{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,13]],"date-time":"2026-10-13T00:25:08Z","timestamp":1791851108623,"version":"4.3.4"},"reference-count":59,"publisher":"American Physical Society (APS)","issue":"9","license":[{"start":{"date-parts":[[2025,3,7]],"date-time":"2025-03-07T00:00:00Z","timestamp":1741305600000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/link.aps.org\/licenses\/aps-default-license"},{"start":{"date-parts":[[2026,3,7]],"date-time":"2026-03-07T00:00:00Z","timestamp":1772841600000},"content-version":"am","delay-in-days":365,"URL":"https:\/\/link.aps.org\/licenses\/aps-default-accepted-manuscript-license"}],"funder":[{"DOI":"10.13039\/100000001","name":"National Science Foundation","doi-asserted-by":"publisher","award":["DMR-2006504"],"award-info":[{"award-number":["DMR-2006504"]}],"id":[{"id":"10.13039\/100000001","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000001","name":"National Science Foundation","doi-asserted-by":"publisher","award":["DMR-2400039"],"award-info":[{"award-number":["DMR-2400039"]}],"id":[{"id":"10.13039\/100000001","id-type":"DOI","asserted-by":"publisher"}]},{"name":"Action de Recherche Concert\u00e9e ULB"}],"content-domain":{"domain":["journals.aps.org"],"crossmark-restriction":true},"short-container-title":["Phys. Rev. Lett."],"accepted":{"date-parts":[[2025,2,6]]},"DOI":"10.1103\/physrevlett.134.098203","type":"journal-article","created":{"date-parts":[[2025,3,7]],"date-time":"2025-03-07T10:02:35Z","timestamp":1741341755000},"update-policy":"https:\/\/doi.org\/10.1103\/crossmark-policy","source":"Crossref","is-referenced-by-count":38,"title":["Mechanistic Picture for the Slow Arrhenius Process in Glass Forming Systems: The Collective Small Displacements Model"],"prefix":"10.1103","volume":"134","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-6593-1736","authenticated-orcid":true,"given":"Ronald P.","family":"White","sequence":"first","affiliation":[{"id":[{"id":"https:\/\/ror.org\/049s0rh22","id-type":"ROR","asserted-by":"publisher"}],"name":"Dartmouth College"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7662-9858","authenticated-orcid":true,"given":"Simone","family":"Napolitano","sequence":"additional","affiliation":[{"id":[{"id":"https:\/\/ror.org\/01r9htc13","id-type":"ROR","asserted-by":"publisher"}],"name":"Universit\u00e9 libre de Bruxelles (ULB)"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0177-9373","authenticated-orcid":true,"given":"Jane E.\u2009G.","family":"Lipson","sequence":"additional","affiliation":[{"id":[{"id":"https:\/\/ror.org\/049s0rh22","id-type":"ROR","asserted-by":"publisher"}],"name":"Dartmouth College"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"16","published-online":{"date-parts":[[2025,3,7]]},"reference":[{"key":"PhysRevLett.134.098203Cc1R1","volume-title":"Viscoelastic Properties of Polymers","author":"J.\u2009D. Ferry","year":"1970","type":"book"},{"key":"PhysRevLett.134.098203Cc2R1","doi-asserted-by":"publisher","DOI":"10.1016\/0079-6700(94)00001-I","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc3R1","doi-asserted-by":"publisher","DOI":"10.1126\/science.267.5206.1945","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc4R1","doi-asserted-by":"publisher","DOI":"10.1038\/209070a0","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc5R1","doi-asserted-by":"publisher","DOI":"10.1063\/1.1675789","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc6R1","doi-asserted-by":"publisher","DOI":"10.1016\/0378-4371(93)90416-2","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc7R1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.abm7154","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc8R1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.macromol.2c00789","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc9R1","doi-asserted-by":"publisher","DOI":"10.1021\/acspolymersau.3c00020","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc10R1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0186755","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc11R1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.118.225901","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc12R1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0189652","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc13R1","doi-asserted-by":"publisher","DOI":"10.1016\/j.nxmate.2024.100168","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc14R1","doi-asserted-by":"publisher","DOI":"10.1016\/j.polymer.2022.124671","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc15R1","doi-asserted-by":"publisher","DOI":"10.1021\/acsmacrolett.3c00003","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc16R1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0174213","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc17R1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpclett.4c00902","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc18R1","doi-asserted-by":"publisher","DOI":"10.1021\/acsmacrolett.9b00116","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc19R1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0185728","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc20R1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0157994","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc21R1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.111.095701","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc22R1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0223415","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc23R1","volume-title":"Broadband