Chun‐Hsiao KuanShakil N. AfrajYu‐Ling HuangArulmozhi VelusamyCHENG-LIANG LIUTing‐Yu SuXianyuan JiangJhih‐Min LinMing‐Chou ChenEric Wei‐Guang Diau2024-09-302024-09-302024-09-2314337851https://www.scopus.com/record/display.uri?eid=2-s2.0-85201824027&origin=resultslisthttps://scholars.lib.ntu.edu.tw/handle/123456789/721600Three functionalized thienopyrazines (TPs), TP-MN (1), TP-CA (2), and TPT-MN (3) were designed and synthesized as self-assembled monolayers (SAMs) deposited on the NiOx film for tin-perovskite solar cells (TPSCs). Thermal, optical, electrochemical, morphological, crystallinity, hole mobility, and charge recombination properties, as well as DFT-derived energy levels with electrostatic surface potential mapping of these SAMs, have been thoroughly investigated and discussed. The structure of the TP-MN (1) single crystal was successfully grown and analyzed to support the uniform SAM produced on the ITO/NiOx substrate. When we used NiOx as HTM in TPSC, the device showed poor performance. To improve the efficiency of TPSC, we utilized a combination of new organic SAMs with NiOx as HTM, the TPSC device exhibited the highest PCE of 7.7 % for TP-MN (1). Hence, the designed NiOx/TP-MN (1) acts as a new model system for the development of efficient SAM-based TPSC. To the best of our knowledge, the combination of organic SAMs with anchoring CN/CN or CN/COOH groups and NiOx as HTM for TPSC has never been reported elsewhere. The TPSC device based on the NiOx/TP-MN bilayer exhibits great enduring stability for performance, retaining ~80 % of its original value for shelf storage over 4000 h.truecyano functionalitySelf-assembled monolayerssolar cellsthienopyrazinestin perovskite[SDGs]SDG7journal article10.1002/anie.2024072282-s2.0-85201824027