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Herein, we report a rapid, artificial intelligence (AI)-accelerated surface-enhanced Raman scattering (SERS) platform for the simultaneous mapping of caspase-3 and matrix metalloproteinase-2 (MMP-2) activities at epileptic foci. To overcome the kinetic mismatch that traditionally stalls dual-enzyme tracking, we employed an AI-driven workflow to identify an MMP-2 peptide substrate whose catalytic kinetics are synchronized with those of its caspase-3 counterpart, compressing measurement times from hours to minutes. A bespoke dual-branch cross-attention Kolmogorov\u2013Arnold Network (DBC-KAN) further accelerated the diagnostic speed by capturing subtle early-stage spectral evolution patterns through learnable edge activations, achieving 98.21% predictive accuracy within 4 min of sample loading, a &amp;gt;7-fold improvement relative to commercial activity assays (30\u201360 min). Notably, these substrates were integrated into a ratiometric SERS array featuring biological-silent-region internal standards, enhancing quantitative robustness while eliminating spectral cross-talk. Leveraging this platform, we established a logic-gated diagnostic framework (caspase-3\/MMP-2 ratio) that successfully discriminated epileptic foci from healthy and inflamed regions in transgenic murine models and resected human cortical tissues. This AI-driven SERS strategy delivers ultrafast intraoperative molecular profiling, providing a high-fidelity roadmap for precision neurosurgery.<\/jats:p>","DOI":"10.1021\/jacs.6c09984","type":"journal-article","created":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T12:01:46Z","timestamp":1786968106000},"page":"43089-43102","source":"Crossref","is-referenced-by-count":0,"title":["AI-Assisted SERS Decoding\nof Dual Enzymatic Activity\nfor Intraoperative Chemical Mapping of Epilepsy"],"prefix":"10.1021","volume":"148","author":[{"given":"Jing","family":"Zhao","sequence":"first","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 201203"]},{"name":"The First Affiliated Hospital of Kunming Medical University , , , ,","place":["Kunming, Yunnan, China, 650032"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhihang","family":"Chen","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zihao","family":"Wei","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming","family":"Chen","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200040"]},{"name":"Fudan University , , ,","place":["Shanghai, China, 200040"]},{"name":"Fudan University , , ,","place":["Shanghai, China, 200040"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuncan","family":"Chen","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200040"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinge","family":"Liang","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Caixia","family":"Liu","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0485-0259","authenticated-orcid":true,"given":"Renxiao","family":"Wang","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiang","family":"Zou","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200040"]},{"name":"Fudan University , , ,","place":["Shanghai, China, 200040"]},{"name":"Fudan University , , ,","place":["Shanghai, China, 200040"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinhua","family":"Yu","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2853-7910","authenticated-orcid":true,"given":"Yifei","family":"Qi","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cong","family":"Wang","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7731-8031","authenticated-orcid":true,"given":"Cong","family":"Li","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,17]]},"reference":[{"issue":"1","key":"2026101611062657000_cit1","doi-asserted-by":"publisher","first-page":"123","DOI":"10.1038\/s42003-025-09402-z","article-title":"Ventral subicular pyramidal neurons contribute to epileptogenesis\nvia anterior thalamic circuit","volume":"9","author":"Gong","year":"2026","journal-title":"Commun. 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Ther."},{"issue":"1","key":"2026101611062657000_cit4","doi-asserted-by":"publisher","first-page":"19567","DOI":"10.1038\/s41598-020-76283-z","article-title":"Radiomics\nfeatures of hippocampal regions in magnetic resonance imaging\ncan differentiate medial temporal lobe epilepsy patients from healthy\ncontrols","volume":"10","author":"Park","year":"2020","journal-title":"Sci. Rep."},{"issue":"1","key":"2026101611062657000_cit5","doi-asserted-by":"publisher","first-page":"36","DOI":"10.1159\/000085025","article-title":"The application\nof optical recording of intrinsic signals to simultaneously acquire\nfunctional, pathological and localizing information and its potential\nrole in neurosurgery","volume":"83","author":"Schwartz","year":"2005","journal-title":"Stereotact. Funct. Neurosurg."},{"issue":"3","key":"2026101611062657000_cit6","doi-asserted-by":"publisher","first-page":"217","DOI":"10.1212\/01.wnl.0000334365.22854.d3","article-title":"Incomplete\nresection of focal cortical dysplasia is the main predictor\nof poor postsurgical outcome","volume":"72","author":"Krsek","year":"2009","journal-title":"Neurology"},{"issue":"5","key":"2026101611062657000_cit7","doi-asserted-by":"publisher","first-page":"1092","DOI":"10.1111\/epi.16893","article-title":"Epilepsy surgery:\nLate seizure recurrence after initial complete seizure freedom","volume":"62","author":"Petrik","year":"2021","journal-title":"Epilepsia"},{"key":"2026101611062657000_cit8","doi-asserted-by":"publisher","first-page":"1616804","DOI":"10.3389\/fnmol.2025.1616804","article-title":"Silencing\nepileptic storms: targeting miRNA-lncRNA\ncrosstalk in astrocytes and microglia to disarm neuroinflammatory\ntriggers","volume":"18","author":"Meng","year":"2025","journal-title":"Front. Mol. 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Bioelectron."},{"key":"2026101611062657000_cit29","doi-asserted-by":"publisher","DOI":"10.1016\/j.bios.2022.114194","article-title":"In situ\nratiometric SERS imaging of intracellular protease\nactivity for subtype discrimination of human breast cancer","volume":"207","author":"Zhong","year":"2022","journal-title":"Biosens. Bioelectron."},{"key":"2026101611062657000_cit30","doi-asserted-by":"publisher","DOI":"10.1016\/j.bios.2021.112965","article-title":"Real-time in situ monitoring\nof Lon and Caspase-3 for assessing the\nstate of cardiomyocytes under hypoxic conditions via a novel Au\u2013Se\nfluorescent nanoprobe","volume":"176","author":"Zhan","year":"2021","journal-title":"Biosens. Bioelectron."},{"issue":"40","key":"2026101611062657000_cit31","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.1406134111","article-title":"Basis for substrate\nrecognition and distinction\nby matrix metalloproteinases","volume":"111","author":"Ratnikov","year":"2014","journal-title":"Proc. Natl. 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