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Monocyclic \u03c0\u2010systems have long been considered intrinsically capped below \u0394\n                    <jats:italic>n<\/jats:italic>\n                    \u00a0=\u00a01.0. Here, we challenge this assumption by demonstrating that geometric precision, rather than \u03c0\u2010system enlargement, can unlock this performance ceiling. We introduce a\u00a0halogenation\u2010induced dimensional reduction\u00a0strategy in which halogen substituents redirect the hydrogen\u2010bonding topology of cytosine from non\u2010directional 2D networks into wave\u2010like 1D chains, whose complementary concave pockets form capsule\u2010shaped cavities. These cavities act as\n                    <jats:italic>lock<\/jats:italic>\n                    \u2010and\u2010\n                    <jats:italic>key<\/jats:italic>\n                    templates that confine linear polyhalides into strict collinear alignment while enforcing \u03c0\u2010plane coplanarity. This strategy affords five new birefringent hybrid crystals: (HXCy)\n                    <jats:sub>2<\/jats:sub>\n                    (I\n                    <jats:sub>2<\/jats:sub>\n                    Cl)\u00b7Cl (X\u00a0=\u00a0Cl,\u00a0\n                    <jats:bold>I<\/jats:bold>\n                    ; Br,\u00a0\n                    <jats:bold>II<\/jats:bold>\n                    , Cy\u00a0=\u00a0cytosine), (HClCy)\n                    <jats:sub>2<\/jats:sub>\n                    (ICl\n                    <jats:sub>2<\/jats:sub>\n                    )\u00b7Cl (\n                    <jats:bold>III<\/jats:bold>\n                    ), and (HBrCy)(BrCy)\u00b7IBr\n                    <jats:sub>2<\/jats:sub>\n                    (\n                    <jats:bold>IV<\/jats:bold>\n                    ) and\u00b7Br\n                    <jats:sub>3<\/jats:sub>\n                    (\n                    <jats:bold>V<\/jats:bold>\n                    ).\n                    <jats:bold>I<\/jats:bold>\n                    \u00a0and\u00a0\n                    <jats:bold>II<\/jats:bold>\n                    \u00a0reach calculated \u0394\n                    <jats:italic>n<\/jats:italic>\n                    \u00a0=\u00a01.336 and 1.324 at 546\u00a0nm, the highest among all \u03c0\u2010conjugated and inorganic crystals reported, while\u00a0\n                    <jats:bold>V<\/jats:bold>\n                    \u00a0retains \u0394\n                    <jats:italic>n<\/jats:italic>\n                    \u00a0=\u00a01.311 with a widened\u00a0\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>g<\/jats:sub>\n                    \u00a0=\u00a02.25\u00a0eV, demonstrating that birefringence and transparency can be independently tuned. These results establish geometric precision, rather than \u03c0\u2010system enlargement, as a powerful design route to high\u2010performance birefringent crystals.\n                  <\/jats:p>","DOI":"10.1002\/anie.4675227","type":"journal-article","created":{"date-parts":[[2026,5,26]],"date-time":"2026-05-26T16:20:53Z","timestamp":1779812453000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Lock\u2010and\u2010Key Assembly Enables Record Birefringence in Monocyclic \u03c0\u2010Conjugated Crystals via Spatial Confinement of Linear Polyhalide"],"prefix":"10.1002","volume":"65","author":[{"given":"Yun\u2010Xia","family":"Hu","sequence":"first","affiliation":[{"name":"Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering College of Chemistry and Material Science Fujian Normal University  Fuzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huai","family":"Yu Wu","sequence":"additional","affiliation":[{"name":"School of Chemistry Sun Yat\u2010Sen University  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia\u2010Jia","family":"Li","sequence":"additional","affiliation":[{"name":"Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering College of Chemistry and Material Science Fujian Normal University  Fuzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming\u2010Chang","family":"Wang","sequence":"additional","affiliation":[{"name":"Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering College of Chemistry and Material Science Fujian Normal University  Fuzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia\u2010Min","family":"Lian","sequence":"additional","affiliation":[{"name":"Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering College of Chemistry and Material Science Fujian Normal University  Fuzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jin","family":"Yu Luo","sequence":"additional","affiliation":[{"name":"Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering College of Chemistry and Material Science Fujian Normal University  Fuzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi\u2010Ru","family":"Fu","sequence":"additional","affiliation":[{"name":"Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering College of Chemistry and Material Science Fujian Normal University  Fuzhou P. R. 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