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In this study, we introduce a coordination\u2010driven approach that significantly enhances optical anisotropy by transforming a loosely packed molecular crystal (\n                    <jats:bold>crystal\u20101<\/jats:bold>\n                    ) into a chiral metal\u2013organic framework (MOF) (\n                    <jats:bold>crystal\u20102<\/jats:bold>\n                    ). This structural transformation leads to a more than 20\u2010fold increase in birefringence (\u0394\n                    <jats:italic>n<\/jats:italic>\n                    \u00a0=\u00a00.226 at 546\u00a0nm) and activates a measurable second\u2010harmonic generation (SHG) activity. First\u2010principles calculations suggest that the observed optical enhancement is driven by three main factors: coordination\u2010driven enhancement of asymmetry, alignment of the \u03c0\u2010conjugated framework, and anisotropic electron distribution. These findings highlight the potential of coordination polymerization as a versatile approach for designing hybrid optical materials with tailored anisotropy, providing a foundation for the development of MOF\u2010based photonic devices.\n                  <\/jats:p>","DOI":"10.1002\/anie.202516178","type":"journal-article","created":{"date-parts":[[2025,11,3]],"date-time":"2025-11-03T08:30:17Z","timestamp":1762158617000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Coordination\u2010Induced Amplification of Birefringence and Nonlinear Optical Response in a Chiral Metal\u2013Organic Framework"],"prefix":"10.1002","volume":"65","author":[{"given":"Xinchao","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian 350002 P.R. 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