However, the high performances are achieved mainly on small area cells with an active area lower than 0.1 cm(2). When enlarging the active area of perovskite solar cells, the efficiency falls dramatically. So, how to reduce the gap between performances of small area cells and large area cells gradually becomes a critical point in the path towards the commercialization of perovskite photovoltaic technology. Herein, a strategy of pre-growing thin layer of TiO2 on a rough FTO substrate by atomic layer deposition method before spin-coating SnO2 nanoparticles is proposed. Due to the inherent conformal film growth mode of atomic layer deposition, the FTO substrate can be completely covered by TiO2, thus preventing the direct contact between local protrusions of FTO and perovskite layer and impeding the current leakage phenomenon, which can be verified by the measurements from X-ray photoelectron spectroscopy, scanning electron microscopy, and atomic force microscopy, and further proved by the dark current measurement. By using this method, the repeatability and consistency of the small area cell fabrication technology on the same substrate are improved obviously. The improved electron transport process revealed by photoluminescence results and incident light management process revealed by external quantum efficiency results also brings about better solar cell performances. More importantly, highly efficient 0.5 cm(2) large area perovskite solar cells are fabricated through optimization of TiO2 thickness. When growing 200 cycles TiO2 (similar to 9 nm in thickness) by using atomic layer deposition technology, the champion large area perovskite solar cell possesses a power conversion efficiency as high as 24.8% (certified 24.65%). The device performances also show excellent repeatability between different fabrication batches. The perovskite solar cell with TiO2 buffer layer grown by the atomic layer deposition method can still retain over 95% of its initial efficiency after having been stored in a nitrogen atmosphere for 1500 h. The technique proposed in this paper can be helpful in manufacturing perovskite solar cell modules in the realistic photovoltaic market and can be extended to the large area fabrication of other perovskite optoelectronic devices such as light emitting diode, laser and detector.