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Herein, we develop a molecular design strategy by constructing a donor\u2010\u03c0\u2010acceptor (D\u2010\u03c0\u2010A) long\u2010chain cation, [DA7ClQ]\n                    <jats:sup>2+<\/jats:sup>\n                    , featuring multiple hydrogen\u2010bonding sites. Hybridization with inorganic [Sb\n                    <jats:sub>2<\/jats:sub>\n                    Cl\n                    <jats:sub>9<\/jats:sub>\n                    ]\n                    <jats:sup>3\u2212<\/jats:sup>\n                    anions yields the non\u2010centrosymmetric crystal (DA7ClQ)SbCl\n                    <jats:sub>5<\/jats:sub>\n                    , which exhibits a record birefringence of 0.46 at 550\u00a0nm among OIMHs\u2010based NLO crystals, coupled with a robust SHG response of 0.4 \u00d7 KTP at 1550\u00a0nm and exceptional thermal and environmental stability. Theoretical calculations reveal that the D\u2010\u03c0\u2010A motif possesses superior first\u2010order hyperpolarizability (12.1 \u00d7 10\n                    <jats:sup>\u221229<\/jats:sup>\n                    esu) and polarizability anisotropy (739 a.u.), while a robust hydrogen\u2010bond network locks the acentric alignment. This work establishes that engineering extended \u03c0\u2010conjugated systems with augmented asymmetry and precise orientational control provides a versatile pathway toward advanced hybrid NLO materials.\n                  <\/jats:p>","DOI":"10.1002\/anie.2193506","type":"journal-article","created":{"date-parts":[[2026,5,22]],"date-time":"2026-05-22T13:39:14Z","timestamp":1779457154000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Engineering Multiple Hydrogen\u2010Bond Sites With D\u2010\u03c0\u2010A Motifs for Strong Optical Nonlinearity and Giant Birefringence in Organic\u2010Inorganic Halides"],"prefix":"10.1002","volume":"65","author":[{"given":"Yangkai","family":"Zhang","sequence":"first","affiliation":[{"name":"College of Physics Qingdao Key Laboratory of Ultrabroadband Terahertz Crystals and System Applications Qingdao Broadband Terahertz Spectroscopy Technology Engineering Research Center Qingdao 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