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Addressing this challenge is crucial for the development of nonlinear nanophotonics. Here, we show that atomically thin, epitaxially grown crystalline silver films circumvent these restrictions through the interplay of vertical electronic quantum confinement and lateral plasmonic enhancement. We fabricate atomically thin films that exhibit an enhanced nonlinear response associated with electronic quantum wells, and subsequently pattern them into periodic nanoribbon and nanotriangle arrays sustaining infrared localized surface plasmon resonances. Strong near\u2010field confinement in these structures further boosts second\u2010harmonic generation compared to unpatterned films. Precise control over nanostructure geometry enables spectral tuning of the plasmonic resonance, and consequently, the enhanced harmonic frequency. Our findings establish an approach for activating robust second\u2010order nonlinearities in quantum\u2010confined metals, where intrinsic size effects and plasmonic resonances act synergistically. The compatibility of high\u2010quality epitaxial growth with microchip fabrication technology offers a scalable route toward ultracompact nonlinear optical components for on\u2010chip frequency conversion, sensing, and quantum photonic\u00a0applications.<\/jats:p>","DOI":"10.1002\/adma.75217","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T11:23:18Z","timestamp":1790853798000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Plasmon\u2010Enhanced\u00a0Second\u2010Harmonic Generation in Atomically Thin Crystalline Silver Nanostructures"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-8760-8427","authenticated-orcid":false,"given":"Saad","family":"Abdullah","sequence":"first","affiliation":[{"name":"ICFO\u2010Institut de Ciencies Fotoniques The Barcelona Institute of Science and Technology  Castelldefels (Barcelona) Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2314-8951","authenticated-orcid":false,"given":"Philipp K.","family":"Jenke","sequence":"additional","affiliation":[{"name":"Vienna Center for Quantum Science and Technology (VCQ) Faculty of Physics University of Vienna  Vienna Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7636-2572","authenticated-orcid":false,"given":"Andrew P.","family":"Weber","sequence":"additional","affiliation":[{"name":"ICFO\u2010Institut de Ciencies Fotoniques The Barcelona Institute of Science and Technology  Castelldefels (Barcelona) Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4634-985X","authenticated-orcid":false,"given":"\u00c1lvaro","family":"Rodr\u00edguez Echarri","sequence":"additional","affiliation":[{"name":"ICFO\u2010Institut de Ciencies Fotoniques The Barcelona Institute of Science and Technology  Castelldefels (Barcelona) Spain"},{"name":"Center for Nanophotonics NWO Institute AMOLF  XG Amsterdam The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3138-8488","authenticated-orcid":false,"given":"Vahagn","family":"Mkhitaryan","sequence":"additional","affiliation":[{"name":"ICFO\u2010Institut de Ciencies Fotoniques The Barcelona Institute of Science and Technology  Castelldefels (Barcelona) Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1786-3235","authenticated-orcid":false,"given":"Fadil","family":"Iyikanat","sequence":"additional","affiliation":[{"name":"ICFO\u2010Institut de Ciencies Fotoniques The Barcelona Institute of Science and Technology  Castelldefels (Barcelona) Spain"},{"name":"Department of Physics Dokuz Eyl\u00fcl University  Izmir Turkey"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1727-3542","authenticated-orcid":false,"given":"Frederik","family":"Schiller","sequence":"additional","affiliation":[{"name":"Centro de F\u00edsica de Materiales CSIC\u2010UPV\/EHU and Materials Physics Center  San Sebastian Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4964-817X","authenticated-orcid":false,"given":"Philip","family":"Walther","sequence":"additional","affiliation":[{"name":"Vienna Center for Quantum Science and Technology (VCQ) Faculty of Physics University of Vienna  Vienna Austria"},{"name":"Research Platform for Testing the Quantum and Gravity Interface (TURIS) University of Vienna  Vienna Austria"},{"name":"Christian Doppler Laboratory for Photonic Quantum Computer Faculty of Physics University of Vienna  Vienna Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6643-806X","authenticated-orcid":false,"given":"J. 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