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Here, we regulate the internal ordering of a 2,2\u2032-((2Z,2\u2032Z)-((12,13-bis(2-ethylhexyl)-3,9-diundecyl-12,13-dihydro-thiadiazolo[3,4-e]thieno[2\u2033,3\u2033:4\u2032,5\u2032]thieno[2\u2032,3\u2032:4,5]pyrrolo[3,2-g]thieno[2\u2032,3\u2032:4,5]thieno[3,2-b]indole-2,10-diyl)bis(methanylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile (Y6)-derived nonfullerene acceptor by removing the core alkyl chains to produce YHD-2F. Compared with Y6, YHD-2F NPs exhibit more pronounced vibronic features in their absorption spectra and a smaller Stokes shift, indicating reduced energetic disorder. Powder X-ray diffraction and cryo-TEM directly reveal that YHD-2F retains discernible lattice order even during rapid NP formation driven by rapid aggregation, whereas Y6 shows broadened diffraction features consistent with heterogeneous packing. Molecular dynamics simulations further indicate tighter and more balanced intermolecular packing in YHD-2F. Transient absorption and photoinduced absorption measurements show that YHD-2F generates a larger population of long-lived electrons, which are further enhanced by l-ascorbic acid and quenched by Pt. Consequently, single-component YHD-2F NPs achieve a hydrogen evolution rate of 116.4 mmol g\u20131 h\u20131 under AM 1.5G irradiation, more than three times higher than that of Y6 NPs, with an apparent quantum yield of 1.50% at 800 nm. These results demonstrate that core alkyl-chain engineering can program intraparticle ordering in organic photocatalyst NPs, providing a general design principle for morphology-controlled NP photocatalysts toward efficient solar-to-hydrogen energy conversion.<\/jats:p>","DOI":"10.1021\/acsnano.6c08786","type":"journal-article","created":{"date-parts":[[2026,7,27]],"date-time":"2026-07-27T05:03:49Z","timestamp":1785128629000},"page":"22138-22148","source":"Crossref","is-referenced-by-count":0,"title":["Programming Intraparticle\nOrdering in Y6-Derived Organic\nPhotocatalyst Nanoparticles for Efficient Solar Hydrogen Evolution"],"prefix":"10.1021","volume":"20","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-4512-9198","authenticated-orcid":true,"given":"Min Gyu","family":"Kang","sequence":"first","affiliation":[{"name":"Korea University , , ,","place":["Seoul, Republic of Korea, 02841"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rose","family":"Newman","sequence":"additional","affiliation":[{"name":"University of Oxford , , 12 Mansfield Road , ,","place":["Oxford, U.K., OX1 3TA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7123-4678","authenticated-orcid":true,"given":"Zhihao","family":"Feng","sequence":"additional","affiliation":[{"name":"Georgia Institute of Technology , , , ,","place":["Atlanta, Georgia, United States, 30332"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jae Hoon","family":"Son","sequence":"additional","affiliation":[{"name":"Korea University , , ,","place":["Seoul, Republic of Korea, 02841"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Charles","family":"Jeffreys","sequence":"additional","affiliation":[{"name":"King Abdullah University of Science and Technology (KAUST) , , ,","place":["Thuwal, Kingdom of Saudi Arabia, 23955-6900"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jin-Woo","family":"Lee","sequence":"additional","affiliation":[{"name":"University of Oxford , , 12 Mansfield Road , ,","place":["Oxford, U.K., OX1 3TA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lingyun","family":"Zhao","sequence":"additional","affiliation":[{"name":"King Abdullah University of Science and Technology (KAUST) , , ,","place":["Thuwal, Kingdom of Saudi Arabia, 23955-6900"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Stanley","family":"Cazaly","sequence":"additional","affiliation":[{"name":"Queen Mary University of London , , Mile End Road , ,","place":["London, U.K., E1 4NS"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Flurin","family":"Eisner","sequence":"additional","affiliation":[{"name":"Queen Mary University of London , , Mile End Road , ,","place":["London, U.K., E1 4NS"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Byung Hui","family":"Lee","sequence":"additional","affiliation":[{"name":"Korea University , , ,","place":["Seoul, Republic of Korea, 02841"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Min Hun","family":"Jee","sequence":"additional","affiliation":[{"name":"Korea University , , ,","place":["Seoul, Republic of Korea, 02841"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9318-2573","authenticated-orcid":true,"given":"Dong Won","family":"Kang","sequence":"additional","affiliation":[{"name":"Inha University , , 100 Inha-Ro , Michuhol-gu, ,","place":["Incheon, Republic of Korea, 22212"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6879-5020","authenticated-orcid":true,"given":"Martin","family":"Heeney","sequence":"additional","affiliation":[{"name":"King Abdullah University of Science and Technology 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