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The introduction of 2D\/3D mixed perovskite phases in tin\u2010based PSCs (TPSCs) has proven to be the most effective approach to improving device efficiency and stability. However, a 2D perovskite phase normally shows relatively low carrier mobility, which will be unfavorable for carrier transfer in the devices. In this work, we used a thiophene\u2010based cation 2\u2010(thiophen\u20103\u2010yl)ethan\u20101\u2010aminium (3\u2010TEA) as a spacer to form a novel 2D perovskite phase in TPSCs, which shows the most promising effect on the performance enhancement in comparison with other cations like 2\u2010(thiophen\u20102\u2010yl)ethan\u20101\u2010aminium (2\u2010TEA) and benzene\u2010based 2\u2010phenylethan\u20101\u2010aminium (PEA). Theoretical calculations reveal that 3\u2010TEA enables the most compact crystal packing of [SnI\n                    <jats:sub>6<\/jats:sub>\n                    ]\n                    <jats:sup>4\u2212<\/jats:sup>\n                    octahedral layers, resulting in the lowest hole effective mass and formation energy in the 2D phase. This effect significantly enhances device efficiency and stability by facilitating more efficient carrier transfer within the 2D phase. These findings indicate that thiophene\u2010based 2D perovskites are well\u2010suited for high\u2010performance TPSCs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202413584","type":"journal-article","created":{"date-parts":[[2024,10,15]],"date-time":"2024-10-15T10:03:40Z","timestamp":1728986620000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":28,"title":["A\u2010Site Engineering with Thiophene\u2010Based Ammonium for High\u2010Efficiency 2D\/3D Tin Halide Perovskite Solar Cells"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0288-7840","authenticated-orcid":false,"given":"Guitao","family":"Feng","sequence":"first","affiliation":[{"name":"Department of Applied Physics The Hong Kong Polytechnic University, Hung Hom  Kowloon, Hong Kong SAR 999077 P.R. 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