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Nanophotonics addresses this challenge by tailoring the size and morphology of nanostructures to manipulate the optical near field, thus modulating the nonlinear response. Here, we explore a complementary strategy based on engineering the electronic band structure in the mesoscopic regime to enhance optical nonlinearities. Specifically, we demonstrate an increase in second-harmonic generation (SHG) from crystalline silver films as their thickness is reduced down to just a few atomic monolayers. Operating at the boundary between bulk and two-dimensional systems, these ultra-thin films exhibit a pronounced enhancement of SHG with decreasing thickness. This enhancement stems from quantum confinement effects that modify the interaction between electronic states and incident light, which we explain based on quantum-mechanical calculation. Our atomically-thin crystalline silver films provide a new means to overcome the small interaction volumes inherent to nanophotonic platforms, enabling efficient nanoscale nonlinear optics with potential applications in photonics, sensing, and quantum technologies.<\/jats:p>","DOI":"10.1038\/s41467-026-74804-4","type":"journal-article","created":{"date-parts":[[2026,7,1]],"date-time":"2026-07-01T19:43:21Z","timestamp":1782935001000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Few-atom-thick silver films for enhanced nanoscale nonlinear optics"],"prefix":"10.1038","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2314-8951","authenticated-orcid":false,"given":"Philipp K.","family":"Jenke","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Saad","family":"Abdullah","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7636-2572","authenticated-orcid":false,"given":"Andrew P.","family":"Weber","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"\u00c1lvaro","family":"Rodr\u00edguez Echarri","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1786-3235","authenticated-orcid":false,"given":"Fadil","family":"Iyikanat","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3138-8488","authenticated-orcid":false,"given":"Vahagn","family":"Mkhitaryan","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1727-3542","authenticated-orcid":false,"given":"Frederik","family":"Schiller","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6643-806X","authenticated-orcid":false,"given":"J. 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