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According to current knowledge, the SOC effect, normally dominated by the elemental composition, is the main spin\u2010relaxation causation in MSCs, and thus the molecular structure\u2010induced SOC change is one of the most concerned issues. In theoretical study, molecular isomerism, a most prototype phenomenon, has long been considered to possess little difference on spin transport previously, since elemental compositions of isomers are totally the same. However, here in this study, quite different spin\u2010transport performances are demonstrated in ITIC and its structural isomers BDTIC experimentally, for the first time, though the charge transport and molecular stacking of the two films are very similar. By further experiments of electron\u2010paramagnetic resonance and density\u2010functional\u2010theory calculations, it is revealed that noncovalent\u2010conformational locks (NCLs) formed in BDTIC can lead to enhancement of SOC and thus decrease the spin lifetime. Hence, this study suggests the influences from the structural\u2010isomeric effect must be considered for developing highly efficient spin\u2010transport MSCs, which also provides a reliable theoretical basis for solving the great challenge of quantificational measurement of NCLs in films in the future.<\/jats:p>","DOI":"10.1002\/adma.202402001","type":"journal-article","created":{"date-parts":[[2024,4,10]],"date-time":"2024-04-10T09:34:18Z","timestamp":1712741658000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Structural Isomeric Effect on Spin Transport in Molecular Semiconductors"],"prefix":"10.1002","volume":"36","author":[{"given":"Tingting","family":"Yang","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology  Beijing 100190 P. R. 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