Chain-Length-Dependent Correlated Molecular Motion in Polymers Article Swipe
Matthew Reynolds
,
Daniel L. Baker
,
Peter D. Olmsted
,
Johan Mattsson
·
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1103/p5r4-2g4q
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1103/p5r4-2g4q
We show how dynamic heterogeneities (DHs), a hallmark of glass-forming materials, depend on chain flexibility and chain length in polymers. For highly flexible polymers, a relatively large number of monomers ( N c ∼ 500 ) undergo correlated motion at the glass transition temperature ( T g ), independent of molecular weight ( M ). In contrast, less flexible polymers show a complex N c ( M ) behavior divided into three regimes, consistent with observations in both T g ( M ) and chain conformational structure. For short oligomers ( ≲ 2 Kuhn steps), a transition from mainly intermolecular correlations and N c ∼ 200 to strongly intramolecular correlations and N c < 50 (roughly the molecular size) is observed; for longer chains, N c increases weakly, before saturating. For poly(methyl methacrylate), a remarkable similarity is found between N c ( M ) and the M -dependent ratio of the activation barriers of the structural ( α ) and secondary ( β ) relaxations; we present evidence that this relationship is a general feature of glass-forming polymers. Our results suggest a direct link between the DH length scale and the number of β relaxation events jointly activated to facilitate the α relaxation.
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Chain-Length-Dependent Correlated Molecular Motion in PolymersWork title
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2025Year of publication
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2025-11-17Full publication date if available
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Matthew Reynolds, Daniel L. Baker, Peter D. Olmsted, Johan MattssonList of authors in order
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https://doi.org/10.1103/p5r4-2g4qPublisher landing page
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hybridOpen access status per OpenAlex
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Chain (unit), Polymer, Materials science, Statistical physics, Physics, Composite material, AstronomyTop concepts (fields/topics) attached by OpenAlex
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10Other works algorithmically related by OpenAlex
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| abstract_inverted_index.<c:msub> | 54 |
| abstract_inverted_index.<cb:math | 223 |
| abstract_inverted_index.<eb:math | 232 |
| abstract_inverted_index.<g:msub> | 82 |
| abstract_inverted_index.<gb:math | 267 |
| abstract_inverted_index.<ib:math | 279 |
| abstract_inverted_index.<k:msub> | 105 |
| abstract_inverted_index.<q:msub> | 141 |
| abstract_inverted_index.<s:msub> | 156 |
| abstract_inverted_index.<u:msub> | 175 |
| abstract_inverted_index.<w:msub> | 196 |
| abstract_inverted_index.barriers | 218 |
| abstract_inverted_index.behavior | 92 |
| abstract_inverted_index.evidence | 241 |
| abstract_inverted_index.flexible | 22, 74 |
| abstract_inverted_index.hallmark | 7 |
| abstract_inverted_index.monomers | 29 |
| abstract_inverted_index.polymers | 75 |
| abstract_inverted_index.regimes, | 96 |
| abstract_inverted_index.strongly | 149 |
| abstract_inverted_index.</a:math> | 40 |
| abstract_inverted_index.</a:msub> | 37 |
| abstract_inverted_index.</c:math> | 58 |
| abstract_inverted_index.</c:msub> | 57 |
| abstract_inverted_index.</e:math> | 69 |
| abstract_inverted_index.</g:math> | 91 |
| abstract_inverted_index.</g:msub> | 85 |
| abstract_inverted_index.</k:math> | 114 |
| abstract_inverted_index.</k:msub> | 108 |
| abstract_inverted_index.</o:math> | 128 |
| abstract_inverted_index.</q:math> | 147 |
| abstract_inverted_index.</q:msub> | 144 |
| abstract_inverted_index.</s:math> | 162 |
| abstract_inverted_index.</s:msub> | 159 |
| abstract_inverted_index.</u:math> | 179 |
| abstract_inverted_index.</u:msub> | 178 |
| abstract_inverted_index.</w:math> | 205 |
| abstract_inverted_index.</w:msub> | 199 |
| abstract_inverted_index.activated | 275 |
| abstract_inverted_index.contrast, | 72 |
| abstract_inverted_index.increases | 180 |
| abstract_inverted_index.molecular | 62, 165 |
| abstract_inverted_index.observed; | 168 |
| abstract_inverted_index.oligomers | 121 |
| abstract_inverted_index.polymers, | 23 |
| abstract_inverted_index.polymers. | 19, 251 |
| abstract_inverted_index.secondary | 230 |
| abstract_inverted_index.-dependent | 213 |
| abstract_inverted_index.</ab:math> | 212 |
| abstract_inverted_index.</cb:math> | 227 |
| abstract_inverted_index.</eb:math> | 236 |
| abstract_inverted_index.</gb:math> | 271 |
| abstract_inverted_index.</ib:math> | 283 |
| abstract_inverted_index.activation | 217 |
