Local vs. cooperative: unraveling glass transition mechanisms with SEER
Which phenomenon slows down the dynamics in supercooled liquids and turns them into glasses is a long-standing question of condensed matter. Most popular theories posit that as the temperature decreases, many events must occur in a coordinated fashion on a growing length scale for relaxation to occu...
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sg-ntu-dr.10356-1792822024-07-29T15:34:50Z Local vs. cooperative: unraveling glass transition mechanisms with SEER Ciamarra, Massimo Pica Ji, Wencheng Wyart, Matthieu School of Physical and Mathematical Sciences Physics Excitation Landscape Which phenomenon slows down the dynamics in supercooled liquids and turns them into glasses is a long-standing question of condensed matter. Most popular theories posit that as the temperature decreases, many events must occur in a coordinated fashion on a growing length scale for relaxation to occur. Instead, other approaches consider that local barriers associated with the elementary rearrangement of a few particles or "excitations" govern the dynamics. To resolve this conundrum, our central result is to introduce an algorithm, Systematic Excitation ExtRaction, which can systematically extract hundreds of excitations and their energy from any given configuration. We also provide a measurement of the activation energy, characterizing the liquid dynamics, based on fast quenching and reheating. We use these two methods in a popular liquid model of polydisperse particles. Such polydisperse models are known to capture the hallmarks of the glass transition and can be equilibrated efficiently up to millisecond time scales. The analysis reveals that cooperative effects do not control the fragility of such liquids: the change of energy of local barriers determines the change of activation energy. More generally, these methods can now be used to measure the degree of cooperativity of any liquid model. Ministry of Education (MOE) Published version M.P.C. discloses support for the research of this work from Singapore Ministry of Education [MOE-T2EP50221-0016]. M.W. acknowledges support from the Simons Foundation Grant (No. 454953, M.W.) and from the SNSF under Grant No. 200021-165509. 2024-07-24T07:09:25Z 2024-07-24T07:09:25Z 2024 Journal Article Ciamarra, M. P., Ji, W. & Wyart, M. (2024). Local vs. cooperative: unraveling glass transition mechanisms with SEER. Proceedings of the National Academy of Sciences (PNAS), 121(22), e2400611121-. https://dx.doi.org/10.1073/pnas.2400611121 0027-8424 https://hdl.handle.net/10356/179282 10.1073/pnas.2400611121 38787876 2-s2.0-85194218211 22 121 e2400611121 en MOE-T2EP50221-0016 Proceedings of the National Academy of Sciences (PNAS) © 2024 the Author(s). Published by PNAS. This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND). application/pdf |
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Physics Excitation Landscape Ciamarra, Massimo Pica Ji, Wencheng Wyart, Matthieu Local vs. cooperative: unraveling glass transition mechanisms with SEER |
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Which phenomenon slows down the dynamics in supercooled liquids and turns them into glasses is a long-standing question of condensed matter. Most popular theories posit that as the temperature decreases, many events must occur in a coordinated fashion on a growing length scale for relaxation to occur. Instead, other approaches consider that local barriers associated with the elementary rearrangement of a few particles or "excitations" govern the dynamics. To resolve this conundrum, our central result is to introduce an algorithm, Systematic Excitation ExtRaction, which can systematically extract hundreds of excitations and their energy from any given configuration. We also provide a measurement of the activation energy, characterizing the liquid dynamics, based on fast quenching and reheating. We use these two methods in a popular liquid model of polydisperse particles. Such polydisperse models are known to capture the hallmarks of the glass transition and can be equilibrated efficiently up to millisecond time scales. The analysis reveals that cooperative effects do not control the fragility of such liquids: the change of energy of local barriers determines the change of activation energy. More generally, these methods can now be used to measure the degree of cooperativity of any liquid model. |
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School of Physical and Mathematical Sciences |
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School of Physical and Mathematical Sciences Ciamarra, Massimo Pica Ji, Wencheng Wyart, Matthieu |
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Article |
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Ciamarra, Massimo Pica Ji, Wencheng Wyart, Matthieu |
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Ciamarra, Massimo Pica |
title |
Local vs. cooperative: unraveling glass transition mechanisms with SEER |
title_short |
Local vs. cooperative: unraveling glass transition mechanisms with SEER |
title_full |
Local vs. cooperative: unraveling glass transition mechanisms with SEER |
title_fullStr |
Local vs. cooperative: unraveling glass transition mechanisms with SEER |
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Local vs. cooperative: unraveling glass transition mechanisms with SEER |
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local vs. cooperative: unraveling glass transition mechanisms with seer |
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2024 |
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https://hdl.handle.net/10356/179282 |
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