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However, in ambient conditions, it is unclear how water solvates nanogaps and even if nominally dry, what water structure persists. Despite its low Raman cross\u2010section, surface\u2010enhanced Raman spectroscopy (SERS) enables the study of water at coinage metal surfaces. Using multi\u2010layer aggregates of close\u2010packed gold nanoparticles with sub\u2010nanometer gaps precisely defined by organic spacer molecules, consistent and large SERS enhancements are achieved, enabling a systematic study of water within these confined spaces. Ostensibly dry facets in air evidence water monolayer coatings, with hydrogen\u2010bonding only reappearing upon immersion in solution. Under negative applied potentials, surface water is seen to re\u2010orient at the metal facets with distinct spectral shifts among the quartet of vibrational peaks that correspond to those expected from interacting water dimers. Comparing nanogaps in deuterated water also reveals how individual water molecules bind onto organic spacer molecules in such nanogaps. Realistic models of water dressing will enable a better understanding of catalytic and contact chemistries.<\/jats:p>","DOI":"10.1002\/smll.202507013","type":"journal-article","created":{"date-parts":[[2025,10,25]],"date-time":"2025-10-25T08:53:36Z","timestamp":1761382416000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Tracking and Controlling Monolayer Water in Gold Nanogaps using Extreme Plasmonic Spectroscopy"],"prefix":"10.1002","volume":"21","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-5372-8217","authenticated-orcid":false,"given":"Elle W.","family":"Wyatt","sequence":"first","affiliation":[{"name":"NanoPhotonics Centre, Cavendish Laboratory, Department of Physics University of Cambridge JJ Thompson Avenue Cambridge CB3 0US UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6015-4090","authenticated-orcid":false,"given":"Sarah May","family":"Sibug\u2010Torres","sequence":"additional","affiliation":[{"name":"NanoPhotonics Centre, Cavendish Laboratory, Department of Physics University of Cambridge JJ Thompson Avenue Cambridge CB3 0US UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8355-2158","authenticated-orcid":false,"given":"Rakesh","family":"Arul","sequence":"additional","affiliation":[{"name":"NanoPhotonics Centre, Cavendish Laboratory, Department of Physics University of Cambridge JJ Thompson Avenue Cambridge CB3 0US UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7701-4660","authenticated-orcid":false,"given":"Marika","family":"Niihori","sequence":"additional","affiliation":[{"name":"NanoPhotonics Centre, Cavendish Laboratory, Department of Physics University of Cambridge JJ Thompson Avenue Cambridge CB3 0US UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7864-2263","authenticated-orcid":false,"given":"Tabitha","family":"Jones","sequence":"additional","affiliation":[{"name":"NanoPhotonics Centre, Cavendish Laboratory, Department of Physics University of Cambridge JJ Thompson Avenue Cambridge CB3 0US UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4028-0150","authenticated-orcid":false,"given":"James W.","family":"Beattie","sequence":"additional","affiliation":[{"name":"NanoPhotonics Centre, Cavendish Laboratory, Department of Physics University of Cambridge JJ Thompson Avenue Cambridge CB3 0US UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8234-723X","authenticated-orcid":false,"given":"Bart","family":"de Nijs","sequence":"additional","affiliation":[{"name":"Physics for Sustainable Chemistry Group, Department of Physics University of Cambridge JJ Thompson Avenue Cambridge CB3 0US UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9606-9488","authenticated-orcid":false,"given":"Jeremy J.","family":"Baumberg","sequence":"additional","affiliation":[{"name":"NanoPhotonics Centre, Cavendish Laboratory, Department of Physics University of Cambridge JJ Thompson Avenue Cambridge CB3 0US UK"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,10,25]]},"reference":[{"key":"e_1_2_9_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.9b04224"},{"key":"e_1_2_9_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.mcat.2019.110734"},{"key":"e_1_2_9_3_1","doi-asserted-by":"publisher","DOI":"10.1155\/2009\/620720"},{"key":"e_1_2_9_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.0c01069"},{"key":"e_1_2_9_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr040369x"},{"key":"e_1_2_9_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpcc.1c09801"},{"key":"e_1_2_9_7_1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0040739"},{"key":"e_1_2_9_8_1","doi-asserted-by":"publisher","DOI":"10.1039\/b919266b"},{"key":"e_1_2_9_9_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0022-0728(81)80086-1"},{"key":"e_1_2_9_10_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-022-05036-x"},{"key":"e_1_2_9_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/jp109599q"},{"key":"e_1_2_9_12_1","doi-asserted-by":"crossref","unstructured":"M. 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