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Herein, the ion\u2013dipole interactions between a single poly[trifluoropropyl(methyl)siloxane] (PMTFPS) chain and 1-allyl-3-methylimidazolium chloride (AMIMCl) have been systematically investigated using single-molecule force spectroscopy combined with complementary techniques. For the first time, the isolated polymer\u2013ion system is shown to reach a state with stoichiometric-like saturated ion\u2013dipole bridges at an AMIMCl-to-PMTFPS repeating unit molar ratio of 0.33:1, in which one AMIMCl molecule bridges the two terminal trifluoropropyl groups within each three-unit segment. Further increasing the AMIMCl content allows for additional association with the intermediate trifluoropropyl group, but steric and electrostatic constraints prevent the formation of new bridges. The ion\u2013dipole binding energy is calculated to be 9.32 \u00b1 0.11\u00a0kJ\/mol. These results reveal the distinctive ion\u2013dipole combining pattern of a single polymer chain under molecular confinement. This work is expected to bridge the gap between the well-defined binding behaviors of small-molecule systems and the complex landscape of bulk macromolecular systems, offering mechanistic insights into how ion\u2013dipole interactions can be tuned within macromolecular materials.<\/jats:p>","DOI":"10.1063\/5.0312162","type":"journal-article","created":{"date-parts":[[2026,3,12]],"date-time":"2026-03-12T12:19:09Z","timestamp":1773317949000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":4,"title":["Stoichiometric-like ion\u2013dipole coordination saturation in an isolated polymer\u2013ion system: Single-molecule force spectroscopy and theoretical insights"],"prefix":"10.1063","volume":"164","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1181-8671","authenticated-orcid":false,"given":"Yu","family":"Bao","sequence":"first","affiliation":[{"name":"School of Chemistry, Southwest Jiaotong University 1 , Chengdu 610031,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuchen","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemistry, Southwest Jiaotong University 1 , Chengdu 610031,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wentao","family":"Yuan","sequence":"additional","affiliation":[{"name":"School of Chemistry, Southwest Jiaotong University 1 , Chengdu 610031,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yong","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Chemistry, Southwest Jiaotong University 1 , Chengdu 610031,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Minghan","family":"Hu","sequence":"additional","affiliation":[{"name":"School of Chemistry, Southwest Jiaotong University 1 , Chengdu 610031,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8149-8776","authenticated-orcid":false,"given":"Hu-jun","family":"Qian","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Supramolecular Structure and Materials, Institute of Theoretical Chemistry, Jilin University 2 , Changchun 130023,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7884-0091","authenticated-orcid":false,"given":"Zhong-yuan","family":"Lu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Supramolecular Structure and Materials, Institute of Theoretical Chemistry, Jilin University 2 , Changchun 130023,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7713-7377","authenticated-orcid":false,"given":"Shuxun","family":"Cui","sequence":"additional","affiliation":[{"name":"Department of Chemistry, College of Sciences, Northeastern University 3 , Shenyang 110819,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2026,3,12]]},"reference":[{"key":"2026031208190413500_c1","doi-asserted-by":"publisher","first-page":"723","DOI":"10.1021\/ar040223k","volume":"38","year":"2005","journal-title":"Acc. 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