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Methods of Ex Situ and In Situ Investigations of Structural Transformations: The Case of Crystallization of Metallic Glasses
Published on: June 7, 2018
Thermal origin of quasilocalized excitations in glasses
Wencheng Ji1, Tom W J de Geus1, Marko Popović1
1Institute of Physics, École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland.
Abstract:
Key aspects of glasses are controlled by the presence of excitations in which a group of particles can rearrange. Surprisingly, recent observations indicate that their density is dramatically reduced and their size decreases as the temperature of the supercooled liquid is lowered. Some theories predict these excitations to cause a gap in the spectrum of quasilocalized modes of the Hessian that grows upon cooling, while others predict a pseudogap D_{L}(ω)∼ω^{α}. To unify these views and observations, we generate glassy configurations of controlled gap magnitude ω_{c} at temperature T=0, using so-called breathing particles, and study how such gapped states respond to thermal fluctuations. We find that (i) the gap always fills up at finite T with D_{L}(ω)≈A_{4}(T)ω^{4} and A_{4}∼exp(-E_{a}/T) at low T, (ii) E_{a} rapidly grows with ω_{c}, in reasonable agreement with a simple scaling prediction E_{a}∼ω_{c}^{4} and (iii) at larger ω_{c} excitations involve fewer particles, as we rationalize, and eventually become stringlike. We propose an interpretation of mean-field theories of the glass transition, in which the modes beyond the gap act as an excitation reservoir, from which a pseudogap distribution is populated with its magnitude rapidly decreasing at lower T. We discuss how this picture unifies the rarefaction as well as the decreasing size of excitations upon cooling, together with a stringlike relaxation occurring near the glass transition.
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