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Here, we report halogenated amorphous zeolitic imidazolate framework (a-ZIF) resists deposited entirely by a dry process, which exhibit a pronounced irradiation-source-dependent tone conversion. Smooth a-ZIF films were grown by chemical vapor deposition (CVD) using 4,5-diiodoimidazole (DI-Im) precursors. Partial in situ thermal decomposition of DI-Im produces a ternary linker mixture (DI-Im, 4-iodoimidazole, imidazole), promoting the growth of uniform, amorphous films. Under electron-beam (e-beam) exposure, the resist operates in a positive-tone mode with high sensitivity (D50 = 0.15 mC cm\u20132, comparable to commercial PMMA resists) and resolves 100 nm line-and-space and 80 nm contact-hole patterns. In contrast, EUV exposure yields high sensitivity in negative-tone development (D50 = 65 mJ cm\u20132) and exhibits a nonmonotonic dose\u2013thickness response in positive-tone development. We demonstrate positive-tone EUV patterning of 90 nm line-and-space features. X-ray photoelectron and near-edge X-ray absorption fine structure spectroscopy trace the tone conversion to distinct reaction pathways: high-energy primary electrons under e-beam exposure drive imidazole ring decomposition into soluble polar fragments, giving rise to the positive-tone response, whereas the low-energy electrons generated under EUV cleave C\u2013I bonds while retaining the ring, and the resulting poorly soluble recombination products account for both the negative-tone behavior and the nonmonotonic positive-tone response. Identifying the electron-energy regimes and reaction pathways responsible for each behavior provides a basis for engineering the resist response through linker design. These results illustrate that electron-beam exposure cannot serve as a universal chemical proxy for EUV lithography.<\/jats:p>","DOI":"10.1021\/acsami.6c16414","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T11:01:35Z","timestamp":1791370895000},"page":"56532-56547","source":"Crossref","is-referenced-by-count":0,"title":["Irradiation-Source-Dependent Tone Conversion in Dry-Deposited Halogenated Amorphous Zeolitic Imidazolate Framework Resistsfor Electron-Beam and Extreme Ultraviolet Lithography"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9715-8861","authenticated-orcid":true,"given":"Jinhwan","family":"Byeon","sequence":"first","affiliation":[{"name":"KU Leuven\u2013University of Leuven , , Celestijnenlaan 200F , ,","place":["Leuven, Belgium, 3001"]},{"name":"Kunsan National University , , 558 Daehak-ro , , ,","place":["Gunsan-si, Jeonbuk State, Republic of Korea, 54150"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nick","family":"Gys","sequence":"additional","affiliation":[{"name":"KU Leuven\u2013University of Leuven , , Celestijnenlaan 200F , ,","place":["Leuven, Belgium, 3001"]},{"name":"Vrije Universiteit Brussel , , ,","place":["Brussels, Belgium, 1050"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4719-7368","authenticated-orcid":true,"given":"Jorid","family":"Smets","sequence":"additional","affiliation":[{"name":"KU Leuven\u2013University of Leuven , , Celestijnenlaan 200F , ,","place":["Leuven, Belgium, 3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ali","family":"Azimi","sequence":"additional","affiliation":[{"name":"KU Leuven\u2013University of Leuven , , Celestijnenlaan 200F , ,","place":["Leuven, Belgium, 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3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kevin M.","family":"Dorney","sequence":"additional","affiliation":[{"name":"IMEC , Kapeldreef 75 , ,","place":["Leuven, Belgium, 3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1334-4788","authenticated-orcid":true,"given":"Jes\u00fas","family":"G\u00e1ndara-Loe","sequence":"additional","affiliation":[{"name":"KU Leuven\u2013University of Leuven , , Celestijnenlaan 200F , ,","place":["Leuven, Belgium, 3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juhyung","family":"Park","sequence":"additional","affiliation":[{"name":"KU Leuven\u2013University of Leuven , , Kasteelpark Arenberg 44 , ,","place":["Leuven, Belgium, 3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Min Jong","family":"Jeong","sequence":"additional","affiliation":[{"name":"Gwangju Institute of Science and Technology , , 123 Cheomdangwagi-ro , , ,","place":["Buk-gu, Gwangju, Republic of Korea, 61005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-4291-4556","authenticated-orcid":true,"given":"Sangjin","family":"Kim","sequence":"additional","affiliation":[{"name":"Gwangju Institute of Science and Technology , , 123 Cheomdangwagi-ro , , ,","place":["Buk-gu, Gwangju, Republic of Korea, 61005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2078-9630","authenticated-orcid":true,"given":"Sukwon","family":"Hong","sequence":"additional","affiliation":[{"name":"Gwangju Institute of Science and Technology , , 123 Cheomdangwagi-ro , , ,","place":["Buk-gu, Gwangju, Republic of Korea, 61005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9661-0932","authenticated-orcid":true,"given":"Tomasz","family":"Sobol","sequence":"additional","affiliation":[{"name":"Jagiellonian University, National Synchrotron Radiation Centre SOLARIS , Czerwone Maki 98 , ,","place":["Krak\u00f3w, Poland, 30-392"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Barbara","family":"Wolanin","sequence":"additional","affiliation":[{"name":"Jagiellonian University, National Synchrotron Radiation Centre SOLARIS , Czerwone Maki 98 , ,","place":["Krak\u00f3w, Poland, 30-392"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tom","family":"Hauffman","sequence":"additional","affiliation":[{"name":"Vrije Universiteit Brussel , , ,","place":["Brussels, Belgium, 1050"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6894-7258","authenticated-orcid":true,"given":"Joris Van de","family":"Vondel","sequence":"additional","affiliation":[{"name":"KU Leuven \u2013 University of Leuven , , Celestijnenlaan 200D , ,","place":["Leuven, Belgium, 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US Patent US20230259025A1, United States Patent and Trademark Office, 2022."},{"key":"2026102108064139600_cit42","doi-asserted-by":"publisher","first-page":"1161203","DOI":"10.1117\/12.2585004","article-title":"Breaking Stochastic Tradeoffs with a Dry Deposited and Dry Developed EUV Photoresist System","volume-title":"SPIE Adv. Lithogr.","author":"Wise","year":"2021"},{"key":"2026102108064139600_cit43","doi-asserted-by":"publisher","first-page":"27140","DOI":"10.1021\/acsami.2c04092","article-title":"Molecular Layer Deposition of a Hafnium-Based Hybrid Thin Film as an Electron Beam Resist","volume":"14","author":"Shi","year":"2022","journal-title":"ACS Appl. Mater. 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