{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,8,26]],"date-time":"2026-08-26T17:23:40Z","timestamp":1787765020108,"version":"build-2784847793"},"reference-count":34,"publisher":"Oxford University Press (OUP)","issue":"4","license":[{"start":{"date-parts":[[2026,7,1]],"date-time":"2026-07-01T00:00:00Z","timestamp":1782864000000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/academic.oup.com\/pages\/standard-publication-reuse-rights"}],"funder":[{"DOI":"10.13039\/100000015","name":"U.S. DOE","doi-asserted-by":"publisher","id":[{"id":"10.13039\/100000015","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100006132","name":"Office of Science","doi-asserted-by":"publisher","id":[{"id":"10.13039\/100006132","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100031156","name":"Materials Sciences and Engineering Division","doi-asserted-by":"publisher","id":[{"id":"10.13039\/100031156","id-type":"DOI","asserted-by":"publisher"}]},{"name":"Center for Nanophase Materials Sciences"},{"DOI":"10.13039\/100006151","name":"Office of Basic Energy Sciences","doi-asserted-by":"publisher","id":[{"id":"10.13039\/100006151","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100017535","name":"Energy Frontier Research Centers program","doi-asserted-by":"publisher","id":[{"id":"10.13039\/100017535","id-type":"DOI","asserted-by":"publisher"}]},{"name":"Center for the Science of Synthesis Across Scales"}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,7,1]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Realizing high-throughput aberration-corrected Scanning Transmission Electron Microscopy (STEM) exploration of atomic structures requires rapid tuning of multipole probe correctors while compensating for the inevitable drift of the optical column. While automated alignment routines exist, conventional approaches rely on serial, gradient-free searches (e.g., Nelder-Mead) that are sample-inefficient and struggle to correct multiple interacting parameters simultaneously. Conversely, emerging deep learning methods offer speed but often lack the flexibility to adapt to varying sample conditions without extensive retraining. Here, we introduce a Multi-Objective Bayesian Optimization (MOBO) framework for rapid, data-efficient aberration correction. Importantly, this framework does not prescribe a single notion of image quality; instead, it enables user-defined, physically motivated reward formulations (e.g., symmetry-induced objectives) and uses Pareto fronts to expose the resulting tradeoffs between competing experimental priorities. We use Gaussian Process regression to build a probabilistic surrogate of the aberration-dependent image-quality landscape, and employ a multi-objective acquisition strategy to select aberration settings that improve the estimated Pareto front across competing physics-informed rewards. We demonstrate that this active learning loop is more robust than traditional optimization algorithms and effectively tunes focus, astigmatism, and higher-order aberrations. By balancing competing objectives, this approach enables \u201cself-optimizing\u201d microscopy by dynamically sustaining optimal performance during experiments.<\/jats:p>","DOI":"10.1093\/mam\/ozag071","type":"journal-article","created":{"date-parts":[[2026,6,30]],"date-time":"2026-06-30T23:15:49Z","timestamp":1782861349000},"source":"Crossref","is-referenced-by-count":0,"title":["Towards Self-Optimizing Electron Microscope: Robust Tuning of Aberration Coefficients via Physics-Aware Multi-Objective Bayesian Optimization"],"prefix":"10.1093","volume":"32","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-7249-103X","authenticated-orcid":false,"given":"Utkarsh","family":"Pratiush","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering, The University of Tennessee , 414 Ferris Hall, 1508 Middle Drive, Knoxville, TN 37996-2100 ,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-8777-4686","authenticated-orcid":false,"given":"Austin","family":"Houston","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, The University of Tennessee , 414 Ferris Hall, 1508 Middle Drive, Knoxville, TN 37996-2100 ,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Richard","family":"Liu","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, The University of Tennessee , 414 Ferris Hall, 1508 Middle Drive, Knoxville, TN 37996-2100 ,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gerd","family":"Duscher","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, The University of Tennessee , 414 Ferris Hall, 1508 Middle Drive, Knoxville, TN 37996-2100 ,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sergei","family":"Kalinin","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering, The University of Tennessee , 414 Ferris Hall, 1508 Middle Drive, Knoxville, TN 37996-2100 ,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"286","published-online":{"date-parts":[[2026,8,26]]},"reference":[{"key":"2026082612564375500_ozag071-B1","doi-asserted-by":"publisher","first-page":"113663","DOI":"10.1016\/j.ultramic.2022.113663","article-title":"Near-real-time