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research article

Local vs. cooperative: Unraveling glass transition mechanisms with SEER

Ciamarra, Massimo Pica
•
Ji, Wencheng
•
Wyart, Matthieu  
May 28, 2024
Proceedings Of The National Academy Of Sciences Of The United States Of America (PNAS)

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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Type
research article
DOI
10.1073/pnas.2400611121
Web of Science ID

WOS:001240125900002

Author(s)
Ciamarra, Massimo Pica
Ji, Wencheng
Wyart, Matthieu  
Date Issued

2024-05-28

Publisher

National Academy of Sciences

Published in
Proceedings Of The National Academy Of Sciences Of The United States Of America (PNAS)
Volume

121

Issue

22

Article Number

e2400611121

Subjects

Glass

•

Excitation

•

Landscape

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
PCSL  
FunderGrant Number

Singapore Ministry of Education

MOE-T2EP50221- 0016

Simons Foundation

454953

SNSF

200021-165509

Available on Infoscience
June 19, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/208762
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