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The electrostatic equations for polarizable surfaces are solved using a 2D periodic Green\u2019s function method combined with a slab-corrected anisotropic 3D Ewald summation. We apply this approach in Monte Carlo simulations to study 1:1 electrolytes confined between both polarizable dielectric and metallic surfaces. Our results show that dielectric anisotropy strongly reshapes the double-layer structure. While the individual ion\u2013image interactions depend strictly on the bulk-like parallel permittivity, the suppression of the perpendicular permittivity dramatically amplifies direct in-plane ion\u2013ion correlations. Under strong anisotropy, these lateral correlations dominate the thermodynamics completely, rendering the structural profiles of mutually opposing dielectric and metallic boundaries practically identical by forcing the smaller cations directly into the contact plane of the larger anions.<\/jats:p>","DOI":"10.1063\/5.0345366","type":"journal-article","created":{"date-parts":[[2026,10,22]],"date-time":"2026-10-22T10:48:14Z","timestamp":1792666094000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Electrolytes confined between polarizable surfaces in slit pores with anisotropic permittivity tensor"],"prefix":"10.1063","volume":"165","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5965-3992","authenticated-orcid":false,"given":"Alexandre P.","family":"dos Santos","sequence":"first","affiliation":[{"name":"Instituto de F\u00edsica, Universidade Federal do Rio Grande do Sul , Caixa Postal 15051, CEP 91501-970 Porto Alegre, RS,","place":["Brazil"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0636-7300","authenticated-orcid":false,"given":"Yan","family":"Levin","sequence":"additional","affiliation":[{"name":"Instituto de F\u00edsica, Universidade Federal do Rio Grande do Sul , Caixa Postal 15051, CEP 91501-970 Porto Alegre, RS,","place":["Brazil"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2026,10,22]]},"reference":[{"key":"2026102206480830700_c1","doi-asserted-by":"publisher","first-page":"8333","DOI":"10.1021\/acs.langmuir.5c05917","volume":"42","year":"2026","journal-title":"Langmuir"},{"key":"2026102206480830700_c2","doi-asserted-by":"publisher","first-page":"10532","DOI":"10.1021\/acs.jpclett.0c03219","volume":"11","year":"2020","journal-title":"J.\u00a0Phys. 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