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Here, we investigate a supramolecularly stabilized, formally tetracationic [Bi4]4+ ring by combining structurally meaningful reference compounds, solid- and solution-state NMR spectroscopy, SQUID magnetometry, and exact two-component relativistic calculations. Comparison with an isostructural [Li4Br]3+-encapsulated analogue and a binuclear Bi(III) reference compound disentangles global ring-current effects from local heavy-atom deshielding and ligand-specific conformational effects. On this basis, the unusually downfield-shifted 1H and 13C NMR signals observed for the Bi4-containing species provide direct spectroscopic evidence for magnetically induced ring currents in the [Bi4]4+ core. By contrast, bulk magnetic measurements do not reveal significant diamagnetic exaltation, indicating that this quantity is not a resolved descriptor of aromaticity in these systems. Stoichiometric studies further identify chemically competent intermediates that provide mechanistic snapshots of [Bi4]4+ ring formation. Complementary calculations support the assignment of a magnetically responsive, \u03c3-delocalized [Bi4]4+ core, reproduce a rare spectroscopically observed puckering motion of the rhomboidal [Bi4]4+, and underscore the critical role of spin\u2013orbit coupling on electronic structure and dynamics. Overall, this work moves the discussion of aromaticity from predominantly computational assignment toward experimentally benchmarked analysis in the heavy-element and all-metal regime.<\/jats:p>","DOI":"10.1021\/jacs.6c14973","type":"journal-article","created":{"date-parts":[[2026,10,10]],"date-time":"2026-10-10T01:02:05Z","timestamp":1791594125000},"page":"44889-44900","source":"Crossref","is-referenced-by-count":0,"title":["NMR Spectroscopic Evidence\nfor Magnetically Induced\nRing Currents in All-Metal-Aromatic [Bi4]4+"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8388-3096","authenticated-orcid":true,"given":"Avijit","family":"Maiti","sequence":"first","affiliation":[{"name":"Universita\u0308t Heidelberg , , ,","place":["Heidelberg, Germany, 69120"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie","family":"Zhang","sequence":"additional","affiliation":[{"name":"Universita\u0308t Heidelberg , , ,","place":["Heidelberg, Germany, 69120"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2375-7607","authenticated-orcid":true,"given":"Ravi","family":"Yadav","sequence":"additional","affiliation":[{"name":"Universita\u0308t Heidelberg , , ,","place":["Heidelberg, Germany, 69120"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Matthias","family":"Heinrich","sequence":"additional","affiliation":[{"name":"Universita\u0308t Heidelberg , , ,","place":["Heidelberg, Germany, 69120"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Luca","family":"Bischof","sequence":"additional","affiliation":[{"name":"Universita\u0308t Heidelberg , , ,","place":["Heidelberg, Germany, 69120"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Adrian","family":"Ellinger","sequence":"additional","affiliation":[{"name":"Karlsruhe Institute of Technology , , ,","place":["Eggenstein-Leopoldshafen, Germany, 76344"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1670-4099","authenticated-orcid":true,"given":"Manuel","family":"Schmitt","sequence":"additional","affiliation":[{"name":"Universita\u0308t Heidelberg , , ,","place":["Heidelberg, Germany, 69120"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ru\u0308diger","family":"Klingeler","sequence":"additional","affiliation":[{"name":"Universita\u0308t Heidelberg , , ,","place":["Heidelberg, Germany, 69120"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Florian","family":"Weigend","sequence":"additional","affiliation":[{"name":"Karlsruhe Institute of Technology , , ,","place":["Eggenstein-Leopoldshafen, Germany, 76344"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5253-419X","authenticated-orcid":true,"given":"Lutz","family":"Greb","sequence":"additional","affiliation":[{"name":"Universita\u0308t Heidelberg , , ,","place":["Heidelberg, Germany, 69120"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,9]]},"reference":[{"issue":"10","key":"2026102111095362200_cit1a","doi-asserted-by":"publisher","first-page":"3716","DOI":"10.1021\/cr030091t","article-title":"All-Metal Aromaticity and Antiaromaticity","volume":"105","author":"Boldyrev","year":"2005","journal-title":"Chem. 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A novel coordination mode in \u201cporphyrin-like\u201d\nchemistry","volume":"38","author":"Cuesta","year":"2009","journal-title":"Chem. Soc. Rev."},{"key":"2026102111095362200_cit20b","doi-asserted-by":"publisher","first-page":"11751","DOI":"10.1039\/D1CC05120B","article-title":"Calix[4]pyrroles as\nligands: recent progress with a focus on the emerging p-block element\nchemistry","volume":"57","author":"Ruppert","year":"2021","journal-title":"Chem. Commun."},{"issue":"13","key":"2026102111095362200_cit20c","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202116615","article-title":"Calix[4]pyrrolato Stannate(II):\nA Tetraamido Tin(II) Dianion and Strong Metal-Centered \u03c3-Donor","volume":"61","author":"Ruppert","year":"2022","journal-title":"Angew. Chem., Int. 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