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Here, we present the successful synthesis of novel \u03c0\u2010extended double [7]helicenes (<jats:bold>ED7Hs<\/jats:bold>) where two helicene units are fused at the <jats:italic>meta\u2010<\/jats:italic> or <jats:italic>para\u2010<\/jats:italic>position of the middle benzene ring, respectively, as the structural isomers of the reported <jats:italic>ortho\u2010<\/jats:italic>fused <jats:bold>ED7H<\/jats:bold>. The structural geometry of these <jats:bold>ED7Hs<\/jats:bold> is clearly characterized by single\u2010crystal X\u2010ray analysis. Notably, this class of <jats:bold>ED7Hs<\/jats:bold> exhibits bright luminescence with high quantum yields exceeding 40\u2009%. Through geometric regulation of two embedded [7]helicene units from <jats:italic>ortho\u2010<\/jats:italic>, <jats:italic>meta\u2010<\/jats:italic> to <jats:italic>para\u2010<\/jats:italic>position, these <jats:bold>ED7Hs<\/jats:bold> display exceptional amplification in chiroptical responses. This enhancement is evident in a remarkable approximate fivefold increase in the absorbance and luminescence dissymmetry factors (<jats:italic>g<\/jats:italic><jats:sub>abs<\/jats:sub> and <jats:italic>g<\/jats:italic><jats:sub>lum<\/jats:sub>), respectively, along with a boosted CPL brightness up to 176\u2005M<jats:sup>\u22121<\/jats:sup>\u2009cm<jats:sup>\u22121<\/jats:sup>, surpassing the performance of most helicene\u2010based chiral NGs. Furthermore, DFT calculations elucidate that the geometric adjustment of two [7]helicene units allows the precise alignment of electric and magnetic transition dipole moments, leading to the observed enhancement of their chiroptical responses. This study offers an effective strategy for magnifying the CPL performance in chiral NGs, promoting their expanded application as CPL emitters.<\/jats:p>","DOI":"10.1002\/anie.202319874","type":"journal-article","created":{"date-parts":[[2024,2,19]],"date-time":"2024-02-19T09:53:56Z","timestamp":1708336436000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":55,"title":["Enhancing Chiroptical Responses in Helical Nanographenes via Geometric Engineering of Double [7]Helicenes"],"prefix":"10.1002","volume":"63","author":[{"given":"Wenhui","family":"Niu","sequence":"first","affiliation":[{"name":"Max Planck Institute of Microstructure Physics  Weinberg 2 Halle 06120 Germany"},{"name":"Center for Advancing Electronics Dresden (cfaed) &amp; Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  Mommsenstrasse 4 01062 Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yubin","family":"Fu","sequence":"additional","affiliation":[{"name":"Max Planck Institute of Microstructure Physics  Weinberg 2 Halle 06120 Germany"},{"name":"Center for Advancing Electronics Dresden (cfaed) &amp; Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  Mommsenstrasse 4 01062 Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qingsong","family":"Deng","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Physical Chemistry of Solid Surfaces and Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University  Xiamen 361005 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhen\u2010Lin","family":"Qiu","sequence":"additional","affiliation":[{"name":"Center for Advancing Electronics Dresden (cfaed) &amp; Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  Mommsenstrasse 4 01062 Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fupin","family":"Liu","sequence":"additional","affiliation":[{"name":"Leibniz Institute for Solid State and Materials Research  01069 Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Alexey A.","family":"Popov","sequence":"additional","affiliation":[{"name":"Leibniz Institute for Solid State and Materials Research  01069 Dresden Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hartmut","family":"Komber","sequence":"additional","affiliation":[{"name":"Leibniz-Institut f\u00fcr Polymerforschung Dresden e. V.  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