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Herein, we report a design principle for spontaneous polarization\u2010enhanced scintillation in 2D organic\u2013inorganic hybrid perovskites. As anticipated, the (4\u2010aminomethyl\u20101\u2010cyclohexanecarboxylate)\n                    <jats:sub>2<\/jats:sub>\n                    PbBr\n                    <jats:sub>4<\/jats:sub>\n                    (APB) perovskite displays high light yield up to 19\u00a0660 photons\/MeV and a lifetime of 0.90\u00a0ns. Combining the experimental and computational results, we demonstrate that enhancement of dielectric screening effect and suppression of free carrier recombination are responsible for the ultrafast decay time and high light yield, respectively. Moreover, the practical applications for fast neutron imaging and flash X\u2010ray radiography are successfully demonstrated with excellent spatial resolutions of 2.4 and 31 lp\/mm, respectively. In addition, the potential for PET technique is verified by shorter CTR values than (Lu\n                    <jats:sub>x<\/jats:sub>\n                    Y\n                    <jats:sub>1\u2010x<\/jats:sub>\n                    )\n                    <jats:sub>2<\/jats:sub>\n                    SiO\n                    <jats:sub>5<\/jats:sub>\n                    : Ce (LYSO). This work will open up a new avenue for developing high\u2010performance ultrafast scintillators for practical applications in biomedical and nuclear detection techniques.\n                  <\/jats:p>","DOI":"10.1002\/adma.202517639","type":"journal-article","created":{"date-parts":[[2026,2,3]],"date-time":"2026-02-03T09:41:26Z","timestamp":1770111686000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Bright 2D Polar Perovskite Scintillator with Ultrafast Decay by Suppressing Free Carrier Recombination"],"prefix":"10.1002","volume":"38","author":[{"given":"Zizhen","family":"Bao","sequence":"first","affiliation":[{"name":"School of Physics and Astronomy Beijing Normal University  Beijing P. R. China"},{"name":"School of Nuclear Science and Technology Xi'an Jiaotong University  Xi'an P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuanma","family":"Yan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Flexible Electronics (LoFE) &amp; Institute of Advanced Materials (IAM) School of Flexible Electronics (Future Technologies) Nanjing Tech University (Nanjing Tech)  Nanjing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhihua","family":"Sun","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystals and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fujian P. R. 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