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Unlike catalysis, where surface reactivity dominates, SEs require simultaneous optimization of bulk ion transport, defect chemistry, mechanical integrity, and interfacial stability. Here, we outline a framework for autonomous SE discovery enabled by large artificial intelligence (AI) models, including machine learning interatomic potentials (MLIPs) and large language models (LLMs). We discuss the evolution from static materials databases to dynamic, self\u2010updating knowledge systems, the role of MLIPs in bridging density functional theory (DFT) and long\u2010timescale ion migration, and the emergence of LLMs as engines for literature mining, hypothesis generation, and scientific reasoning. We further describe a closed\u2010loop architecture integrating AI\u2010driven candidate design, multiscale simulation, uncertainty\u2010aware selection, and experimental validation. Such systems shift SE research from intuition\u2010guided exploration to data\u2010informed, self\u2010improving cycles. We conclude by highlighting challenges in data standardization, interfacial complexity, and reproducibility, and we propose design principles for building autonomous laboratories for solid\u2010state battery materials.<\/jats:p>","DOI":"10.1002\/adma.75354","type":"journal-article","created":{"date-parts":[[2026,10,13]],"date-time":"2026-10-13T08:43:04Z","timestamp":1791880984000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Breaking Bottlenecks in Solid Electrolyte Discovery With Large Artificial Intelligence Models"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0904-802X","authenticated-orcid":false,"given":"Eric Jianfeng","family":"Cheng","sequence":"first","affiliation":[{"name":"Advanced Institute for Materials Research (WPI\u2010AIMR) Tohoku University  Sendai Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6972-394X","authenticated-orcid":false,"given":"Min","family":"Hong","sequence":"additional","affiliation":[{"name":"Advanced Institute for Materials Research (WPI\u2010AIMR) Tohoku University  Sendai Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiquan","family":"Zeng","sequence":"additional","affiliation":[{"name":"Department of Chemistry National University of Singapore  Singapore Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuanyu","family":"Liu","sequence":"additional","affiliation":[{"name":"Department of Materials Design and Innovation University At Buffalo  Buffalo New York USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4935-7508","authenticated-orcid":false,"given":"Qian","family":"Wang","sequence":"additional","affiliation":[{"name":"Advanced Institute for Materials Research (WPI\u2010AIMR) Tohoku University  Sendai Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Melissa Jane","family":"Meadowcroft","sequence":"additional","affiliation":[{"name":"London School of Economics  London UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7956-345X","authenticated-orcid":false,"given":"Vlad","family":"Badilita","sequence":"additional","affiliation":[{"name":"Institute of Microstructure Technology Karlsruhe Institute of Technology  Eggenstein\u2010 Leopoldshafen Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9266-3669","authenticated-orcid":false,"given":"Carlos Miguel","family":"Costa","sequence":"additional","affiliation":[{"name":"Physics Centre of Minho and Porto Universities (CF\u2010UM\u2010UP) University of Minho  Braga Portugal"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6791-7620","authenticated-orcid":false,"given":"Senentxu","family":"Lanceros\u2010M\u00e9ndez","sequence":"additional","affiliation":[{"name":"Basque Center for Materials, Applications and Nanostructures UPV\/EHU Science Park  Leioa Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ying","family":"Li","sequence":"additional","affiliation":[{"name":"Advanced Institute for Materials Research (WPI\u2010AIMR) Tohoku University  Sendai Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-5142-3815","authenticated-orcid":false,"given":"Chenyao","family":"Ma","sequence":"additional","affiliation":[{"name":"Suzhou MatSource Technology Co., Ltd.  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