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However, it remains a major challenge to achieve the desired phosphorescent properties due to the limited regulatory methods and indistinct mechanism. Herein, the coordination solvent and second metal ion costrategy is firstly proposed to prepare seven robust heterometallic\u2013organic frameworks (HMOFs) with two configurations, <jats:bold>ZnMg\/Ca\u2010sol<\/jats:bold> [sol\u00a0=\u00a0H<jats:sub>2<\/jats:sub>O, dimethylformamide (DMF), dimethylacetamide (DMA), and formyldiethylamine (DEF)] and <jats:bold>ZnSr\/Ba\u2010H<jats:sub>2<\/jats:sub>O<\/jats:bold>, exhibiting different ultralong RTP. The tunable phosphorescence lifetimes within 14.5\u2013195.4\u00a0ms are achieved gradually by altering the type of alkaline earth metals, coordination solvent, and hydrogen\u2010bonding in the HMOFs. Significantly, the theoretical calculations reveal that the promotion of spin\u2013orbit coupling by heavy metals and the rigid constraint on the skeleton by solvent result in excellent balance between high phosphorescence quantum yield (<jats:italic>\u0424<\/jats:italic><jats:sub>P<\/jats:sub>) and long lifetime, especially for <jats:bold>ZnSr\u2010H<jats:sub>2<\/jats:sub>O<\/jats:bold> (6.8%, 195.4\u00a0ms). Depending on the wide\u2010range tuning of ultralong RTP and great stability, the HMOFs are successfully applied in spatial\u2010time resolved anticounterfeiting and multilevel information encryption. This work may provide a new approach to designing target phosphorescent materials while resolving the contradiction between high <jats:italic>\u0424<\/jats:italic><jats:sub>P<\/jats:sub> and long lifetime.<\/jats:p>","DOI":"10.1002\/anie.202501951","type":"journal-article","created":{"date-parts":[[2025,3,12]],"date-time":"2025-03-12T05:38:14Z","timestamp":1741757894000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":34,"title":["Engineering Solvent\u2010Coordinated Heterometallic\u2013Organic Frameworks for Wide\u2010Range Tuning of Ultralong Room Temperature Phosphorescence toward Time\u2010Resolved Anticounterfeiting"],"prefix":"10.1002","volume":"64","author":[{"given":"Juanjuan","family":"Xue","sequence":"first","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education Shaanxi Key Laboratory of Physico\u2010Inorganic Chemistry Xi'an Key Laboratory of Functional Supramolecular Structure and Materials College of Chemistry and Materials Science Northwest University  Xi'an 710127 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhenhong","family":"Qi","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Energy Conversion and Storage Materials, and Key Laboratory of Radiopharmaceuticals Ministry of Education College of Chemistry Beijing Normal University  Beijing 100875 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongpeng","family":"Yan","sequence":"additional","affiliation":[{"name":"Beijing Key Laboratory of Energy Conversion and Storage Materials, and Key Laboratory of Radiopharmaceuticals Ministry of Education College of Chemistry Beijing Normal University  Beijing 100875 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guo\u2010Ping","family":"Yang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education Shaanxi Key Laboratory of Physico\u2010Inorganic Chemistry Xi'an Key Laboratory of Functional Supramolecular Structure and Materials College of Chemistry and Materials Science Northwest University  Xi'an 710127 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yao\u2010Yu","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education Shaanxi Key Laboratory of Physico\u2010Inorganic Chemistry Xi'an Key Laboratory of Functional Supramolecular Structure and Materials College of Chemistry and Materials Science Northwest University  Xi'an 710127 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,3,12]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202204744"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2022.214523"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202103321"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/D2CS00993E"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202207985"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-47674-x"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202315911"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202217284"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202407420"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202114100"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-23742-4"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202412350"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202312491"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-020-0223-z"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202107612"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202300021"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202311659"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202403977"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2024.150919"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202313749"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2019.213107"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202108025"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1002\/agt2.125"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202007571"},{"key":"e_1_2_7_25_1","volume":"63","author":"Wang Z. 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