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In this study, guided by theoretical calculations, we report a series of new SAI materials (\n                    <jats:bold>BT\u2010nBZCz<\/jats:bold>\n                    ;\n                    <jats:italic>n<\/jats:italic>\n                    = 2, 3, and 4) based on a benzocarbazole core functionalized with a benzo[b]thiophene (BT) unit, and systematically investigate their impact on nonradiative losses and OSC performance. Notably, binary OSCs incorporating\n                    <jats:bold>BT\u20104BZCz<\/jats:bold>\n                    achieve a significantly higher power conversion efficiency (PCE) of 20.46% compared to 18.08% for BT\u2010free SAIs. Combined theoretical and experimental analyses reveal that BT functionalization improves energy level alignment, enhances dipole moment, and optimizes molecular packing, crystallization kinetics, and fibrillar network formation relative to BT\u2010free SAIs. These improvements promote more efficient exciton dissociation, reduce charge recombination, and in particular, suppress nonradiative energy losses (0.284\u00a0vs. 0.217\u00a0eV) in the corresponding OSCs. Furthermore,\n                    <jats:bold>BT\u20104BZCz<\/jats:bold>\n                    exhibits excellent universality, maintaining high performance across various binary photoactive blends. This work presents a viable molecular engineering strategy for SAIs to suppress nonradiative losses and advance the development of high\u2010performance OSCs.\n                  <\/jats:p>","DOI":"10.1002\/adma.74526","type":"journal-article","created":{"date-parts":[[2026,8,6]],"date-time":"2026-08-06T06:24:28Z","timestamp":1785997468000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Suppressing Nonradiative Losses via Computation\u2010Guided Molecular Design of Self\u2010Assembled Interfacial Layers for High\u2010Performance Organic Solar Cells"],"prefix":"10.1002","volume":"38","author":[{"given":"Tianyu","family":"Zeng","sequence":"first","affiliation":[{"name":"Chongqing Institute of Green and Intelligent Technology Key Laboratory of Mountain Hazards and Engineering Resilience Chinese Academy of Sciences  Chongqing P. R. 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