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Title: Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy

Abstract

Supercooled liquids exhibit spatial heterogeneity in the dynamics of their fluctuating atomic arrangements. The length and time scales of the heterogeneous dynamics are central to the glass transition and influence nucleation and growth of crystals from the liquid. In this work, we report direct experimental visualization of the spatially heterogeneous dynamics as a function of temperature in the supercooled liquid state of a Pt-based metallic glass, using electron correlation microscopy with sub-nanometer resolution. An experimental four-point space-time correlation function demonstrates a growing dynamic correlation length, ξ, upon cooling of the liquid toward the glass transition temperature. ξ as a function of the relaxation time τ are in good agreement with Adam-Gibbs theory, inhomogeneous mode-coupling theory and random first-order transition theory of the glass transition. The same experiments demonstrate the existence of a nanometer thickness near-surface layer with order of magnitude shorter relaxation time than inside the bulk.

Authors:
 [1]; ORCiD logo [1];  [2];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Wisconsin, Madison, WI (United States)
  2. Yale Univ., New Haven, CT (United States)
Publication Date:
Research Org.:
Yale Univ., New Haven, CT (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1526297
Grant/Contract Number:  
SC0004889; DMR-1121288; DMR-1506564
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Zhang, Pei, Maldonis, Jason J., Liu, Ze, Schroers, Jan, and Voyles, Paul M. Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy. United States: N. p., 2018. Web. doi:10.1038/s41467-018-03604-2.
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Zhang, Pei, Maldonis, Jason J., Liu, Ze, Schroers, Jan, & Voyles, Paul M. Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy. United States. https://doi.org/10.1038/s41467-018-03604-2
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Zhang, Pei, Maldonis, Jason J., Liu, Ze, Schroers, Jan, and Voyles, Paul M. Mon . "Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy". United States. https://doi.org/10.1038/s41467-018-03604-2. https://www.osti.gov/servlets/purl/1526297.
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@article{osti_1526297,
title = {Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy},
author = {Zhang, Pei and Maldonis, Jason J. and Liu, Ze and Schroers, Jan and Voyles, Paul M.},
abstractNote = {Supercooled liquids exhibit spatial heterogeneity in the dynamics of their fluctuating atomic arrangements. The length and time scales of the heterogeneous dynamics are central to the glass transition and influence nucleation and growth of crystals from the liquid. In this work, we report direct experimental visualization of the spatially heterogeneous dynamics as a function of temperature in the supercooled liquid state of a Pt-based metallic glass, using electron correlation microscopy with sub-nanometer resolution. An experimental four-point space-time correlation function demonstrates a growing dynamic correlation length, ξ, upon cooling of the liquid toward the glass transition temperature. ξ as a function of the relaxation time τ are in good agreement with Adam-Gibbs theory, inhomogeneous mode-coupling theory and random first-order transition theory of the glass transition. The same experiments demonstrate the existence of a nanometer thickness near-surface layer with order of magnitude shorter relaxation time than inside the bulk.},
doi = {10.1038/s41467-018-03604-2},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Mon Mar 19 00:00:00 EDT 2018},
month = {Mon Mar 19 00:00:00 EDT 2018}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41467-018-03604-2
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Cited by: 70 works
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Figures / Tables:

Fig. 1 Fig. 1: Tilted dark-field electron correlation microscopy. a Schematic of the experiment. Tilted illumination shifts the transmitted beam off the optic axis of a microscope. A small, on-axis objective aperture selects one speckle in the diffraction pattern, forming a real-space image. Structural rearrangements cause fluctuations in the intensity of themore » image speckles. A time series of ~4000 dark-field images is recorded and then aligned to correct drift of the sample. b The time autocorrelation function $g$2($t$) is calculated from the intensity time series at every pixel, then fit to the KWW equation to extract the relaxation time $τ$ and stretching parameter $β$. The figure shows a typical $g$2($t$, which is well converged. This calculation is repeated for every pixel in the image« less
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