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Here, we establish interfacial defect templating as a general materials\u2010design strategy for phase engineering in confined two\u2010dimensional metals, using monolayer silver as a model system. By tailoring the defect chemistry of a graphene overlayer, we selectively stabilize two competing crystalline phases of two\u2010dimensional Ag at the graphene\/SiC interface: a near\u2010commensurate phase promoted by vacancy and line defects in epitaxial graphene, and a denser phase favored beneath intrinsically sp\n                    <jats:sup>3<\/jats:sup>\n                    \u2010rich zero\u2010layer graphene. Multimodal characterization reveals distinct lattice registries, electronic structures, and charge transfer to the graphene overlayer for each phase. First\u2010principles calculations show that phase selectivity arises from a competition between kinetically favored nucleation pathways and thermodynamically preferred packing configurations, explaining both controlled phase formation and long\u2010term evolution. The defect\u2010programmed Ag phases exhibit strongly contrasting linear and nonlinear optical responses, enabling phase\u2010tunable optical functionality at atomic thickness. More broadly, this work reframes defects as deliberate design elements for programming structure\u2013property relationships in confined two\u2010dimensional metals.\n                  <\/jats:p>","DOI":"10.1002\/adma.74689","type":"journal-article","created":{"date-parts":[[2026,8,20]],"date-time":"2026-08-20T06:42:25Z","timestamp":1787208145000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Defect\u2010Templated Phase Engineering in Atomically Thin Metals"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9370-7942","authenticated-orcid":false,"given":"Arpit","family":"Jain","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering The Pennsylvania State University  University Park Pennsylvania USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Boyang","family":"Zheng","sequence":"additional","affiliation":[{"name":"Department of Physics The Pennsylvania State University  University Park Pennsylvania USA"},{"name":"2\u2010Dimensional Crystal Consortium The Pennsylvania State University  University Park Pennsylvania USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-7669-0186","authenticated-orcid":false,"given":"Sawani","family":"Datta","sequence":"additional","affiliation":[{"name":"Max\u2010Planck\u2010Institut F\u00fcr Festk\u00f6rperforschung  Stuttgart Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kanchan","family":"Ulman","sequence":"additional","affiliation":[{"name":"Department of Physics National University of Singapore  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jakob","family":"Henz","sequence":"additional","affiliation":[{"name":"Institute of Physics and Center for Soft Nanoscience (SoN) University of M\u00fcnster  M\u00fcnster Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-9342-8447","authenticated-orcid":false,"given":"Matthew Wei\u2010Jun","family":"Liu","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering The Pennsylvania State University  University Park Pennsylvania USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1416-2575","authenticated-orcid":false,"given":"Van Dong","family":"Pham","sequence":"additional","affiliation":[{"name":"Paul\u2010Drude\u2010Institut F\u00fcr Festk\u00f6rperelektronik Leibniz\u2010Institut Im Forschungsverbund Berlin e. 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