diagnosis of electron optical phase aberrations in scanning transmission electron microscopy using an artificial neural network","volume":"245","author":"Bertoni","year":"2023","journal-title":"Ultramicroscopy"},{"key":"2026082612564375500_ozag071-B2","doi-asserted-by":"publisher","first-page":"247","DOI":"10.1111\/j.1365-2818.1974.tb03937.x","article-title":"Scanning transmission electron microscopy*","volume":"100","author":"Crewe","year":"1974","journal-title":"J Microsc"},{"key":"2026082612564375500_ozag071-B3","doi-asserted-by":"crossref","DOI":"10.1007\/978-1-4419-9583-4","volume-title":"Electron Energy-Loss Spectroscopy in the Electron Microscope","author":"Egerton","year":"2011","edition":"Third edition"},{"key":"2026082612564375500_ozag071-B4","doi-asserted-by":"publisher","first-page":"185","DOI":"10.1111\/j.1365-2818.1982.tb00412.x","article-title":"An automatic focusing and astigmatism correction system for the SEM and CTEM","volume":"127","author":"Erasmus","year":"1982","journal-title":"J Microsc"},{"key":"2026082612564375500_ozag071-B5","doi-asserted-by":"crossref","DOI":"10.1142\/p960","volume-title":"Aberration-Corrected Imaging in Transmission Electron Microscopy","author":"Erni","year":"2015","edition":"2nd ed"},{"key":"2026082612564375500_ozag071-B6","author":"Houston","year":"2025"},{"key":"2026082612564375500_ozag071-B7","doi-asserted-by":"publisher","first-page":"113215","DOI":"10.1016\/j.ultramic.2021.113215","article-title":"Automated geometric aberration correction for large\u2013angle illumination STEM","volume":"222","author":"Ishikawa","year":"2021","journal-title":"Ultramicroscopy"},{"key":"2026082612564375500_ozag071-B8","doi-asserted-by":"publisher","first-page":"11","DOI":"10.1038\/s43586-022-00095-w","article-title":"Machine learning in scanning transmission electron microscopy","volume":"2","author":"Kalinin","year":"2022","journal-title":"Nat Rev Methods Primers"},{"key":"2026082612564375500_ozag071-B9","doi-asserted-by":"publisher","first-page":"12604","DOI":"10.1021\/acsnano.1c02104","article-title":"Automated and autonomous experiments in electron and scanning probe microscopy","volume":"15","author":"Kalinin","year":"2021","journal-title":"ACS Nano"},{"key":"2026082612564375500_ozag071-B10","doi-asserted-by":"publisher","first-page":"931","DOI":"10.1557\/s43577-022-00413-3","article-title":"Deep learning for electron and scanning probe microscopy: From materials design to atomic fabrication","volume":"47","author":"Kalinin","year":"2022","journal-title":"MRS Bulletin"},{"key":"2026082612564375500_ozag071-B11","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1107\/S205327331501757X","article-title":"Computation in electron microscopy","volume":"72","author":"Kirkland","year":"2016","journal-title":"Acta Crystallogr A Found Adv"},{"key":"2026082612564375500_ozag071-B12","doi-asserted-by":"publisher","first-page":"62","DOI":"10.1016\/j.ultramic.2017.12.002","article-title":"Fine tuning an aberration corrected ADF-STEM","volume":"186","author":"Kirkland","year":"2018","journal-title":"Ultramicroscopy"},{"key":"2026082612564375500_ozag071-B13","doi-asserted-by":"publisher","first-page":"571","DOI":"10.1038\/nature08879","article-title":"Atom-by-atom structural and chemical analysis by annular dark-field electron microscopy","volume":"464","author":"Krivanek","year":"2010","journal-title":"Nature"},{"key":"2026082612564375500_ozag071-B14","doi-asserted-by":"publisher","first-page":"19659","DOI":"10.1021\/acsnano.4c18760","article-title":"Machine learning-based reward-driven tuning of scanning probe microscopy: Toward fully automated microscopy","volume":"19","author":"Liu","year":"2025","journal-title":"ACS Nano"},{"key":"2026082612564375500_ozag071-B15","doi-asserted-by":"publisher","DOI":"10.1016\/j.ultramic.2025.114138","article-title":"Emittance minimization for aberration correction II: Physics-informed Bayesian optimization of an electron microscope","volume":"273","author":"Ma","year":"2025","journal-title":"Ultramicroscopy"},{"key":"2026082612564375500_ozag071-B16","doi-asserted-by":"publisher","DOI":"10.1016\/j.ultramic.2025.114137","article-title":"Emittance minimization for aberration correction I: Aberration correction of an electron microscope without knowing the aberration coefficients","volume":"273","author":"Ma","year":"2025","journal-title":"Ultramicroscopy"},{"key":"2026082612564375500_ozag071-B17","doi-asserted-by":"publisher","first-page":"24","DOI":"10.12688\/openreseurope.13015.1","article-title":"The abTEM code: Transmission electron microscopy from first principles","volume":"1","author":"Madsen","year":"2021","journal-title":"Open Res Eur"},{"key":"2026082612564375500_ozag071-B18","doi-asserted-by":"publisher","first-page":"345","DOI":"10.1016\/j.ultramic.2006.09.003","article-title":"Separation of bulk and surface-losses in low-loss EELS measurements in