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So far methodological challenges limited probing structures of the fragments. Herein, we resolve the geometric structures of the primary fragments of [Ag<jats:sub>29<\/jats:sub>L<jats:sub>12<\/jats:sub>]<jats:sup>3\u2212<\/jats:sup>, i.e. [Ag<jats:sub>24<\/jats:sub>L<jats:sub>9<\/jats:sub>]<jats:sup>2\u2212<\/jats:sup>, [Ag<jats:sub>19<\/jats:sub>L<jats:sub>6<\/jats:sub>]<jats:sup>\u2212<\/jats:sup> and [Ag<jats:sub>5<\/jats:sub>L<jats:sub>3<\/jats:sub>]<jats:sup>\u2212<\/jats:sup> (L is 1,3\u2010benzene dithiolate). For this, we used trapped ion mobility mass spectrometry to determine collision cross sections of the fragments and compared them to structures calculated by density functional theory. We also report that following two sequential [Ag<jats:sub>5<\/jats:sub>L<jats:sub>3<\/jats:sub>]<jats:sup>\u2212<\/jats:sup> elimination steps, further dissociation of [Ag<jats:sub>19<\/jats:sub>L<jats:sub>6<\/jats:sub>]<jats:sup>\u2212<\/jats:sup> also involves a new channel of Ag<jats:sub>2<\/jats:sub> loss and Ag\u2212S and C\u2212S bond cleavages. This reflects a competition between retaining the electronic stability of 8\u2009e<jats:sup>\u2212<\/jats:sup> superatom cluster cores and increasing steric strain of ligands and staples. These results are also of potential interest for future soft\u2010landing deposition studies aimed at probing catalytic behavior of Ag clusters on supports.<\/jats:p>","DOI":"10.1002\/anie.202305836","type":"journal-article","created":{"date-parts":[[2023,5,22]],"date-time":"2023-05-22T17:20:32Z","timestamp":1684776032000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Elucidating the Structures of Intermediate Fragments during Stepwise Dissociation of Monolayer\u2010Protected Silver Clusters"],"prefix":"10.1002","volume":"62","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1353-7734","authenticated-orcid":false,"given":"Papri","family":"Chakraborty","sequence":"first","affiliation":[{"name":"Institute of Nanotechnology Karlsruhe Institute of Technology  76344 Eggenstein-Leopoldshafen Germany"},{"name":"Institute of Physical Chemistry Karlsruhe Institute of Technology  76131 Karlsruhe 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