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Title: Dynamics at the crystal-melt interface in a supercooled chalcogenide liquid near the glass transition

Abstract

Direct quantitative measurements of nanoscale dynamical processes associated with structural relaxation and crystallization near the glass transition are a major experimental challenge. These type of processes have been primarily treated as macroscopic phenomena within the framework of phenomenological models and bulk experiments. Here, we report x-ray photon correlation spectroscopy measurements of dynamics at the crystal-melt interface during the radiation induced formation of Se nano-crystallites in pure Se and in binary AsSe4 glass-forming liquids near their glass transition temperature. We observe a heterogeneous dynamical behaviour where the intensity correlation functions g2(q, t) exhibits either a compressed or a stretched exponential decay, depending on the size of the Se nano-crystallites. The corresponding relaxation timescale for the AsSe4 liquid increases as the temperature is raised, which can be attributed to changes in the chemical composition of the melt at the crystal-melt interface with the growth of the Se nano-crystallites.

Authors:
 [1];  [1];  [1];  [1];  [2];  [2];  [1];  [1]
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  1. Univ. of California, Davis, CA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1656447
Report Number(s):
BNL-216312-2020-JAAM
Journal ID: ISSN 2045-2322
Grant/Contract Number:  
SC0012704; DMR 1855176; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Li, Jianheng, Jangid, Rahul, Zhu, Weidi, Kohne, Chris, Fluerasu, Andrei, Zhang, Yugang, Sen, Sabyasachi, and Kukreja, Roopali. Dynamics at the crystal-melt interface in a supercooled chalcogenide liquid near the glass transition. United States: N. p., 2020. Web. doi:10.1038/s41598-020-62783-5.
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Li, Jianheng, Jangid, Rahul, Zhu, Weidi, Kohne, Chris, Fluerasu, Andrei, Zhang, Yugang, Sen, Sabyasachi, & Kukreja, Roopali. Dynamics at the crystal-melt interface in a supercooled chalcogenide liquid near the glass transition. United States. https://doi.org/10.1038/s41598-020-62783-5
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Li, Jianheng, Jangid, Rahul, Zhu, Weidi, Kohne, Chris, Fluerasu, Andrei, Zhang, Yugang, Sen, Sabyasachi, and Kukreja, Roopali. Fri . "Dynamics at the crystal-melt interface in a supercooled chalcogenide liquid near the glass transition". United States. https://doi.org/10.1038/s41598-020-62783-5. https://www.osti.gov/servlets/purl/1656447.
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@article{osti_1656447,
title = {Dynamics at the crystal-melt interface in a supercooled chalcogenide liquid near the glass transition},
author = {Li, Jianheng and Jangid, Rahul and Zhu, Weidi and Kohne, Chris and Fluerasu, Andrei and Zhang, Yugang and Sen, Sabyasachi and Kukreja, Roopali},
abstractNote = {Direct quantitative measurements of nanoscale dynamical processes associated with structural relaxation and crystallization near the glass transition are a major experimental challenge. These type of processes have been primarily treated as macroscopic phenomena within the framework of phenomenological models and bulk experiments. Here, we report x-ray photon correlation spectroscopy measurements of dynamics at the crystal-melt interface during the radiation induced formation of Se nano-crystallites in pure Se and in binary AsSe4 glass-forming liquids near their glass transition temperature. We observe a heterogeneous dynamical behaviour where the intensity correlation functions g2(q, t) exhibits either a compressed or a stretched exponential decay, depending on the size of the Se nano-crystallites. The corresponding relaxation timescale for the AsSe4 liquid increases as the temperature is raised, which can be attributed to changes in the chemical composition of the melt at the crystal-melt interface with the growth of the Se nano-crystallites.},
doi = {10.1038/s41598-020-62783-5},
journal = {Scientific Reports},
number = 1,
volume = 10,
place = {United States},
year = {Fri Apr 03 00:00:00 EDT 2020},
month = {Fri Apr 03 00:00:00 EDT 2020}
}
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https://doi.org/10.1038/s41598-020-62783-5
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