STEM","volume":"107","author":"Mkhoyan","year":"2007","journal-title":"Ultramicroscopy"},{"key":"2026082612564375500_ozag071-B19","doi-asserted-by":"publisher","first-page":"263","DOI":"10.1038\/nmat2380","article-title":"Structure and bonding at the atomic scale by scanning transmission electron microscopy","volume":"8","author":"Muller","year":"2009","journal-title":"Nat Mater"},{"key":"2026082612564375500_ozag071-B20","doi-asserted-by":"publisher","first-page":"052003","DOI":"10.1088\/1361-6501\/abd96d","article-title":"Electron microscopy in semiconductor inspection","volume":"32","author":"Nakamae","year":"2021","journal-title":"Meas Sci Technol"},{"key":"2026082612564375500_ozag071-B21","doi-asserted-by":"publisher","DOI":"10.1016\/j.micron.2021.103032","article-title":"STEM-EELS investigation of c-Si\/a-AlO interface for solar cell applications","volume":"145","author":"Noircler","year":"2021","journal-title":"Micron"},{"key":"2026082612564375500_ozag071-B22","doi-asserted-by":"publisher","first-page":"274","DOI":"10.1038\/s41524-025-01766-4","article-title":"BEACON\u2014Automated aberration correction for scanning transmission electron microscopy using Bayesian optimization","volume":"11","author":"Pattison","year":"2025","journal-title":"NPJ Comput Mater"},{"key":"2026082612564375500_ozag071-B23","doi-asserted-by":"crossref","DOI":"10.1007\/978-1-4419-7200-2","volume-title":"Scanning Transmission Electron Microscopy","author":"Pennycook","year":"2011"},{"key":"2026082612564375500_ozag071-B24","author":"Pratiush","year":"2025"},{"key":"2026082612564375500_ozag071-B25","doi-asserted-by":"publisher","first-page":"103701","DOI":"10.1063\/5.0225401","article-title":"Realizing smart scanning transmission electron microscopy using high performance computing","volume":"95","author":"Pratiush","year":"2024","journal-title":"Rev Sci Instrum"},{"key":"2026082612564375500_ozag071-B26","author":"Pratiush","year":"2026"},{"key":"2026082612564375500_ozag071-B27","doi-asserted-by":"publisher","author":"Pratiush","year":"2026","DOI":"10.31224\/4645"},{"key":"2026082612564375500_ozag071-B28","doi-asserted-by":"publisher","DOI":"10.1093\/mam\/ozaf048.1066","article-title":"STEM orchestrator: Managing multi-hardware-component STEM automation seamlessly","volume":"31","author":"Pratiush","year":"2025","journal-title":"Microsc Microanal"},{"key":"2026082612564375500_ozag071-B29","doi-asserted-by":"publisher","DOI":"10.1016\/j.isci.2023.107072","article-title":"Recent advances in in-situ transmission electron microscopy techniques for heterogeneous catalysis","volume":"26","author":"Qu","year":"2023","journal-title":"iScience"},{"key":"2026082612564375500_ozag071-B30","doi-asserted-by":"publisher","first-page":"361","DOI":"10.1007\/BF01246212","article-title":"EELS nanoanalysis for investigating both chemical composition and bonding of interlayers in composites","volume":"125","author":"Schneider","year":"1997","journal-title":"Mikrochim Acta"},{"key":"2026082612564375500_ozag071-B31","doi-asserted-by":"publisher","first-page":"948","DOI":"10.1038\/s41467-024-45042-3","article-title":"DeepFocus: Fast focus and astigmatism correction for electron microscopy","volume":"15","author":"Schubert","year":"2024","journal-title":"Nat Commun"},{"key":"2026082612564375500_ozag071-B32","doi-asserted-by":"crossref","first-page":"3","DOI":"10.1007\/978-1-4757-2519-3_1","volume-title":"Transmission Electron Microscopy","author":"Williams","year":"1996"},{"key":"2026082612564375500_ozag071-B33","doi-asserted-by":"crossref","DOI":"10.1007\/978-0-387-76501-3","volume-title":"Transmission Electron Microscopy: A Textbook for Materials Science","author":"Williams","year":"2009","edition":"2nd ed"},{"key":"2026082612564375500_ozag071-B34","doi-asserted-by":"publisher","first-page":"5186","DOI":"10.1039\/D1QM00275A","article-title":"(S)TEM-EELS as an advanced characterization technique for lithium-ion batteries","volume":"5","author":"Yu","year":"2021","journal-title":"Mater Chem Front"}],"container-title":["Microscopy and Microanalysis"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/academic.oup.com\/mam\/article-pdf\/32\/4\/ozag071\/70806863\/ozag071.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/academic.oup.com\/mam\/article-pdf\/32\/4\/ozag071\/70806863\/ozag071.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,8,26]],"date-time":"2026-08-26T16:56:50Z","timestamp":1787763410000},"score":1,"resource":{"primary":{"URL":"https:\/\/academic.oup.com\/mam\/article\/doi\/10.1093\/mam\/ozag071\/8771271"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,7,1]]},"references-count":34,"journal-issue":{"issue":"4","published-print":{"date-parts":[[2026,7,1]]}},"URL":"https:\/\/doi.org\/10.1093\/mam\/ozag071","relation":{},"ISSN":["1431-9276","1435-8115"],"issn-type":[{"value":"1431-9276","type":"print"},{"value":"1435-8115","type":"electronic"}],"subject":[],"published-other":{"date-parts":[[2026,8]]},"published":{"date-parts":[[2026,7,1]]},"article-number":"ozag071"}}