| abstract_inverted_index.consistent | 97 |
| abstract_inverted_index.correlated | 43 |
| abstract_inverted_index.facilitate | 277 |
| abstract_inverted_index.materials, | 10 |
| abstract_inverted_index.relatively | 25 |
| abstract_inverted_index.relaxation | 272 |
| abstract_inverted_index.remarkable | 188 |
| abstract_inverted_index.similarity | 189 |
| abstract_inverted_index.structural | 221 |
| abstract_inverted_index.structure. | 118 |
| abstract_inverted_index.transition | 48, 132 |
| abstract_inverted_index.flexibility | 14 |
| abstract_inverted_index.independent | 60 |
| abstract_inverted_index.poly(methyl | 185 |
| abstract_inverted_index.relaxation. | 284 |
| abstract_inverted_index.saturating. | 183 |
| abstract_inverted_index.temperature | 49 |
| abstract_inverted_index.correlations | 136, 151 |
| abstract_inverted_index.observations | 99 |
| abstract_inverted_index.relationship | 244 |
| abstract_inverted_index.relaxations; | 238 |
| abstract_inverted_index.glass-forming | 9, 250 |
| abstract_inverted_index.<a:mi>N</a:mi> | 35 |
| abstract_inverted_index.<a:mi>c</a:mi> | 36 |
| abstract_inverted_index.<c:mi>T</c:mi> | 55 |
| abstract_inverted_index.<c:mi>g</c:mi> | 56 |
| abstract_inverted_index.<e:mi>M</e:mi> | 68 |
| abstract_inverted_index.<g:mi>M</g:mi> | 88 |
| abstract_inverted_index.<g:mi>N</g:mi> | 83 |
| abstract_inverted_index.<g:mi>c</g:mi> | 84 |
| abstract_inverted_index.<k:mi>M</k:mi> | 111 |
| abstract_inverted_index.<k:mi>T</k:mi> | 106 |
| abstract_inverted_index.<k:mi>g</k:mi> | 107 |
| abstract_inverted_index.<o:mn>2</o:mn> | 127 |
| abstract_inverted_index.<q:mi>N</q:mi> | 142 |
| abstract_inverted_index.<q:mi>c</q:mi> | 143 |
| abstract_inverted_index.<s:mi>N</s:mi> | 157 |
| abstract_inverted_index.<s:mi>c</s:mi> | 158 |
| abstract_inverted_index.<u:mi>N</u:mi> | 176 |
| abstract_inverted_index.<u:mi>c</u:mi> | 177 |
| abstract_inverted_index.<w:mi>M</w:mi> | 202 |
| abstract_inverted_index.<w:mi>N</w:mi> | 197 |
| abstract_inverted_index.<w:mi>c</w:mi> | 198 |
| abstract_inverted_index.conformational | 117 |
| abstract_inverted_index.intermolecular | 135 |
| abstract_inverted_index.intramolecular | 150 |
| abstract_inverted_index.methacrylate), | 186 |
| abstract_inverted_index.<s:mn>50</s:mn> | 161 |
| abstract_inverted_index.heterogeneities | 4 |
| abstract_inverted_index.<a:mn>500</a:mn> | 39 |
| abstract_inverted_index.<a:mo>∼</a:mo> | 38 |
| abstract_inverted_index.<ab:mi>M</ab:mi> | 211 |
| abstract_inverted_index.<o:mo>≲</o:mo> | 126 |
| abstract_inverted_index.<q:mn>200</q:mn> | 146 |
| abstract_inverted_index.<q:mo>∼</q:mo> | 145 |
| abstract_inverted_index.<cb:mi>α</cb:mi> | 226 |
| abstract_inverted_index.<eb:mi>β</eb:mi> | 235 |
| abstract_inverted_index.<gb:mi>β</gb:mi> | 270 |
| abstract_inverted_index.<ib:mi>α</ib:mi> | 282 |
| abstract_inverted_index.<s:mo><</s:mo> | 160 |
| abstract_inverted_index.display="inline"> | 33, 53, 67, 81, 104, 125, 140, 155, 174, 195, 210, 225, 234, 269, 281 |
| abstract_inverted_index.stretchy="false">(</g:mo> | 87 |
| abstract_inverted_index.stretchy="false">(</k:mo> | 110 |
| abstract_inverted_index.stretchy="false">(</w:mo> | 201 |
| abstract_inverted_index.stretchy="false">)</g:mo> | 90 |
| abstract_inverted_index.stretchy="false">)</k:mo> | 113 |
| abstract_inverted_index.stretchy="false">)</w:mo> | 204 |
| abstract_inverted_index.xmlns:a="http://www.w3.org/1998/Math/MathML" | 32 |
| abstract_inverted_index.xmlns:c="http://www.w3.org/1998/Math/MathML" | 52 |
| abstract_inverted_index.xmlns:e="http://www.w3.org/1998/Math/MathML" | 66 |
| abstract_inverted_index.xmlns:g="http://www.w3.org/1998/Math/MathML" | 80 |
| abstract_inverted_index.xmlns:k="http://www.w3.org/1998/Math/MathML" | 103 |
| abstract_inverted_index.xmlns:o="http://www.w3.org/1998/Math/MathML" | 124 |
| abstract_inverted_index.xmlns:q="http://www.w3.org/1998/Math/MathML" | 139 |
| abstract_inverted_index.xmlns:s="http://www.w3.org/1998/Math/MathML" | 154 |
| abstract_inverted_index.xmlns:u="http://www.w3.org/1998/Math/MathML" | 173 |
| abstract_inverted_index.xmlns:w="http://www.w3.org/1998/Math/MathML" | 194 |
| abstract_inverted_index.xmlns:ab="http://www.w3.org/1998/Math/MathML" | 209 |
| abstract_inverted_index.xmlns:cb="http://www.w3.org/1998/Math/MathML" | 224 |
| abstract_inverted_index.xmlns:eb="http://www.w3.org/1998/Math/MathML" | 233 |
| abstract_inverted_index.xmlns:gb="http://www.w3.org/1998/Math/MathML" | 268 |
| abstract_inverted_index.xmlns:ib="http://www.w3.org/1998/Math/MathML" | 280 |
| cited_by_percentile_year | |
| countries_distinct_count | 0 |
| institutions_distinct_count | 4 |
| citation_normalized_percentile.value | 0.00112229 |
| citation_normalized_percentile.is_in_top_1_percent | False |
| citation_normalized_percentile.is_in_top_10_percent | False |