Interface Engineering for Both Cathode and Anode Enables Low‐Cost Highly Efficient Solution‐Processed CdTe Nanocrystal Solar Cells

Low‐cost solution‐processed CdTe nanocrystal (NC) solar cells always suffer from a high interface energy barrier and unbalanced hole/electron transport as well as anisotropic atom diffusion on the CdTe surface due to the limited amount of hole/electron interface materials or the difficulty in interface processing. In this work, a novel strategy is first adopted with gradient electron transport layer (CdS/CdSe) modification in the cathode and a new crosslinkable hole transport polymer (P‐TPA) implantation in the anode. The carrier recombination at interfaces is greatly decreased and thus the carrier collection is increased. Moreover, the light harvesting is improved both in short and long wavelength regions, making J_sc and V_oc increase simultaneously. A champion solar cell shows a very high power conversion efficiency of 9.2% and an outstanding J_sc of 25.31 mA cm^?2, which are among the highest values for all solution‐processed CdTe NC solar cells with a superstrate structure, and the latter value is even higher than that of traditional thick CdTe thin‐film solar cells (2 µm) via the high temperature close space sublimation method. This work demonstrates that facile surface modifications in both the cathode and anode with stepped extraction and organic–inorganic hybridization are very promising in constructing next‐generation highly efficient NC photovoltaic devices.