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The conjugation of PEG chains has a minor impact on ssODN binding; however, PEG chains of extended length can hinder ion pairing due to steric effects. The complexation of ssODN-PEG with branched PEI (BPEI) leads to the self-assembly of spherical core\u2013shell PCMs. When PEG chains are too short relative to the complexed core, aggregation of the PCMs occurs, evidenced by a deviation from the spheroid form factor and a rapid increase in the hydrodynamic size over time. The complexation of ssODN-PEG with linear PEI (LPEI) is also investigated. In phosphate-buffered saline (PBS) at physiologically relevant ionic strength, LPEI exhibits significantly weaker binding to ssODN-PEG compared to BPEI. However, well-defined PCMs are formed in either salt-free water or NaCl solutions, highlighting the strong ion sensitivity of LPEI-mediated complexation.<\/jats:p>","DOI":"10.1021\/acs.biomac.5c00623","type":"journal-article","created":{"date-parts":[[2025,9,19]],"date-time":"2025-09-19T23:20:35Z","timestamp":1758324035000},"page":"6528-6541","source":"Crossref","is-referenced-by-count":2,"title":["Investigating\nthe Self-Assembly of Polyelectrolyte\nComplex Micelles from Single-Stranded Oligodeoxynucleotide-Poly(ethylene\nglycol) Conjugates and Polyethylenimine"],"prefix":"10.1021","volume":"26","author":[{"given":"Kwanghee","family":"Lee","sequence":"first","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Takahiro","family":"Yokoyama","sequence":"additional","affiliation":[{"name":"Leibniz-Institut fu\u0308r Polymerforschung Dresden e.V. , ,","place":["Dresden, Germany, 01069"]},{"name":"Technische Universita\u0308t Dresden , , ,","place":["Dresden, Germany, 01069"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0563-825X","authenticated-orcid":true,"given":"Arash","family":"Nikoubashman","sequence":"additional","affiliation":[{"name":"Leibniz-Institut fu\u0308r Polymerforschung Dresden e.V. , ,","place":["Dresden, Germany, 01069"]},{"name":"Technische Universita\u0308t Dresden , , ,","place":["Dresden, Germany, 01069"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Seunghan","family":"Kang","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6020-3091","authenticated-orcid":true,"given":"Siyoung Q.","family":"Choi","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3127-3450","authenticated-orcid":true,"given":"Jeehae","family":"Shin","sequence":"additional","affiliation":[{"name":"Hankuk University of Foreign Studies , , ,","place":["Yong-In, Republic of Korea, 17035"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6172-5705","authenticated-orcid":true,"given":"Sheng","family":"Li","sequence":"additional","affiliation":[{"name":"Korea Advanced Institute of Science and Technology (KAIST) , , ,","place":["Daejeon, Republic of Korea, 34141"]},{"name":"KAIST Institute for the Nanocentury, KAIST , ,","place":["Daejeon, Republic of Korea, 34141"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2025,9,19]]},"reference":[{"issue":"10","key":"2026081812174529400_cit1","doi-asserted-by":"publisher","first-page":"673","DOI":"10.1038\/s41573-020-0075-7","article-title":"Advances in Oligonucleotide Drug\nDelivery","volume":"19","author":"Roberts","year":"2020","journal-title":"Nat. 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