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However, for most of low\u2010D OMHHs, especially the zero\u2010D (0D) compounds, the inferior electronic coupling between organic ligands and inorganic metal halides prevents efficient charge transfer at the hybrid interfaces and thus limits their further tunability of optical and electronic properties. Here, using pressure to regulate the interfacial interactions, efficient charge transfer from organic ligands to metal halides is achieved, which leads to a near\u2010unity photoluminescence quantum yield (PLQY) at around 6.0\u2005GPa in a 0D OMHH, [(C<jats:sub>6<\/jats:sub>H<jats:sub>5<\/jats:sub>)<jats:sub>4<\/jats:sub>P]<jats:sub>2<\/jats:sub>SbCl<jats:sub>5<\/jats:sub>. <jats:italic>In situ<\/jats:italic> experimental characterizations and theoretical simulations reveal that the pressure\u2010induced electronic coupling between the lone\u2010pair electrons of Sb<jats:sup>3+<\/jats:sup> and the \u03c0 electrons of benzene ring (lp\u2010\u03c0 interaction) serves as an unexpected \u201cbridge\u201d for the charge transfer. Our work opens a versatile strategy for the new materials design by manipulating the lp\u2010\u03c0 interactions in organic\u2013inorganic hybrid systems.<\/jats:p>","DOI":"10.1002\/anie.202304494","type":"journal-article","created":{"date-parts":[[2023,7,19]],"date-time":"2023-07-19T06:44:06Z","timestamp":1689749046000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":67,"title":["Anomalous Charge Transfer from Organic Ligands to Metal Halides in Zero\u2010Dimensional [(C<sub>6<\/sub>H<sub>5<\/sub>)<sub>4<\/sub>P]<sub>2<\/sub>SbCl<sub>5<\/sub> Enabled by Pressure\u2010Induced Lone Pair\u2010\u03c0 Interaction"],"prefix":"10.1002","volume":"62","author":[{"given":"Hui","family":"Luo","sequence":"first","affiliation":[{"name":"Center for High Pressure Science and Technology Advanced Research (HPSTAR)  201203 Shanghai 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