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Yet a long\u2010standing assumption in the field holds that minimizing excited\u2010state structural displacement (\u0394\n                    <jats:italic>Q<\/jats:italic>\n                    ) is essential for achieving narrow emission bandwidth. Here we challenge this notion by demonstrating that \u0394\n                    <jats:italic>Q<\/jats:italic>\n                    and molecular vibrational frequency (\n                    <jats:italic>\u03c9<\/jats:italic>\n                    ) act as independent, rather than coupled, determinants of the emission full width at half maximum (FWHM). Through systematic\n                    <jats:italic>ortho<\/jats:italic>\n                    (\n                    <jats:italic>o<\/jats:italic>\n                    DB\u2010BN),\n                    <jats:italic>meta<\/jats:italic>\n                    (\n                    <jats:italic>m<\/jats:italic>\n                    DB\u2010BN), and\n                    <jats:italic>para<\/jats:italic>\n                    (\n                    <jats:italic>p<\/jats:italic>\n                    DB\u2010BN) positional isomerism of a sterically bulky dimesitylboryl acceptor on an archetypal MR scaffold, we reveal that small \u0394\n                    <jats:italic>Q<\/jats:italic>\n                    reduces the Stokes shift but does not guarantee narrow FWHM; instead, low\n                    <jats:italic>\u03c9<\/jats:italic>\n                    emerges as the decisive factor. The meta\u2010substituted isomer, despite exhibiting the smallest \u0394\n                    <jats:italic>Q<\/jats:italic>\n                    , displays the broadest FWHM owing to a prominent low\u2010frequency torsional vibration. Conversely, the\n                    <jats:italic>ortho<\/jats:italic>\n                    \u2010 and\n                    <jats:italic>para<\/jats:italic>\n                    \u2010isomers retain ultranarrow emission despite pronounced molecular distortion. The resulting OLEDs achieve excellent external quantum efficiencies of up to 33.3% with suppressed roll\u2010off, and pDB\u2010BN delivers a remarkable luminance of 109\u00a0600 cd m\n                    <jats:sup>\u22122<\/jats:sup>\n                    . This work provides an alternative perspective on the design of narrowband emitters, suggesting that controlling vibrational coupling, in addition to minimizing structural displacement, is a valuable consideration in molecular engineering.\n                  <\/jats:p>","DOI":"10.1002\/anie.2538716","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T13:27:54Z","timestamp":1792070874000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Positional Isomerism Reveals Intrinsic Decoupling of Structural Relaxation and Vibrational Frequency in MR\u2010TADF Emitters"],"prefix":"10.1002","author":[{"given":"Xiaojuan","family":"Song","sequence":"first","affiliation":[{"name":"Institute of Molecular Aggregation Science Tianjin University  Tianjin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yangyang","family":"Xin","sequence":"additional","affiliation":[{"name":"Laboratory of Flexible Electronics Technology Tsinghua University  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoning","family":"Li","sequence":"additional","affiliation":[{"name":"Institute of Molecular Aggregation Science Tianjin University  Tianjin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiyun","family":"Ye","sequence":"additional","affiliation":[{"name":"Institute of Molecular Aggregation Science Tianjin University  Tianjin P. R. China"},{"name":"Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University Binhai New City  Fuzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4990-1550","authenticated-orcid":false,"given":"Yujun","family":"Xie","sequence":"additional","affiliation":[{"name":"Institute of Molecular Aggregation Science Tianjin University  Tianjin P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6664-527X","authenticated-orcid":false,"given":"Yuewei","family":"Zhang","sequence":"additional","affiliation":[{"name":"Laboratory of Flexible Electronics Technology Tsinghua University  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2750-0972","authenticated-orcid":false,"given":"Lian","family":"Duan","sequence":"additional","affiliation":[{"name":"Laboratory of Flexible Electronics Technology Tsinghua University  Beijing P. R. 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