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Exploring lead‐free candidates and improving efficiency and stability remain the obstacle of hybrid organic‐inorganic perovskite‐based devices commercialization. Traditional trial‐and‐error methods seriously restrict the discovery especially for large search space, complex crystal structure and multi‐objective properties. Here, the authors propose a multi‐step and multi‐stage screening scheme to accelerate the discovery of hybrid organic‐inorganic perovskites A2BB′X6 from a large number of candidates through combining machine learning with high‐throughput calculations for pursuing excellent efficiency and thermal stability in solar cells. Followed by a series of screenings, the structure‐property relationships mapping A2BB′X6 properties are built and the predictions are close to reported experimental results. Successfully, four experimental‐feasibly candidates with good stability, high Debye temperature and suitable band gap are screened out and further verified by density‐functional theory calculations, in which the predicted efficiency for three lead‐free candidates ((CH3NH3)2AgGaBr6, (CH3NH3)2AgInBr6 and (C2NH6)2AgInBr6) achieves 20.6%, 19.9% and 27.6% due to ultrabroadband absorption region ranging from UVC to IRC with excitonic radiative combination rates as low as 10 ps, large or intermediate polarons form with properties similar to CH3NH3PbI3 and the calculated thermal conductivities are 5.04, 4.39 and 5.16 Wm−1K−1, respectively, with Debye temperatures larger than 500 K, beneficial for suppression of both nonradiative combination and heat‐induced degradation. A multi‐step screening scheme is proposed to accelerate the discovery of potential perovskite A2BB′X6 through combining machine learning with high‐throughput calculations for the target of excellent efficiency and thermal stability in solar cells. Among final candidates, the predicted efficiency for three lead‐free candidates achieves 20.6%, 19.9% and 27.6%, and the calculated thermal conductivities are 5.04, 4.39 and 5.16 Wm−1K−1, respectively.

Energy loss in perovskite grain boundaries (GBs) is a primary limitation toward high‐efficiency perovskite solar cells (PSCs). Two critical strategies to address this issue are high‐quality crystallization and passivation of GBs. However, the established methods are generally carried out discretely due to the complicated mechanisms of grain growth and defect formation. In this study, a combined method is proposed by introducing 3,4,5‐Trifluoroaniline iodide (TFAI) into the perovskite precursor. The TFAI triggers the union of nano‐sized colloids into microclusters and facilitates the complete phase transition of α‐FAPbI3 at room temperature. The controlled chemical reactivity and strong steric hindrance effect enable the fixed location of TFAI and suppress defects at GBs. This combination of well‐crystallized perovskite grains and effectively passivated GBs leads to an improvement in the open circuit voltage (Voc) of PSCs from 1.08 V to 1.17 V, which is one of the highest recorded Voc without interface modification. The TFAI‐incorporated device achieved a champion PCE of 24.81%. The device maintained a steady power output near its maximum power output point, showing almost no decay over 280 h testing without pre‐processing. A combined method is proposed by introducing 3,4,5‐Trifluoroaniline iodide (TFAI) into the perovskite precursor. The TFAI induces a complete phase transition of α‐FAPbI3 at room temperature and serves as a passivation agent at grain boundaries. The TFAI‐modified device achieves over 24% PCE and maintains steady power output for 380 h with almost no performance decay.

Energy loss in perovskite grain boundaries (GBs) is a primary limitation toward high‐efficiency perovskite solar cells (PSCs). Two critical strategies to address this issue are high‐quality crystallization and passivation of GBs. However, the established methods are generally carried out discretely due to the complicated mechanisms of grain growth and defect formation. In this study, a combined method is proposed by introducing 3,4,5‐Trifluoroaniline iodide (TFAI) into the perovskite precursor. The TFAI triggers the union of nano‐sized colloids into microclusters and facilitates the complete phase transition of α‐FAPbI 3 at room temperature. The controlled chemical reactivity and strong steric hindrance effect enable the fixed location of TFAI and suppress defects at GBs. This combination of well‐crystallized perovskite grains and effectively passivated GBs leads to an improvement in the open circuit voltage ( V oc ) of PSCs from 1.08 V to 1.17 V, which is one of the highest recorded V oc without interface modification. The TFAI‐incorporated device achieved a champion PCE of 24.81%. The device maintained a steady power output near its maximum power output point, showing almost no decay over 280 h testing without pre‐processing.