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Here we show that Au\u2010coordinated Pt single atoms function as charge\u2010transfer bridges within a TiO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    nanocavity\/Au nanoparticle architecture, coupling molecular coordination to near\u2010resonant Raman enhancement. The Pt single atoms serve three interdependent roles: binding target molecules, modulating interfacial electronic states, and mediating charge transfer. Together with photonic confinement and plasmonic hotspots, this atomically defined pathway produces an apparent SERS enhancement factor of 3.6 \u00d7 10\n                    <jats:sup>11<\/jats:sup>\n                    and enables measurements within a statistically defined single\u2010molecule occupancy regime. We term this cooperative process Spatial\u2013Plasmonic Atomic Coupling Enhancement (SPACE), which connects atomic\u2010scale coordination and energy\u2010level alignment with macroscopic Raman amplification. As a proof of analytical utility, cysteamine functionalization couples benzaldehyde capture through Schiff\u2010base formation to the single\u2010atom\u2010mediated enhancement pathway, enabling gas\u2010phase detection down to 0.3 ppbv. These findings establish single\u2010atom coordination as a general design principle for transforming interfacial molecular binding into near\u2010resonant vibrational amplification.\n                  <\/jats:p>","DOI":"10.1002\/anie.4147834","type":"journal-article","created":{"date-parts":[[2026,9,23]],"date-time":"2026-09-23T06:00:08Z","timestamp":1790143208000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Single Atoms Couple Molecular Coordination to Near\u2010Resonant Charge Transfer in Surface\u2010Enhanced Raman Scattering"],"prefix":"10.1002","volume":"65","author":[{"given":"Dawei","family":"Xu","sequence":"first","affiliation":[{"name":"School of Chemistry and Molecular Engineering East China Normal University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xue","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Chemistry and Molecular 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