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Here, the cross-plane electric field at the electrode surface modulates the refractive index of the IL due to the Pockels effect. This is observed as a shift in the resonant angle of the grating (i.e., \u0394\u03d5), which can be related to the change in the local index of refraction of the electrolyte (i.e., \u0394nlocal). The reflection modulation of the IL is compared against a polar (D2O) and a non-polar solvent (benzene) to confirm the electro-optic origin of resonance shift. The electrostatic accumulation of ions from the IL induces local index changes to the gratings over the extent of electrical double layer (EDL) thickness. Finite difference time domain simulations are used to relate the observed shifts in the plasmon resonance and change in reflection to the change in the local index of refraction of the electrolyte and the thickness of the EDL. Simultaneously using the wavelength and intensity shift of the resonance enables us to determine both the effective thickness and \u0394n of the double layer. We believe that this technique can be used more broadly, allowing the dynamics associated with the potential-induced ordering and rearrangement of ionic species in electrode\u2013solution interfaces.<\/jats:p>","DOI":"10.1063\/5.0202642","type":"journal-article","created":{"date-parts":[[2024,7,15]],"date-time":"2024-07-15T09:54:33Z","timestamp":1721037273000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":2,"title":["Voltage-induced modulation of interfacial ionic liquids measured using surface plasmon resonant grating nanostructures"],"prefix":"10.1063","volume":"161","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0908-9887","authenticated-orcid":false,"given":"Indu","family":"Aravind","sequence":"first","affiliation":[{"name":"Department of Physics and Astronomy 1 , University of Southern California, Los Angeles, California 90089, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0307-1301","authenticated-orcid":false,"given":"Yu","family":"Wang","sequence":"additional","affiliation":[{"name":"Mork Family Department of Chemical Engineering and Materials Science 2 , University of Southern California, Los Angeles, California 90089, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3741-5715","authenticated-orcid":false,"given":"Zhi","family":"Cai","sequence":"additional","affiliation":[{"name":"Mork Family Department of Chemical Engineering and Materials Science 2 , University of Southern California, Los Angeles, California 90089, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6432-6072","authenticated-orcid":false,"given":"Ruoxi","family":"Li","sequence":"additional","affiliation":[{"name":"Mork Family Department of Chemical Engineering and Materials Science 2 , University of Southern California, Los Angeles, California 90089, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1245-6753","authenticated-orcid":false,"given":"Rifat","family":"Shahriar","sequence":"additional","affiliation":[{"name":"Ming Hsieh Department of Electrical Engineering 3 , University of Southern California, Los Angeles, California 90089, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7537-2680","authenticated-orcid":false,"given":"George N.","family":"Gibson","sequence":"additional","affiliation":[{"name":"Department of Physics, University of Connecticut 4 , Storrs, Connecticut 06269, USA"},{"name":"Ciencia Inc. 5 , East Hartford, Connecticut 06108, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Ernest","family":"Guignon","sequence":"additional","affiliation":[{"name":"Ciencia Inc. 5 , East Hartford, Connecticut 06108, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4345-3627","authenticated-orcid":false,"given":"Nathaniel C.","family":"Cady","sequence":"additional","affiliation":[{"name":"Colleges of Nanoscale Science and Engineering, SUNY Polytechnic Institute 6 , Albany, New York 12203, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-3116-9478","authenticated-orcid":false,"given":"William D.","family":"Page","sequence":"additional","affiliation":[{"name":"Ciencia Inc. 5 , East Hartford, Connecticut 06108, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Arturo","family":"Pilar","sequence":"additional","affiliation":[{"name":"Ciencia Inc. 5 , East Hartford, Connecticut 06108, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9153-7687","authenticated-orcid":false,"given":"Stephen B.","family":"Cronin","sequence":"additional","affiliation":[{"name":"Department of Physics and Astronomy 1 , University of Southern California, Los Angeles, California 90089, USA"},{"name":"Ming Hsieh Department of Electrical Engineering 3 , University of Southern California, Los Angeles, California 90089, USA"},{"name":"Department of Chemistry, University of Southern California 7 , Los Angeles, California 90089, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"317","published-online":{"date-parts":[[2024,7,15]]},"reference":[{"key":"2024071509541269800_c1","doi-asserted-by":"publisher","first-page":"9464","DOI":"10.1021\/acs.jpclett.2c02768","article-title":"Innermost ion association configuration is a key structural descriptor of ionic liquids at electrified interfaces","volume":"13","year":"2022","journal-title":"J.\u00a0Phys. 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