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However, their strong dipole\u2010dipole interactions remain a key challenge in designing non\u2010centrosymmetric structures. To overcome this, we proposed a novel non\u2010centrosymmetric structure design strategy based on the local proton distribution complementary effect. Importantly, it could induce the groups to form a zigzag ordered arrangement along the direction perpendicular to the \u03c0\u2010conjugated plane, thereby significantly increasing the probability of forming non\u2010centrosymmetric structures. Based on this strategy, we successfully designed and synthesized two novel solar\u2010blind ultraviolet non\u2010centrosymmetric crystals, (C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>5<\/jats:sub>\n                    )Na\n                    <jats:sub>3<\/jats:sub>\n                    (S\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    \u03872H\n                    <jats:sub>2<\/jats:sub>\n                    O and (C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>5<\/jats:sub>\n                    )ClO\n                    <jats:sub>4<\/jats:sub>\n                    \u0387(C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    ), with imidazolium\/imidazole groups. Both crystals exhibit excellent optical performances, with a large birefringence of 0.158 @ 546\u00a0nm in (C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>5<\/jats:sub>\n                    )ClO\n                    <jats:sub>4<\/jats:sub>\n                    \u0387(C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>4<\/jats:sub>\n                    ) and a strong NLO effect approximately 2.6 times that of KH\n                    <jats:sub>2<\/jats:sub>\n                    PO\n                    <jats:sub>4<\/jats:sub>\n                    in (C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>2<\/jats:sub>\n                    H\n                    <jats:sub>5<\/jats:sub>\n                    )Na\n                    <jats:sub>3<\/jats:sub>\n                    (S\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>3<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    \u03872H\n                    <jats:sub>2<\/jats:sub>\n                    O, which mainly result from the intrinsic characteristics of imidazolium\/imidazole groups and their ordered arrangement. Consequently, this work not only develops two promising solar\u2010blind UV NLO crystals but also offers a novel structure design strategy that is expected to promote the development of NLO materials.\n                  <\/jats:p>","DOI":"10.1002\/anie.6572259","type":"journal-article","created":{"date-parts":[[2026,8,11]],"date-time":"2026-08-11T12:23:50Z","timestamp":1786451030000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Designing Novel Solar\u2010Blind Ultraviolet Nonlinear Optical Crystals Based on Local Proton Distribution Complementary Effect"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8559-2145","authenticated-orcid":false,"given":"Hongyuan","family":"Sha","sequence":"first","affiliation":[{"name":"Research Center for Crystal Materials CAS Key Laboratory of Functional Materials and Devices for Special Environmental Conditions Xinjiang Key Laboratory of 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