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However, their inherent instability, prone to decomposition upon exposure to moisture and light, hinders their broader ferroelectric applications. Herein, for the first time, we present a series of isoreticular metal\u2013organic framework (MOF)\u2010type lead halide luminescent ferroelectrics, demonstrating exceptional robustness under ambient conditions for at least 15\u2005months and even when subjected to aqueous boiling conditions. Unlike conventional metal\u2010oxo secondary building units (SBUs) in MOFs adopting highly centrosymmetric structure with limited structural distortion, our lead halide\u2010based MOFs occupy structurally deformable [Pb<jats:sub>2<\/jats:sub>X]<jats:sup>+<\/jats:sup> (X=Cl<jats:sup>\u2212<\/jats:sup>\/Br<jats:sup>\u2212<\/jats:sup>\/I<jats:sup>\u2212<\/jats:sup>) SBUs that facilitate a <jats:italic>c<\/jats:italic>\u2010axis\u2010biased displacement of Pb<jats:sup>2+<\/jats:sup> centers and substantially contribute to thermoinducible structural transformation. Importantly, this class of MOF\u2010type lead halide ferroelectrics undergo ferroelectric\u2010to\u2010paraelectric phase transitions with remarkably high Curie temperature of up to 505\u2005K, superior to most of molecular ferroelectrics. Moreover, the covalent bonding between phosphorescent organic component and the light\u2010harvesting inorganic component achieves efficient spin\u2010orbit coupling and intersystem crossing, resulting in long\u2010lived afterglow emission. The compelling combination of high stability, ferroelectricity and afterglow emission exhibited by lead halide MOFs opens up many potential opportunities in energy\u2010conversion applications.<\/jats:p>","DOI":"10.1002\/anie.202407102","type":"journal-article","created":{"date-parts":[[2024,5,15]],"date-time":"2024-05-15T02:25:51Z","timestamp":1715739951000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":26,"title":["Highly Stable MOF\u2010Type Lead Halide Luminescent Ferroelectrics"],"prefix":"10.1002","volume":"63","author":[{"given":"Chen","family":"Sun","sequence":"first","affiliation":[{"name":"Shanghai Key Laboratory of Chemical Assessment and Sustain ability School of Chemical Science and Engineering Tongji University  1239 Siping Rd. Shanghai 200092 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yukong","family":"Li","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Chemical Assessment and Sustain ability School of Chemical Science and Engineering Tongji University  1239 Siping Rd. Shanghai 200092 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinlin","family":"Yin","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Chemical Assessment and Sustain ability School of Chemical Science and Engineering Tongji University  1239 Siping Rd. Shanghai 200092 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongyang","family":"Li","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Chemical Assessment and Sustain ability School of Chemical Science and Engineering Tongji University  1239 Siping Rd. 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