Isoelectronic cation substitution is a potential method to decrease the density of Cu‐Zn anti‐site defects in CZTSSe, thus improving the VOC and performance of CZTSSe solar cells. The proper doping concentration is determined traditionally by the trial and error approach, costing much time, and materials. How to shorten the time to find the proper doping concentration is a big challenge for the development of solar cells. Here, by utilizing the machine learning model, the authors carry out an adaptive design for predicting the optimal doping ratio of Mn2+ ions in CZTSSe solar cells for improved solar cell efficiency. With the help of machine learning prediction, the authors rapidly and efficiently find the optimal doping ratio of Mn2+ in CZTSSe solar cells to be 0.05, achieving a highest solar cell efficiency of 8.9% in experiment. Further experimental characterizations of Mn‐doped CZTSSe show that the defect in CZTSSe after Mn doping is changed from an anti‐site CuZn defect to VCu defect. Our findings suggest that machine learning is a very powerful and efficient approach to aid the development of solar cell materials for its application in the photovoltaic field.

Double layer distribution exists in Cu2SnZnSe4 (CZTSe) thin films prepared by selenizing the metallic precursors, which will degrade the back contact of Mo substrate to absorber layer and thus suppressing the performance of solar cell. In this work, the double‐layer distribution of CZTSe film is eliminated entirely and the formation of MoSe2 interfacial layer is inhibited successfully. CZTSe film is prepared by selenizing the precursor deposited by electrodeposition method under Se and SnSex mixed atmosphere. It is found that the insufficient reaction between ZnSe and Cu‐Sn‐Se phases in the bottom of the film is the reason why the double layer distribution of CZTSe film is formed. By increasing Sn content in the metallic precursor, thus making up the loss of Sn because of the decomposition of CZTSe and facilitate the diffusion of liquid Cu2Se, the double layer distribution is eliminated entirely. The crystallization of the formed thin film is dense and the grains go through the entire film without voids. And there is no obvious MoSe2 layer formed between CZTSe and Mo. As a consequence, the series resistance of the solar cell reduces significantly to 0.14 Ω cm2 and a CZTSe solar cell with efficiency of 7.2% is fabricated.

Zn(O,S) film is a promising low‐cost and environment‐friendly Cd‐free buffer layer for chalcopyrite and kesterite thin film solar cells. However, the devices with Zn(O,S) buffer layer usually suffer from poor interface performance, resulting in a much lower efficiency, especially for kesterite solar cells. Here, the band fluctuation caused by ZnO secondary phase in Zn(O,S) layer is identified as the main reason deteriorating the device performance. By a concentrated ammonium etching and subsequent soft annealing treatment, the detrimental ZnO and Zn(OH)2 secondary phases are eliminated from the Zn(O,S) layer and the hetero‐junction performance is improved significantly. Consequently, the power conversion efficiency of the Zn(O,S)/CZTSe solar cells was improved from 1.17% to a favorable value of 7.2%. Temperature dependent J–V properties reveal a defect level assisted charge carrier transport mechanism across the Zn(O,S)/CZTSe interface. These encouraging results imply that Zn(O,S) buffer layer is a promising substitution for toxic CdS in future manufacturing of high performance thin film solar cells.

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