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Traditional approaches to fabricating small gaps have relied on localizing dielectric spacers between gold nanoparticles (AuNPs). However, doing so has encountered challenges in producing high-density, clean gaps across large surface areas. Here, we demonstrate a straightforward, self-assembly-guided method for the consistent fabrication of topologically anchored AuNPs featuring sub-5 nm nanogaps, arranged on a nanostructured block copolymer template. The solution-based method enables time-dependent tuning toward high plasmonic coupling density, resulting in an extensive number of hotspots, with an equivalent sensing enhancement factor (ESEF) exceeding that of thermally annealed gold nanoisland chips by 1 \u00d7 105. Laser excitation of these densely packed AuNPs at their plasmonic resonance efficiently drives both nucleic acid hybridization and amplification-based cyclic fluorescence probe cleavage, enabling SARS-CoV-2 viral sequence quantification down to the attomolar level. Our results demonstrate that a carefully engineered template nanostructure and the AuNP diameter integrate plasmonic hotspots, target adsorption, thermoplasmonic heating, and signal transduction within a single platform. This facile strategy for densely packed hotspots offers a potentially scalable avenue for ultrasensitive biomolecular assays.<\/jats:p>","DOI":"10.1021\/acsnanoscienceau.5c00190","type":"journal-article","created":{"date-parts":[[2026,4,14]],"date-time":"2026-04-14T23:37:39Z","timestamp":1776209859000},"page":"570-581","source":"Crossref","is-referenced-by-count":4,"title":["Mismatch-Tuned\nPlasmonic Nanogap Networks on Block\nCopolymers for Ultrasensitive Nucleic Acid Quantification"],"prefix":"10.1021","volume":"6","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0450-2406","authenticated-orcid":true,"given":"Yizhou","family":"Zhang","sequence":"first","affiliation":[{"name":"Tohoku University , , ,","place":["Sendai, Japan, 980-8577"]},{"name":"Shanghai University , , ,","place":["Shanghai, China, 200444"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ying","family":"Du","sequence":"additional","affiliation":[{"name":"University of Shanghai for Science and Technology , , ,","place":["Shanghai, China, 200093"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Martin","family":"Spillmann","sequence":"additional","affiliation":[{"name":"ETH Zu\u0308rich , , ,","place":["Zu\u0308rich, Switzerland, 8093"]},{"name":"Empa, Swiss Federal Laboratories for Materials Science and Technology , , ,","place":["Du\u0308bendorf, Switzerland, 8600"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kazuto","family":"Akagi","sequence":"additional","affiliation":[{"name":"Tohoku University , , ,","place":["Sendai, Japan, 980-8577"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiukai","family":"Tang","sequence":"additional","affiliation":[{"name":"ETH Zu\u0308rich , , ,","place":["Zu\u0308rich, Switzerland, 8093"]},{"name":"Empa, Swiss Federal Laboratories for Materials Science and Technology , , ,","place":["Du\u0308bendorf, Switzerland, 8600"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shivaprakash N.","family":"Ramakrishna","sequence":"additional","affiliation":[{"name":"ETH Zu\u0308rich , , ,","place":["Zu\u0308rich, Switzerland, 8093"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7873-1485","authenticated-orcid":true,"given":"Guangyu","family":"Qiu","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, P. R. China, 200240"]},{"name":"Shanghai Jiao Tong University , , ,","place":["Shanghai, P. R. China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2078-137X","authenticated-orcid":true,"given":"Jing","family":"Wang","sequence":"additional","affiliation":[{"name":"ETH Zu\u0308rich , , ,","place":["Zu\u0308rich, Switzerland, 8093"]},{"name":"Empa, Swiss Federal Laboratories for Materials Science and Technology , , ,","place":["Du\u0308bendorf, Switzerland, 8600"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,4,14]]},"reference":[{"key":"2026081909071880400_cit1","doi-asserted-by":"publisher","first-page":"8531","DOI":"10.1039\/D3CS00417A","article-title":"On-Site Airborne Pathogen Detection for Infection Risk Mitigation","volume":"52","author":"Qiu","year":"2023","journal-title":"Chem. Soc. 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