Cd-Free CZTS solar cell with above 10% efficiency was achieved by an Al2O3 passivation layer prepared by ALD.

Majority carrier mobility is one of the most fundamental and yet important carrier transport parameters determining the optimal device architecture and performance of the emerging antimony chalcogenide solar cells. However, carrier mobility measurements based on the Hall effect have limitations for these highly anisotropy materials due to the discrepancy of transport directions under Hall measurement and device operation. Herein, a defect‐resolved mobility measurement (DRMM) method enabling the evaluation of effective majority carrier mobility from a working device without such limitations is presented. Using this method, comprehensive information about the carrier transport in representative Sb2S3 and Sb2Se3 solar cells is extracted. Though with preferred [hk1]‐crystalline orientation, Sb2S3 and Sb2Se3 still suffer from extremely low carrier mobility and low carrier density, respectively, resulting in large bulk resistance and poor carrier collection efficiency. Further crystalline structure analysis discloses that crystalline defects such as dislocations may significantly constrain carrier transport in these low‐dimensional materials. These results suggest that a p‐i‐n device architecture with fully depleted absorber is a promising optimization approach for further efficiency advances of antimony chalcogenide solar cells.

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