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The dendrimers, featuring a tetrafunctional silicon core, trifunctional =Si(CH3)\u2013 branching units, and terminal hydroxyl groups, adopt a characteristic \u201cumbrella\u201d conformation at low coverage, with hydrophilic termini anchored in water and the hydrophobic core aligned with the nonpolar phase. Interfacial chemistry fundamentally modulates this architecture: favorable toluene\u2013core interactions promote core swelling and homogeneous lateral dispersion, whereas the sharp hydrophobic mismatch at the water\u2013air interface drives dendrimer aggregation. Lateral compression induces a systematic transition from flattened, anisotropic conformations to more isotropic, near-spherical geometries, accompanied by redistribution of hydrogen bonds from dendrimer\u2013water to intra- and interdendrimer contacts. Under strong confinement, steric crowding and transient interdendrimer hydrogen bonding lead to dynamic arrest, with lateral diffusion suppressed by orders of magnitude. These findings establish a unified molecular picture of how surface density and solvent compatibility jointly control conformation, interactions, and mobility in amphiphilic dendrimer monolayers, providing design principles for tunable interfacial materials with tailored mechanical and transport properties.<\/jats:p>","DOI":"10.1063\/5.0358208","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T10:56:47Z","timestamp":1792061807000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Hydroxyl-terminated carbosilane dendrimer films at water\u2013toluene and water\u2013air interfaces"],"prefix":"10.1063","volume":"165","author":[{"given":"Kirill A.","family":"Litvin","sequence":"first","affiliation":[{"name":"Faculty of Physics, Lomonosov Moscow State University 1 , Moscow 119991,","place":["Russia"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1161-4369","authenticated-orcid":false,"given":"Andrey O.","family":"Kurbatov","sequence":"additional","affiliation":[{"name":"Faculty of Physics, Lomonosov Moscow State University 1 , Moscow 119991,","place":["Russia"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7883-8119","authenticated-orcid":false,"given":"Nikolay K.","family":"Balabaev","sequence":"additional","affiliation":[{"name":"Faculty of Physics, Lomonosov Moscow State University 1 , Moscow 119991,","place":["Russia"]},{"name":"Institute of Mathematical Problems of Biology RAS\u2014The Branch of Keldysh Institute of Applied Mathematics of Russian Academy of Sciences 2 , Pushchino 142290, Moscow Region,","place":["Russia"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1716-7010","authenticated-orcid":false,"given":"Elena Yu.","family":"Kramarenko","sequence":"additional","affiliation":[{"name":"Faculty of Physics, Lomonosov Moscow State University 1 , Moscow 119991,","place":["Russia"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2026,10,15]]},"reference":[{"key":"2026101506564172500_c1","doi-asserted-by":"crossref","DOI":"10.1002\/0470845821","volume-title":"Dendrimers and Other Dendritic Polymers","author":"Fr\u00e9chet","year":"2001"},{"key":"2026101506564172500_c2","volume-title":"Dendrimers and Dendrons: Concepts, Syntheses, Applications","year":"2001"},{"key":"2026101506564172500_c3","doi-asserted-by":"crossref","DOI":"10.1007\/978-1-4020-8174-3","volume-title":"Silicon-Containing Dendritic Polymers","author":"Dvornic","year":"2009"},{"issue":"1","key":"2026101506564172500_c4","doi-asserted-by":"publisher","first-page":"35","DOI":"10.1016\/s1359-6446(04)03276-3","volume":"10","year":"2005","journal-title":"Drug Discovery Today"},{"key":"2026101506564172500_c5","doi-asserted-by":"publisher","first-page":"102","DOI":"10.1016\/j.addr.2012.09.030","volume":"64","year":"2012","journal-title":"Adv. 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