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A comparable performance for proteins in immunoassays has yet to be fully assessed. Surface\u2010plasmon\u2010resonance (SPR) serves as a probe capable of performing assays at concentrations typically around 10\u207b\u2079 molar. In this study, plasmonic single\u2010molecule assays for both proteins and DNA are demonstrated, achieving limits\u2010of\u2010detections (LODs) as low as 10\u207b\n                    <jats:sup>2<\/jats:sup>\n                    \u2070 molar (1\u00a0\u00b1\u00a01 molecule in 0.1\u00a0mL), even in human serum, in 1 h. This represents an improvement in typical SPR LODs by eleven orders\u2010of\u2010magnitude. The single\u2010molecule SPR assay is achieved with a millimeter\u2010wide surface functionalized with a physisorbed biolayer comprising trillions of recognition\u2010elements (antibodies or protein\u2013probe complexes) which undergo an acidic or alkaline pH\u2010conditioning. Potentiometric and surface\u2010probing imaging experiments reveal the phenomenon underlying this extraordinary performance enhancement. The data suggest an unexplored amplification process within the biomaterial, where pH\u2010conditioning, driving the biolayer in a metastable state, induces a self\u2010propagating aggregation of partially misfolded proteins, following single\u2010affinity binding. This process triggers an electrostatic rearrangement, resulting in the displacement of a charge equivalent to 1.5e per 10\n                    <jats:sup>2<\/jats:sup>\n                    recognition elements. Such findings open new opportunities for reliable SPR\u2010based biosensing at the physical detection limits, with promising applications in point\u2010of\u2010care plasmonic systems.\n                  <\/jats:p>","DOI":"10.1002\/adma.202418610","type":"journal-article","created":{"date-parts":[[2025,1,23]],"date-time":"2025-01-23T06:24:25Z","timestamp":1737613465000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Plasmonic Single\u2010Molecule Affinity Detection at 10\n                    <sup>\u221220<\/sup>\n                    Molar"],"prefix":"10.1002","volume":"37","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1534-7336","authenticated-orcid":false,"given":"Eleonora","family":"Macchia","sequence":"first","affiliation":[{"name":"Dipartimento di Farmacia\u2010Scienze del Farmaco Universit\u00e0 degli Studi di Bari Aldo Moro  Bari 70125 Italy"},{"name":"Centre for Colloid and Surface Science Dipartimento 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