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Here, we introduce halogen substitution on chiral molecular cations as a \u201cchirality editor\u201d to modulate the chiral electrostatic environment and thereby amplify spin\u2010selective transport in bismuth\u2010based hybrids. A series of nine (\n                    <jats:italic>S<\/jats:italic>\n                    \/\n                    <jats:italic>rac<\/jats:italic>\n                    \/\n                    <jats:italic>R<\/jats:italic>\n                    \u2010XPEA)\n                    <jats:sub>4<\/jats:sub>\n                    Bi\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>10<\/jats:sub>\n                    compounds, where X = F, Cl, or Br and XPEA = 1\u2010(4\u2010halophenyl)ethylamine, is systematically investigated, revealing that substitution from F to Br modulates molecular dipoles and local structural distortions, and enhances Rashba spin splitting. Consequently, chiroptical activity increases by nearly one order of magnitude and spin polarization efficiency rises from 68% to 89%, as confirmed by magnetoconductive atomic force microscopy. The amplified chiral\u2010induced spin selectivity (CISS) effect yields a 3.4\u2010fold enhancement in carrier mobility\u2010lifetime product (\n                    <jats:italic>\u03bc\u03c4<\/jats:italic>\n                    up to 3.26\u00a0\u00d7\u00a010\n                    <jats:sup>\u22123<\/jats:sup>\n                    cm\n                    <jats:sup>2<\/jats:sup>\n                    V\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) while simultaneously reducing dark\u2010current drift by threefold. The optimized Br\u2010substituted homochiral flexible X\u2010ray detector achieves a sensitivity of 8865.82 \u00b1 403 \u00b5C Gy\n                    <jats:sup>\u22121<\/jats:sup>\n                    cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and an ultralow detection limit of 7.16 nGy s\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Overall, this work establishes a structure\u2010property\u2010performance framework that positions halogen\u2010based \u201cchirality editing\u201d as an efficient strategy for high\u2010performance radiation detectors.\n                  <\/jats:p>","DOI":"10.1002\/anie.3778438","type":"journal-article","created":{"date-parts":[[2026,8,14]],"date-time":"2026-08-14T16:39:26Z","timestamp":1786725566000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Halogen Substitution as a \u201cChirality Editor\u201d for Amplifying Spin\u2010Selective Transport in Lead\u2010Free Metal\u2010Halide Hybrids"],"prefix":"10.1002","volume":"65","author":[{"given":"Xinmei","family":"Liu","sequence":"first","affiliation":[{"name":"Key Laboratory of Applied Surface and Colloid Chemistry, National Ministry of Education, Shaanxi Provincial Basic Discipline (Surface and Interface Chemistry) Research Center School of Materials Science and Engineering, Shaanxi Normal University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyi","family":"Geng","sequence":"additional","affiliation":[{"name":"Key Laboratory of Applied Surface and Colloid Chemistry, National Ministry of Education, Shaanxi Provincial Basic Discipline (Surface and Interface Chemistry) Research Center School of Materials Science and Engineering, Shaanxi Normal University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuting","family":"Xu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Flexible Electronics Institute of Flexible Electronics (IFE) Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Aowen","family":"Ma","sequence":"additional","affiliation":[{"name":"Department of Applied Physics Research Center for Organic Electronics The Hong Kong Polytechnic University  Hong Kong 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Ministry of Education, Shaanxi Provincial Basic Discipline (Surface and Interface Chemistry) Research Center School of Materials Science and Engineering, Shaanxi Normal University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyue","family":"Ma","sequence":"additional","affiliation":[{"name":"Key Laboratory of Applied Surface and Colloid Chemistry, National Ministry of Education, Shaanxi Provincial Basic Discipline (Surface and Interface Chemistry) Research Center School of Materials Science and Engineering, Shaanxi Normal University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenqing","family":"Tian","sequence":"additional","affiliation":[{"name":"Key Laboratory of Applied Surface and Colloid Chemistry, National Ministry of Education, Shaanxi Provincial Basic Discipline (Surface and Interface Chemistry) Research Center School of Materials Science and Engineering, Shaanxi Normal University  Xi'an 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