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While considerable efforts have focused on reducing \u0394\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>S1T1<\/jats:sub>\n                    , investigations on SOCs remain limited. Here, blocking \u03c0\u2010conjugation in carbonyl\u2010embedded polycyclic heteroaromatic (PHA) molecules as potential approach to elevate \u03c0\u03c0* excitation energy, allowing its hybridization with n\u03c0* excitation, thereby increasing SOCs is proposed. Two proof\u2010of\u2010concept isomers, DNDK\u20101 and DNDK\u20102 are synthesized, with different orientations of carbonyl units. DNDK\u20101 adopts a heavily twisted structure that hinders \u03c0\u2010conjugation, while DNDK\u20102 remains quasi\u2010planar, maintaining stronger \u03c0\u2010conjugation. Experimental measurements reveals stark differences in their photophysical properties, with DNDK\u20101 exhibiting faster\n                    <jats:italic>k<\/jats:italic>\n                    <jats:sub>RISC<\/jats:sub>\n                    and much higher electroluminescence efficiency. The\n                    <jats:italic>ab\u2010initio<\/jats:italic>\n                    calculations elucidate that hindered conjugation in DNDK\u20101 elevates \u03c0\u03c0* excitation energy, enabling n\u03c0*\u2010\u03c0\u03c0* mixing, thus significantly boosting SOCs. In contrast, smooth \u03c0\u2010conjugation in DNDK\u20102 leads to marginal n\u03c0*\u2010\u03c0\u03c0* mixing. In addition, utilizing groups composed of meta\u2010arranged carbonyl\u2010Ar\u2010carbonyl and meta\u2010arranged N\u2010Ar\u2010N units emerges as another approach to block \u03c0\u2010conjugation and enhance SOCs. This joint experimental and theoretical work provides promising pathways to enhance SOCs by blocking \u03c0\u2010conjugation, offering crucial insights for designing carbonyl\u2010embedded PHA emitters with larger SOCs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202503371","type":"journal-article","created":{"date-parts":[[2025,3,11]],"date-time":"2025-03-11T19:54:20Z","timestamp":1741722860000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Blocking Orbital \u03c0\u2010Conjugation to Boost Spin\u2010Orbit Coupling in Carbonyl\u2010Embedded Polycyclic Heteroaromatic Emitters"],"prefix":"10.1002","volume":"64","author":[{"given":"Rajat","family":"Walia","sequence":"first","affiliation":[{"name":"Institute of Functional Nano and Soft Materials (FUNSOM) Joint International Research Laboratory of Carbon\u2010Based Functional Materials and Devices Soochow University  Suzhou Jiangsu P.R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kai","family":"Wang","sequence":"additional","affiliation":[{"name":"Institute of Functional Nano and Soft Materials (FUNSOM) Joint International Research Laboratory of Carbon\u2010Based Functional Materials and Devices Soochow University  Suzhou Jiangsu P.R. China"},{"name":"Jiangsu Key Laboratory for Carbon\u2010Based Functional Materials &amp; Devices Soochow University  Suzhou Jiangsu P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chihaya","family":"Adachi","sequence":"additional","affiliation":[{"name":"Center for Organic Photonics and Electronics Research (OPERA) Kyushu University  15 Fukuoka 819\u20100395 Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xian\u2010Kai","family":"Chen","sequence":"additional","affiliation":[{"name":"Institute of Functional Nano and Soft Materials (FUNSOM) Joint International Research Laboratory of Carbon\u2010Based Functional Materials and Devices Soochow University  Suzhou Jiangsu P.R. China"},{"name":"Center for Organic Photonics and Electronics Research (OPERA) Kyushu University  15 Fukuoka 819\u20100395 Japan"},{"name":"Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University  Suzhou Jiangsu P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiao\u2010Hong","family":"Zhang","sequence":"additional","affiliation":[{"name":"Institute of Functional Nano and Soft Materials (FUNSOM) Joint International Research Laboratory of Carbon\u2010Based Functional Materials and Devices Soochow University  Suzhou Jiangsu P.R. China"},{"name":"Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University  Suzhou Jiangsu P.R. 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