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Title: Chain Breakage in the Supercooled Liquid - Liquid Transition and Re-entry of the λ-transition in Sulfur

Amorphous sulfur was prepared by rapid compression of liquid sulfur at temperatures above the λ-transition for to preserve the high-temperature liquid structure. We conducted synchrotron highenergy X-ray diffraction and Raman spectroscopy to diagnose the structural evolution of amorphous sulfur from room temperature to post-λ-transition temperature. Discontinuous changes of the first and second peaks in atomic pair-distribution-function, g(r), were observed during the transition from amorphous to liquid sulfur. The average first-neighbor coordination numbers showed an abrupt drop from 1.92 to 1.81. The evolution of the chain length clearly shows that the transition was accompanied by polymeric chains breaking. Furthermore, a re-entry of the λ-transition structure was involved in the heating process. The amorphous sulfur, which inherits the post-λ-transition structure from its parent melts, transformed to the pre-λ-transition liquid structure at around 391 K. Upon further heating, the pre-λ-transition liquid transformed to a post-λ-transition structure through the wellknown λ-transition process. Furthermore, this discovery offers a new perspective on amorphous sulfur’s structural inheritance from its parent liquid and has implications for understanding the structure, evolution and properties of amorphous sulfur and its liquids.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [3] ;  [3] ;  [3] ;  [3] ;  [4]
  1. Southwest Jiaotong Univ., Chengdu (China); Center for High Pressure and Technology Advanced Research, Shanghai (China)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Southwest Jiaotong Univ., Chengdu (China)
  4. Center for High Pressure and Technology Advanced Research, Shanghai (China); Carnegie Inst. of Washington, Argonne, IL (United States); Florida Intl Univ., Miami, FL (United States)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
National Science Foundation of China; Fundamental Research Funds for the Central Universities; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS
OSTI Identifier:
1461349

Zhang, Linji, Ren, Yang, Liu, Xiuru, Han, Fei, Evans-Lutterodt, Kenneth, Wang, Hongyan, He, Yali, Wang, Junlong, Zhao, Yong, and Yang, Wenge. Chain Breakage in the Supercooled Liquid - Liquid Transition and Re-entry of the λ-transition in Sulfur. United States: N. p., Web. doi:10.1038/s41598-018-22775-y.
Zhang, Linji, Ren, Yang, Liu, Xiuru, Han, Fei, Evans-Lutterodt, Kenneth, Wang, Hongyan, He, Yali, Wang, Junlong, Zhao, Yong, & Yang, Wenge. Chain Breakage in the Supercooled Liquid - Liquid Transition and Re-entry of the λ-transition in Sulfur. United States. doi:10.1038/s41598-018-22775-y.
Zhang, Linji, Ren, Yang, Liu, Xiuru, Han, Fei, Evans-Lutterodt, Kenneth, Wang, Hongyan, He, Yali, Wang, Junlong, Zhao, Yong, and Yang, Wenge. 2018. "Chain Breakage in the Supercooled Liquid - Liquid Transition and Re-entry of the λ-transition in Sulfur". United States. doi:10.1038/s41598-018-22775-y. https://www.osti.gov/servlets/purl/1461349.
@article{osti_1461349,
title = {Chain Breakage in the Supercooled Liquid - Liquid Transition and Re-entry of the λ-transition in Sulfur},
author = {Zhang, Linji and Ren, Yang and Liu, Xiuru and Han, Fei and Evans-Lutterodt, Kenneth and Wang, Hongyan and He, Yali and Wang, Junlong and Zhao, Yong and Yang, Wenge},
abstractNote = {Amorphous sulfur was prepared by rapid compression of liquid sulfur at temperatures above the λ-transition for to preserve the high-temperature liquid structure. We conducted synchrotron highenergy X-ray diffraction and Raman spectroscopy to diagnose the structural evolution of amorphous sulfur from room temperature to post-λ-transition temperature. Discontinuous changes of the first and second peaks in atomic pair-distribution-function, g(r), were observed during the transition from amorphous to liquid sulfur. The average first-neighbor coordination numbers showed an abrupt drop from 1.92 to 1.81. The evolution of the chain length clearly shows that the transition was accompanied by polymeric chains breaking. Furthermore, a re-entry of the λ-transition structure was involved in the heating process. The amorphous sulfur, which inherits the post-λ-transition structure from its parent melts, transformed to the pre-λ-transition liquid structure at around 391 K. Upon further heating, the pre-λ-transition liquid transformed to a post-λ-transition structure through the wellknown λ-transition process. Furthermore, this discovery offers a new perspective on amorphous sulfur’s structural inheritance from its parent liquid and has implications for understanding the structure, evolution and properties of amorphous sulfur and its liquids.},
doi = {10.1038/s41598-018-22775-y},
journal = {Scientific Reports},
number = 1,
volume = 8,
place = {United States},
year = {2018},
month = {3}
}

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