Dielectric Spectroscopy","author":"A. Schonhals","year":"2003","type":"book"},{"key":"PhysRevLett.134.098203Cc24R1","doi-asserted-by":"publisher","DOI":"10.1063\/1.1674335","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc25R1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.91.115701","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc26R1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevE.69.031501","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc27R1","doi-asserted-by":"publisher","DOI":"10.1021\/ma048555s","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc28R1","unstructured":"We note that a set of slower processes was identified in Ref.\u00a0[27]. Differently from the SAP, the activation barrier of these processes depends on temperature, and their timescales are sensitive to molecular weight.","type":"other"},{"key":"PhysRevLett.134.098203Cc29R1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0184382","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc30R1","unstructured":"Because the displacements explored by segments are assumed limited and roughly T-independent, and noting how the shearlike collective motion means that directly adjacent near neighbor segments often move nearly together with little change in their mutual separation distance, we expect the process\u2019 volume sensitivity (its need for density fluctuations) to be small. Thus, as volume changes with T at ambient pressure, the activation energy should remain approximately constant (unlike the \u03b1-process).","type":"other"},{"key":"PhysRevLett.134.098203Cc31R1","unstructured":"The total entropy change, subsystem plus matrix, is \u0394Eact(Too\u22121\u2212T\u22121). For energy flow between bulk systems, total entropy must increase, and while here fluctuations can still oppose this natural direction to a degree, there are probabilistic limits. This implies that Too cannot be too different from T. The SAP is observed experimentally in the T=300\u2013500\u2009\u2009K range, so Too\u2248400\u2009\u2009K would be a good guess. See also the SM for further discussion related to Too.","type":"other"},{"key":"PhysRevLett.134.098203Cc32R1","unstructured":"As thermodynamic segmental interaction energies (\u03f5) increase in strength, it will hinder movement and should require a larger number of segments to participate (move together) in the collective motion. This expectation is sensible given the modest segmental displacements.","type":"other"},{"key":"PhysRevLett.134.098203Cc33R1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.macromol.6b00215","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc34R1","doi-asserted-by":"publisher","DOI":"10.1063\/1.3200925","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc35R1","doi-asserted-by":"publisher","DOI":"10.1021\/je5002818","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc36R1","unstructured":"The material-specific partitioning into segments is key; only a molecular (stat-mech) based model can do this. This way an energy (\u03f5) can be assigned that is specifically relevant to each material\u2019s individual moving parts. These \u201cthermodynamic segments\u201d are expected, at least proportionally, to reflect the effective SAP \u201cdynamics segments.\u201d","type":"other"},{"key":"PhysRevLett.134.098203Cc37R1","unstructured":"Below about that \u03f5 value (1.7\u2009\u2009kJ\/mol) a \u201chypothetical\u201d model system would exhibit unpolymerlike thermodynamic behavior, e.g., coefficient of thermal expansion too high, density too low, and compressibility too high.","type":"other"},{"key":"PhysRevLett.134.098203Cc38R1","unstructured":"See Supplemental Material at http:\/\/link.aps.org\/supplemental\/10.1103\/PhysRevLett.134.098203 for details on thermodynamic analysis and implementation of the CSD model, which includes Refs.