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This approach reveals that, under the conditions used here (20 \u03bcm diameter KCl electrolyte meniscus, ca. 40\u201360% relative humidity, ITO partial wetting properties, and several tens of seconds of contact time), a nanometric electrolyte film extends beyond the visible meniscus, over several micrometers. This expands the three-phase region, enabling nanocatalytic sites located outside the meniscus-confined electrochemical cell to react. During cathodic polarization, IRM monitors these beyond-meniscus events through the appearance of emerging optical features associated with the formation of localized electrolyte microdroplets and dendritic metallic structures. These events are quantified at the single-entity level, particularly in the framework of the capillary work associated with microdroplet growth and relaxation. This analysis shows that fA-level electrochemical activity can be partly converted into mechanical capillary work via electrolyte transport through the nanometric electrolyte film. We finally discuss how such thin-film-mediated peripheral activity can potentially bias meniscus-confined electrochemical measurements.<\/jats:p>","DOI":"10.1021\/cbmi.6c00040","type":"journal-article","created":{"date-parts":[[2026,7,6]],"date-time":"2026-07-06T23:34:48Z","timestamp":1783380888000},"page":"1858-1868","source":"Crossref","is-referenced-by-count":0,"title":["Operando Optical Imaging Reveals Beyond-Meniscus Nanoelectrochemistry\nMediated by a Nanometric Wetting Film"],"prefix":"10.1021","volume":"4","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-2763-0408","authenticated-orcid":true,"given":"Louis","family":"Godeffroy","sequence":"first","affiliation":[{"name":"ENS, Universite\u0301 PSL, CNRS, Sorbonne Universite\u0301, Universite\u0301 Paris Cite\u0301 , , ,","place":["Paris, France, F-75005"]},{"name":"Universite\u0301 Paris Cite\u0301, CNRS, ITODYS , ,","place":["Paris, France, F-75013"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hugo","family":"Chotard","sequence":"additional","affiliation":[{"name":"Colle\u0300ge de France , , ,","place":["Paris Cedex, France, 75231"]},{"name":"Re\u0301seau sur le Stockage Electrochimique de l\u2019Energie (RS2E), CNRS FR 3459 , ,","place":["Amiens Cedex, France, 80039"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ivette","family":"Aguilar","sequence":"additional","affiliation":[{"name":"Colle\u0300ge de France , , ,","place":["Paris Cedex, France, 75231"]},{"name":"Re\u0301seau sur le Stockage Electrochimique de l\u2019Energie (RS2E), CNRS FR 3459 , ,","place":["Amiens Cedex, France, 80039"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Viacheslav","family":"Shkirskiy","sequence":"additional","affiliation":[{"name":"Universite\u0301 Paris Cite\u0301, CNRS, ITODYS , ,","place":["Paris, France, F-75013"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jean-Marc","family":"Noe\u0308l","sequence":"additional","affiliation":[{"name":"Universite\u0301 Paris Cite\u0301, CNRS, ITODYS , ,","place":["Paris, France, F-75013"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9635-2737","authenticated-orcid":true,"given":"Jean-Franc\u0327ois","family":"Lemineur","sequence":"additional","affiliation":[{"name":"Universite\u0301 Paris Cite\u0301, CNRS, ITODYS , ,","place":["Paris, France, F-75013"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9784-2380","authenticated-orcid":true,"given":"Fre\u0301de\u0301ric","family":"Kanoufi","sequence":"additional","affiliation":[{"name":"Universite\u0301 Paris Cite\u0301, CNRS, ITODYS , ,","place":["Paris, France, F-75013"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,6]]},"reference":[{"issue":"20","key":"2026083104094505000_cit1","doi-asserted-by":"publisher","first-page":"3539","DOI":"10.1021\/jz501898r","article-title":"Electrochemical\nMeasurements of Single H2 Nanobubble Nucleation and Stability at Pt\nNanoelectrodes","volume":"5","author":"Chen","year":"2014","journal-title":"J. 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