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We studied the structure at the liquid\/liquid interfaces of carbon tetrachloride (CCl4) and 1-alkyl-3-methylimidazolium bis(trifluoromethanesulfonyl)amide ([Cnmim][TFSA]; n = 4 and 8) RTILs using infrared\u2013visible sum frequency generation (SFG) vibrational spectroscopy. A comparison of the SFG spectra of the CCl4\/RTIL and air\/RTIL interfaces revealed that the solvation of the alkyl chains of the [Cnmim]+ cations by CCl4 reduces the number of gauche defects in the alkyl chain and the interface number density of the cation at the CCl4 interface. The orientational change of the [TFSA]\u2212 anion and concomitant increase in the area it occupies at the CCl4 interface was observed to be greater than that at the air interface. This is accompanied by the expansion of the space among the alkyl chains of the cations to be solvated by CCl4. The structural change of the CCl4 interface from the air interface can be attributed to the solvophilic effect of CCl4 on the alkyl chains of the cations at the CCl4\/[Cnmim][TFSA] interface. This is in contrast with the solvophobic effect of CCl4 on the Langmuir film at the CCl4\/water interface. This phenomenon is caused by the loosely packed alkyl chains of the cations at the RTIL surface and the flexible anion\u2013cation arrangement owing to the weak basicity and acidity of the ions in the RTILs.<\/jats:p>","DOI":"10.1063\/5.0237698","type":"journal-article","created":{"date-parts":[[2025,1,2]],"date-time":"2025-01-02T12:22:30Z","timestamp":1735820550000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":7,"title":["A sum-frequency generation vibrational spectroscopy studies on buried liquid\/liquid interfaces of CCl4\/[C<i>n<\/i>mim][TFSA] (<i>n<\/i> = 4 and 8) hydrophobic ionic liquids"],"prefix":"10.1063","volume":"162","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-2684-030X","authenticated-orcid":false,"given":"Takashi","family":"Iwahashi","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering, Tokyo Institute of Technology 1 , O-okayama, Meguro-ku, Tokyo 152-8552,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6909-9924","authenticated-orcid":false,"given":"Doseok","family":"Kim","sequence":"additional","affiliation":[{"name":"Department of Physics, Sogang University 2 , Seoul 121-742,","place":["Republic of Korea"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8437-4557","authenticated-orcid":false,"given":"Yukio","family":"Ouchi","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, Tokyo Institute of Technology 1 , O-okayama, Meguro-ku, Tokyo 152-8552,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2025,1,2]]},"reference":[{"issue":"13","key":"2025010212222457100_c1","doi-asserted-by":"publisher","first-page":"2133","DOI":"10.1039\/A902818H","article-title":"The phase behaviour of 1-alkyl-3-methylimidazolium tetrafluoroborates; ionid liquids and ionic liquid crystals","volume":"1999","journal-title":"J.\u00a0Chem. 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