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In this study, we investigate the impact of peripheral <jats:italic>tert<\/jats:italic>\u2010butyl (t\u2010Bu)\u2010 and phenyl (Ph)\u2010substituents on the typical 9\u2010(phenylcarbazol\u20103\u2010yl)\u20109H\u2010carbazole\u20103\u2010carbonitrile (CzBN) MR framework. Although these modifications preserve the frontier molecular orbital distribution with large oscillator strengths, they significantly influence excited\u2010state dynamics and molecular aggregation even at low doping concentrations. Introducing Ph substituents extends the \u03c0\u2013conjugation extension of CzBN, promoting closer molecular packing, detrimental molecular aggregation, and significantly broadening the excited\u2010state absorption (ESA) band, which negatively impacts lasing performance. In contrast, CzBN\u2010tBu, incorporating <jats:italic>t<\/jats:italic>\u2010Bu groups as nonconjugated substituents, demonstrated reduced molecular aggregation and a distinct separation between the ESA band and stimulated emission region. Consequently, the optimal distributed feedback lasing performance is achieved by CzBN\u2010tBu across various doping concentrations, resulting in the lowest lasing threshold of 3.4\u00a0\u00b5J\u00a0cm<jats:sup>\u22122<\/jats:sup>. These findings underscore the impact of inherent aggregation at low doping ratios on lasing activities, highlighting the crucial role of rational peripheral engineering in modulating molecular interactions and excited\u2010state dynamics, offering design strategies for developing MR lasing molecules.<\/jats:p>","DOI":"10.1002\/anie.202504652","type":"journal-article","created":{"date-parts":[[2025,3,31]],"date-time":"2025-03-31T07:22:42Z","timestamp":1743405762000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Peripheral Engineering of Multiple\u2010Resonance Framework Targeting Efficient Organic Lasers"],"prefix":"10.1002","volume":"64","author":[{"given":"Tuul","family":"Tsagaantsooj","sequence":"first","affiliation":[{"name":"Center for Organic Photonics and Electronics Research (OPERA) Kyushu University  744 Motooka Nishi Fukuoka 819\u20100395 Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xun","family":"Tang","sequence":"additional","affiliation":[{"name":"Center for Organic Photonics and Electronics Research (OPERA) Kyushu University  744 Motooka Nishi Fukuoka 819\u20100395 Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tao","family":"Zhang","sequence":"additional","affiliation":[{"name":"Institute of Functional Nano &amp; Soft Materials (FUNSOM) Soochow University  Suzhou Jiangsu 215123 P.R. 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