\u00a0[7,15,16,27,33\u201335,39\u201349].","type":"other"},{"key":"PhysRevLett.134.098203Cc39R1","doi-asserted-by":"publisher","DOI":"10.1039\/D3CP05044K","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc40R1","doi-asserted-by":"publisher","DOI":"10.1021\/ma5005474","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc41R1","doi-asserted-by":"publisher","DOI":"10.1021\/j100562a008","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc42R1","volume-title":"Standard Pressure Volume\u00a0Temperature Data for Polymers","author":"P. Zoller","year":"1995","type":"book"},{"key":"PhysRevLett.134.098203Cc43R1","doi-asserted-by":"publisher","DOI":"10.1007\/BF00396562","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc44R1","doi-asserted-by":"publisher","DOI":"10.1002\/pol.1982.180200811","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc45R1","doi-asserted-by":"publisher","DOI":"10.1021\/ma060315k","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc46R1","doi-asserted-by":"publisher","DOI":"10.1021\/ma402074b","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc47R1","doi-asserted-by":"publisher","DOI":"10.1002\/app.30768","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc48R1","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2100738118","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc49R1","doi-asserted-by":"publisher","DOI":"10.1039\/D2SM00959E","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc50R1","doi-asserted-by":"publisher","DOI":"10.1088\/0034-4885\/69\/4\/R04","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc51R1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.65.618","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc52R1","doi-asserted-by":"publisher","DOI":"10.1039\/cs9891800477","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc53R1","unstructured":"The dS\/dE of any finite-sized system must decrease as more and more energy is transferred into it. If, rather than assumption 2, subsystem sizes were all about the same, the average effective subsystem dS\/dE=1\/Too would be lower for those materials with higher \u0394Eact, and so there could not be a common Too shared by all systems.","type":"other"},{"key":"PhysRevLett.134.098203Cc54R1","unstructured":"Note that while f0 is obtained from extrapolation of experimental measurements, it is unlikely that the relaxation rate would ever reach such a value. As real materials degrade at finite temperatures (carbon-based polymers do not survive above 900\u00a0K), in the model terms, f0 is simply expressing a reasonable approximation for the process\u2019s entropy of activation that is only expected to be valid in the limited T range where experiments are performed [31].","type":"other"},{"key":"PhysRevLett.134.098203Cc55R1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.132.248101","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc56R1","unstructured":"While at the molecular level adsorption might be a complex phenomenon involving several mechanisms, Thoms et\u00a0al. [55] have recently verified that for melts of linear polymers adsorbed on flat surfaces the adsorption rate can be obtained by multiplying fSAP by a constant, which does not depend on temperature or on the interfacial chemistry. This point verifies the hypothesis used to build up Eq.\u00a0(4).","type":"other"},{"key":"PhysRevLett.134.098203Cc57R1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.aay1454","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc58R1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-023-40417-4","type":"journal-article"},{"key":"PhysRevLett.134.098203Cc59R1","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2407030121","type":"journal-article"}],"container-title":["Physical Review Letters"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/link.aps.org\/accepted\/10.1103\/PhysRevLett.134.098203","content-type":"application\/pdf","content-version":"am","intended-application":"unspecified"},{"URL":"https:\/\/link.aps.org\/article\/10.1103\/PhysRevLett.134.098203","content-type":"unspecified","content-version":"vor","intended-application":"syndication"},{"URL":"http:\/\/harvest.aps.org\/v2\/journals\/articles\/10.1103\/PhysRevLett.134.098203\/fulltext","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T18:46:05Z","timestamp":1790707565000},"score":1,"resource":{"primary":{"URL":"https:\/\/link.aps.org\/doi\/10.1103\/PhysRevLett.134.098203"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2025,3,7]]},"references-count":59,"journal-issue":{"issue":"9","published-print":{"date-parts":[[2025,3]]}},"URL":"https:\/\/doi.org\/10.1103\/physrevlett.134.098203","relation":{},"ISSN":["0031-9007","1079-7114"],"issn-type":[{"value":"0031-9007","type":"print"},{"value":"1079-7114","type":"electronic"}],"subject":[],"published":{"date-parts":[[2025,3,7]]},"assertion":[{"value":"2024-09-20","name":"date_received","label":"Date Received","group":{"name":"publication_dates","label":"Publication dates"}},{"value":"\u00a9 2025 American Physical Society. All rights are reserved, including those for text and data mining, AI training, and similar technologies.","name":"copyright_statement","label":"Copyright statement","group":{"name":"copyright","label":"copyright"}},{"value":"2025","name":"copyright_year","label":"Copyright year","group":{"name":"copyright","label":"copyright"}},{"value":"American Physical Society","name":"copyright_holder","label":"Copyright holder","group":{"name":"copyright","label":"copyright"}}],"article-number":"098203"}}