{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,2,17]],"date-time":"2026-02-17T23:11:31Z","timestamp":1771369891508,"version":"3.50.1"},"posted":{"date-parts":[[2026]]},"group-title":"SSRN","reference-count":50,"publisher":"Elsevier BV","content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"abstract":"<jats:p>Here we report a strategy to control ion assembly in Ionic Liquids (ILs) through the rational modulation of ion electrostatic distribution. To this end, the imidazolium core was systematically tri-substituted at the 2-, 4-, and 5-positions with halogens, yielding [CnC1X3Im][OTf] salts. While ab initio calculations confirmed altered charge distributions, Molecular Dynamics simulations and crystallographic studies revealed the corresponding structural changes: increasing the substituent electronegativity drives anions from in-plane positions to stacked arrangements above and below the ring, with progressive relocation of residual in-plane contacts. These results establish electrostatic tuning as a design principle to modulate three-dimensional ion architectures in ILs.<\/jats:p>","DOI":"10.2139\/ssrn.6258113","type":"posted-content","created":{"date-parts":[[2026,2,17]],"date-time":"2026-02-17T22:39:32Z","timestamp":1771367972000},"source":"Crossref","is-referenced-by-count":0,"title":["Charge Distribution-Driven Organization in Ionic Liquids"],"prefix":"10.2139","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-3646-0899","authenticated-orcid":true,"given":"Lois","family":"Morandeira","sequence":"first","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9461-9493","authenticated-orcid":true,"given":"Tiago  F. C.","family":"Cruz","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9615-8678","authenticated-orcid":true,"given":"Jos\u00e9  M. S. S.","family":"Esperan\u00e7a","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8148-2130","authenticated-orcid":true,"given":"M. \u00c1ngeles","family":"Sanroman","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8406-8763","authenticated-orcid":true,"given":"Pedro  T.","family":"Gomes","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4483-6294","authenticated-orcid":true,"given":"Jos\u00e9  N.","family":"Canongia Lopes","sequence":"additional","affiliation":[]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2454-1795","authenticated-orcid":true,"given":"Karina","family":"Shimizu","sequence":"additional","affiliation":[]}],"member":"78","reference":[{"key":"ref1","doi-asserted-by":"crossref","first-page":"13132","DOI":"10.1021\/acs.chemrev.0c01265","article-title":"Toward the Proactive Design of Sustainable Chemicals: Ionic Liquids as a Prime Example","volume":"121","author":"S Beil","year":"2021","journal-title":"Chem. 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