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In many experimentally relevant systems, the nanoparticles are not covalently attached to the polymer network but are instead physically trapped within its meshes. Despite this weak mechanical coupling, experiments reveal signatures of hindered rotational dynamics. Here, we investigate the microscopic origin of this behavior by combining experiments on polyacrylamide hydrogels loaded with cobalt ferrite nanoparticles with simulations that explicitly account for polymers, nanoparticles, and hydrodynamic interactions. We probe the nanoparticle\u2013polymer coupling by exploring the systems\u2019 magnetic AC susceptibility\u2014a quantity that is accessible both by experiment and in simulations, and that is sensitive to rotational dynamics. Experimentally, we observe a reduced low-frequency susceptibility, indicating partial orientational blocking of the nanoparticles, even in the absence of covalent bonding. Simulations show that this behavior cannot be explained by hydrodynamic coupling or isotropic van der Waals-like interactions alone. Instead, our results demonstrate that a degree of preferential attachment of polymers to spots on the nanoparticle surface\u2014arising from chemical or topographical heterogeneity\u2014is essential to reproduce the experimentally observed response.<\/jats:p>","DOI":"10.1063\/5.0323088","type":"journal-article","created":{"date-parts":[[2026,5,4]],"date-time":"2026-05-04T15:50:40Z","timestamp":1777909840000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Nanoparticle\u2013polymer coupling in magnetic gels studied by means of computer simulations and experiments"],"prefix":"10.1063","volume":"164","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-7488-2222","authenticated-orcid":false,"given":"Rebecca","family":"Stephan","sequence":"first","affiliation":[{"name":"Institute for Computational Physics, University of Stuttgart 1 , 70569 Stuttgart,","place":["Germany"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5551-8155","authenticated-orcid":false,"given":"Surojit","family":"Ranoo","sequence":"additional","affiliation":[{"name":"Institute of Physical Chemistry, Department of Chemistry, University of Cologne 2 , D-50939 Cologne,","place":["Germany"]},{"name":"Laboratoire Collo\u00efdes et Mat\u00e9riaux Divis\u00e9s, CBI, ESPCI Paris, Universit\u00e9 PSL, CNRS 3 , 75005 Paris,","place":["France"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0228-9034","authenticated-orcid":false,"given":"Patrick","family":"Kreissl","sequence":"additional","affiliation":[{"name":"Institute for Computational Physics, University of Stuttgart 1 , 70569 Stuttgart,","place":["Germany"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-9857-9965","authenticated-orcid":false,"given":"Chinmay","family":"Pabshettiwar","sequence":"additional","affiliation":[{"name":"Institute for Computational Physics, University of Stuttgart 1 , 70569 Stuttgart,","place":["Germany"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-4551-9017","authenticated-orcid":false,"given":"Jessica","family":"Kubis","sequence":"additional","affiliation":[{"name":"Institute of Physical Chemistry, Department of Chemistry, University of Cologne 2 , D-50939 Cologne,","place":["Germany"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2739-310X","authenticated-orcid":false,"given":"Christian","family":"Holm","sequence":"additional","affiliation":[{"name":"Institute for Computational Physics, University of Stuttgart 1 , 70569 Stuttgart,","place":["Germany"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7284-7847","authenticated-orcid":false,"given":"Annette M.","family":"Schmidt","sequence":"additional","affiliation":[{"name":"Institute of Physical Chemistry, Department of Chemistry, University of Cologne 2 , D-50939 Cologne,","place":["Germany"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0555-5104","authenticated-orcid":false,"given":"Regine","family":"von Klitzing","sequence":"additional","affiliation":[{"name":"Institute for Condensed Matter Physics, Technical University of Darmstadt 4 , 64289 Darmstadt,","place":["Germany"]}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1128-2093","authenticated-orcid":false,"given":"Rudolf","family":"Weeber","sequence":"additional","affiliation":[{"name":"Institute for Computational Physics, University of Stuttgart 1 , 70569 Stuttgart,","place":["Germany"]}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"317","published-online":{"date-parts":[[2026,5,4]]},"reference":[{"key":"2026050411503508800_c1","doi-asserted-by":"publisher","first-page":"98","DOI":"10.1007\/s003960050017","volume":"278","year":"2000","journal-title":"Colloid Polym. 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