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Nonmonotonic Dynamical Correlations beneath the Surface of Glass-Forming Liquids

Peng, H. and Liu, Huashan and Voigtmann, Thomas (2022) Nonmonotonic Dynamical Correlations beneath the Surface of Glass-Forming Liquids. Physical Review Letters, 129, p. 215501. American Physical Society. doi: 10.1103/PhysRevLett.129.215501. ISSN 0031-9007.

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Abstract

Collective motion over increasing length scales is a signature of the vitrification process of liquids. We demonstrate how distinct static and dynamic length scales govern the dynamics of vitrifying films. In contrast to a monotonically growing static correlation length, the dynamical correlation length that measures the extent of surface-dynamics acceleration into the bulk displays a striking nonmonotonic temperature evolution that is robust also against changes in detailed interatomic interaction. This nonmonotonic change defines a crossover temperature T* that is distinct from the critical temperature Tc of mode-coupling theory. We connect this nonmonotonic change to a morphological change of cooperative rearrangement regions of fast particles, and to the point where the decoupling of fast-particle motion from the bulk relaxation is most sensitive to fluctuations. We propose a rigorous definition of this new crossover temperature T* within a recent extension of mode-coupling theory, the stochastic beta-relaxation theory.

Item URL in elib:https://elib.dlr.de/190254/
Document Type:Article
Title:Nonmonotonic Dynamical Correlations beneath the Surface of Glass-Forming Liquids
Authors:
AuthorsInstitution or Email of AuthorsAuthor's ORCID iDORCID Put Code
Peng, H.UNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Liu, HuashanUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Voigtmann, ThomasUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Date:16 November 2022
Journal or Publication Title:Physical Review Letters
Refereed publication:Yes
Open Access:Yes
Gold Open Access:No
In SCOPUS:Yes
In ISI Web of Science:Yes
Volume:129
DOI:10.1103/PhysRevLett.129.215501
Page Range:p. 215501
Publisher:American Physical Society
ISSN:0031-9007
Status:Published
Keywords:glass transition; thin films; surfaces; dynamical correlation length
HGF - Research field:Aeronautics, Space and Transport
HGF - Program:Space
HGF - Program Themes:Research under Space Conditions
DLR - Research area:Raumfahrt
DLR - Program:R FR - Research under Space Conditions
DLR - Research theme (Project):R - Material Design and New Materials
Location: Köln-Porz
Institutes and Institutions:Institute of Materials Physics in Space
Deposited By: Voigtmann, Dr.rer.nat. Thomas
Deposited On:28 Nov 2022 07:31
Last Modified:19 Oct 2023 11:27

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