The role of excitations in supercooled liquids: Density, geometry, and relaxation dynamics

Low-energy excitations play a key role in all condensed-matter systems, yet there is limited understanding of their nature in glasses, where they correspond to local rearrangements of groups of particles. Here, we introduce an algorithm to systematically uncover these excitations up to the activation energy scale relevant to structural relaxation. We use it in a model system to measure the density of states on a scale never achieved before, confirming that this quantity shifts to higher energy under cooling, precisely as the activation energy does. Second, we show that the excitations' energetic and spatial features allow one to predict with great accuracy the dynamic propensity, i.e., the location of future relaxation dynamics. Finally, we find that excitations have a primary field whose properties, including the displacement of the most mobile particle, scale as a power-law of their activation energy and are independent of temperature. Additionally, they exhibit an outer deformation field that depends on the material's stability and, therefore, on temperature. We build a scaling description of these findings. Overall, our analysis supports that excitations play a crucial role in regulating relaxation dynamics near the glass transition, effectively suppressing the transition to dynamical arrest predicted by mean-field theories while also being strongly influenced by it.

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Publication Details

Journal
Proceedings of the National Academy of Sciences
Published
2025-03-12
DOI
https://doi.org/10.1073/pnas.2416800122
Citations
3
Primary Topic
Material Dynamics and Properties
Type
article
Field-Weighted Citation Impact
1.55

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article

The role of excitations in supercooled liquids: Density, geometry, and relaxation dynamics

Matthieu Wyart, Wencheng Ji, Massimo Pica Ciamarra
3 citations
Proceedings of the National Academy of Sciences
Material Dynamics and Properties
1.55
article

The role of excitations in supercooled liquids: Density, geometry, and relaxation dynamics

Matthieu Wyart, Wencheng Ji, Massimo Pica Ciamarra
article en
3 citations

Abstract

Low-energy excitations play a key role in all condensed-matter systems, yet there is limited understanding of their nature in glasses, where they correspond to local rearrangements of groups of particles. Here, we introduce an algorithm to systematically uncover these excitations up to the activation energy scale relevant to structural relaxation. We use it in a model system to measure the density of states on a scale never achieved before, confirming that this quantity shifts to higher energy under cooling, precisely as the activation energy does. Second, we show that the excitations' energetic and spatial features allow one to predict with great accuracy the dynamic propensity, i.e., the location of future relaxation dynamics. Finally, we find that excitations have a primary field whose properties, including the displacement of the most mobile particle, scale as a power-law of their activation energy and are independent of temperature. Additionally, they exhibit an outer deformation field that depends on the material's stability and, therefore, on temperature. We build a scaling description of these findings. Overall, our analysis supports that excitations play a crucial role in regulating relaxation dynamics near the glass transition, effectively suppressing the transition to dynamical arrest predicted by mean-field theories while also being strongly influenced by it.

Proceedings of the National Academy of SciencesVol. 122(11)
Nanyang Technological University (SG), Superconducting and other Innovative Materials and Devices Institute (IT), FZU ‒ Institute of Physics of the Academy of Sciences of the Czech Republic (CZ), National Research Council (IT), École Polytechnique Fédérale de Lausanne (CH), Weizmann Institute of Science (IL)
Juliet Lea Hillman Simonds Foundation, Ministry of Education - Singapore, Swiss National Centre of Competence in Research Kidney Control of Homeostasis
Affordable and clean energy
Openalex Percentile: Top 19%
Material Dynamics and Properties
1.55
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