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Title: Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid

Abstract

Onset of cooperative dynamics has been observed in many molecular liquids, colloids, and granular materials in the metastable regime on approaching their respective glass or jamming transition points, and is considered to play a significant role in the emergence of the slow dynamics. However, the nature of such dynamical cooperativity remains elusive in multicomponent metallic liquids characterized by complex many-body interactions and high mixing entropy. Herein, we report evidence of onset of cooperative dynamics in an equilibrium glass-forming metallic liquid (LM601: Zr51Cu36Ni4Al9). This is revealed by deviation of the mean effective diffusion coefficient from its high-temperature Arrhenius behavior below TA ≈ 1300 K, i.e., a crossover from uncorrelated dynamics above TA to landscape-influenced correlated dynamics below TA. Moreover, the onset/ crossover temperature TA in such a multicomponent bulk metallic glass-forming liquid is observed at approximately twice of its calorimetric glass transition temperature (Tg ≈ 697 K) and in its stable liquid phase, unlike many molecular liquids.

Authors:
 [1];  [2];  [3];  [3];  [3];  [4];  [4];  [2];  [4];  [5]
+ Show Author Affiliations
  1. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States). Dept. of Nuclear, Plasma and Radiological Engineering
  2. Liquidmetal Technologies Inc., Santa Margarita, CA (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
  4. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering, Dept. of Physics and Astronomy
  5. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States). Dept. of Nuclear, Plasma and Radiological Engineering; Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1328272
Grant/Contract Number:  
AC05-00OR22725; SC0014804
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 120; Journal Issue: 6; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Jaiswal, Abhishek, O’Keeffe, Stephanie, Mills, Rebecca, Podlesynak, Andrey, Ehlers, Georg, Dmowski, Wojciech, Lokshin, Konstantin, Stevick, Joseph, Egami, Takeshi, and Zhang, Yang. Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid. United States: N. p., 2016. Web. doi:10.1021/acs.jpcb.5b11452.
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Jaiswal, Abhishek, O’Keeffe, Stephanie, Mills, Rebecca, Podlesynak, Andrey, Ehlers, Georg, Dmowski, Wojciech, Lokshin, Konstantin, Stevick, Joseph, Egami, Takeshi, & Zhang, Yang. Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid. United States. https://doi.org/10.1021/acs.jpcb.5b11452
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Jaiswal, Abhishek, O’Keeffe, Stephanie, Mills, Rebecca, Podlesynak, Andrey, Ehlers, Georg, Dmowski, Wojciech, Lokshin, Konstantin, Stevick, Joseph, Egami, Takeshi, and Zhang, Yang. Fri . "Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid". United States. https://doi.org/10.1021/acs.jpcb.5b11452. https://www.osti.gov/servlets/purl/1328272.
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@article{osti_1328272,
title = {Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid},
author = {Jaiswal, Abhishek and O’Keeffe, Stephanie and Mills, Rebecca and Podlesynak, Andrey and Ehlers, Georg and Dmowski, Wojciech and Lokshin, Konstantin and Stevick, Joseph and Egami, Takeshi and Zhang, Yang},
abstractNote = {Onset of cooperative dynamics has been observed in many molecular liquids, colloids, and granular materials in the metastable regime on approaching their respective glass or jamming transition points, and is considered to play a significant role in the emergence of the slow dynamics. However, the nature of such dynamical cooperativity remains elusive in multicomponent metallic liquids characterized by complex many-body interactions and high mixing entropy. Herein, we report evidence of onset of cooperative dynamics in an equilibrium glass-forming metallic liquid (LM601: Zr51Cu36Ni4Al9). This is revealed by deviation of the mean effective diffusion coefficient from its high-temperature Arrhenius behavior below TA ≈ 1300 K, i.e., a crossover from uncorrelated dynamics above TA to landscape-influenced correlated dynamics below TA. Moreover, the onset/ crossover temperature TA in such a multicomponent bulk metallic glass-forming liquid is observed at approximately twice of its calorimetric glass transition temperature (Tg ≈ 697 K) and in its stable liquid phase, unlike many molecular liquids.},
doi = {10.1021/acs.jpcb.5b11452},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 6,
volume = 120,
place = {United States},
year = {Fri Jan 22 00:00:00 EST 2016},
month = {Fri Jan 22 00:00:00 EST 2016}
}
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https://doi.org/10.1021/acs.jpcb.5b11452
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