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Title: Experimental and Theoretical Insights into the Structure of Tellurium Chloride Glasses

Here, the structure of the binary chalcohalide glasses Te 1-xCL x (0.35 <= x <= 0.65) is considered by combining experimental and theoretical results. The structural network properties are influenced by a competition between ionic and covalent bonding in such glasses. At first, a focus is placed on the detailed information available by using the complementary high-energy X-ray and the neutron diffractions in both the reciprocal and real spaces. The main characteristic suggested by the structure factors S(Q) concerns the presence of three length scales in the intermediate range order. The total correlation function T(r) lets us also suppose that the structure of these glasses is more complicated than Te-chain fragments with terminal Cl as demonstrated in crystalline Te 3Cl 2. Molecular dynamics simulations were subsequently performed on Te 3Cl 2 and Te 2Cl 3, and coupled with the experimental data, a highly reticulated network of chalcogen atoms, with a fair amount of chlorine atoms bonded in a bridging mode, is proposed. The simulations clearly lead to a glass description that differs markedly from the simple structural model based on only Te atom chains and terminal Cl atoms. Solidstate NMR experiments and NMR parameters calculations allowed validation of the presencemore » of Te highly coordinated with chlorine in these glasses.« less
Authors:
 [1] ; ORCiD logo [1] ;  [2] ;  [1] ;  [3] ;  [4] ;  [5] ;  [6]
  1. Univ. of Rennes, UMR 6226 CNRS (France). National School of Chemistry of Rennes and Inst. of Chemical Sciences Rennes (ISCR)
  2. Univ. of Rennes, UMR 6226 CNRS (France). National School of Chemistry of Rennes, Inst. of Chemical Sciences Rennes (ISCR) and Glass and Ceramics Team
  3. National Inst. for Materials Science (NIMS), Tsukuba (Japan). Synchrotron X-ray Group and Light/Quantum Beam Field Research Center for Advanced Measurement and Characterization
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS) and X-ray Science Division
  5. Univ. of the Littoral Opal Coast, Dunkirk (France). Lab. of Physico-Chemistry of the Atmosphere
  6. Univ. of Rennes, UMR 6226 CNRS (France). Inst. of Chemical Sciences Rennes (ISCR) and Glass and Ceramics Team
Publication Date:
Grant/Contract Number:
AC02-06CH11357; AC02-06CH1135; 2011B1565; 2016-086045
Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry
Additional Journal Information:
Journal Volume: 57; Journal Issue: 5; Journal ID: ISSN 0020-1669
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Japan Synchrotron Radiation Research Inst. (JASRI), Hyogo (Japan); Large Intensive National Calculation Equipment (GENCI), Paris (France)
Contributing Orgs:
CEA-Saclay Centre, Gif-sur-Yvette (France). Leon Brillouin Lab. (LLB)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
OSTI Identifier:
1462748

Bouessel Du Bourg, Lila, Furet, Eric, Lecomte, Alicia, Le Polles, Laurent, Kohara, Shinji, Benmore, Chris J., Bychkov, Eugene, and Le Coq, David. Experimental and Theoretical Insights into the Structure of Tellurium Chloride Glasses. United States: N. p., Web. doi:10.1021/acs.inorgchem.7b02868.
Bouessel Du Bourg, Lila, Furet, Eric, Lecomte, Alicia, Le Polles, Laurent, Kohara, Shinji, Benmore, Chris J., Bychkov, Eugene, & Le Coq, David. Experimental and Theoretical Insights into the Structure of Tellurium Chloride Glasses. United States. doi:10.1021/acs.inorgchem.7b02868.
Bouessel Du Bourg, Lila, Furet, Eric, Lecomte, Alicia, Le Polles, Laurent, Kohara, Shinji, Benmore, Chris J., Bychkov, Eugene, and Le Coq, David. 2018. "Experimental and Theoretical Insights into the Structure of Tellurium Chloride Glasses". United States. doi:10.1021/acs.inorgchem.7b02868.
@article{osti_1462748,
title = {Experimental and Theoretical Insights into the Structure of Tellurium Chloride Glasses},
author = {Bouessel Du Bourg, Lila and Furet, Eric and Lecomte, Alicia and Le Polles, Laurent and Kohara, Shinji and Benmore, Chris J. and Bychkov, Eugene and Le Coq, David},
abstractNote = {Here, the structure of the binary chalcohalide glasses Te1-xCLx (0.35 <= x <= 0.65) is considered by combining experimental and theoretical results. The structural network properties are influenced by a competition between ionic and covalent bonding in such glasses. At first, a focus is placed on the detailed information available by using the complementary high-energy X-ray and the neutron diffractions in both the reciprocal and real spaces. The main characteristic suggested by the structure factors S(Q) concerns the presence of three length scales in the intermediate range order. The total correlation function T(r) lets us also suppose that the structure of these glasses is more complicated than Te-chain fragments with terminal Cl as demonstrated in crystalline Te3Cl2. Molecular dynamics simulations were subsequently performed on Te3Cl2 and Te2Cl3, and coupled with the experimental data, a highly reticulated network of chalcogen atoms, with a fair amount of chlorine atoms bonded in a bridging mode, is proposed. The simulations clearly lead to a glass description that differs markedly from the simple structural model based on only Te atom chains and terminal Cl atoms. Solidstate NMR experiments and NMR parameters calculations allowed validation of the presence of Te highly coordinated with chlorine in these glasses.},
doi = {10.1021/acs.inorgchem.7b02868},
journal = {Inorganic Chemistry},
number = 5,
volume = 57,
place = {United States},
year = {2018},
month = {2}
}