skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Origin of structural analogies and differences between the atomic structures of GeSe{sub 4} and GeS{sub 4} glasses: A first principles study

Abstract

First-principles molecular dynamics simulations based on density functional theory are employed for a comparative study of structural and bonding properties of two stoichiometrically identical chalcogenide glasses, GeSe{sub 4} and GeS{sub 4}. Two periodic cells of 120 and 480 atoms are adopted. Both glasses feature a coexistence of Ge-centered tetrahedra and Se(S) homopolar connections. Results obtained for N = 480 indicate substantial differences at the level of the Se(S) environment, since Ge–Se–Se connections are more frequent than the corresponding Ge–S–S ones. The presence of a more prominent first sharp diffraction peak in the total neutron structure factor of glassy GeS{sub 4} is rationalized in terms of a higher number of large size rings, accounting for extended Ge–Se correlations. Both the electronic density of states and appropriate electronic localization tools provide evidence of a higher ionic character of Ge–S bonds when compared to Ge–Se bonds. An interesting byproduct of these investigations is the occurrence of discernible size effects that affect structural motifs involving next nearest neighbor distances, when 120 or 480 atoms are used.

Authors:
; ; ; ;  [1]
  1. Institut de Physique et de Chimie des Matériaux de Strasbourg, Université de Strasbourg and CNRS UMR 7504, 23 rue du Loess, BP43, F-67034 Strasbourg Cedex 2 (France)
Publication Date:
OSTI Identifier:
22489729
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 3; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; BONDING; COMPARATIVE EVALUATIONS; DENSITY FUNCTIONAL METHOD; DENSITY OF STATES; DIFFRACTION; GERMANIUM SELENIDES; GERMANIUM SULFIDES; GLASS; MOLECULAR DYNAMICS METHOD; NEUTRONS; PEAKS; SIMULATION; STRUCTURE FACTORS

Citation Formats

Bouzid, Assil, Le Roux, Sébastien, Ori, Guido, Boero, Mauro, and Massobrio, Carlo. Origin of structural analogies and differences between the atomic structures of GeSe{sub 4} and GeS{sub 4} glasses: A first principles study. United States: N. p., 2015. Web. doi:10.1063/1.4926830.
Bouzid, Assil, Le Roux, Sébastien, Ori, Guido, Boero, Mauro, & Massobrio, Carlo. Origin of structural analogies and differences between the atomic structures of GeSe{sub 4} and GeS{sub 4} glasses: A first principles study. United States. https://doi.org/10.1063/1.4926830
Bouzid, Assil, Le Roux, Sébastien, Ori, Guido, Boero, Mauro, and Massobrio, Carlo. 2015. "Origin of structural analogies and differences between the atomic structures of GeSe{sub 4} and GeS{sub 4} glasses: A first principles study". United States. https://doi.org/10.1063/1.4926830.
@article{osti_22489729,
title = {Origin of structural analogies and differences between the atomic structures of GeSe{sub 4} and GeS{sub 4} glasses: A first principles study},
author = {Bouzid, Assil and Le Roux, Sébastien and Ori, Guido and Boero, Mauro and Massobrio, Carlo},
abstractNote = {First-principles molecular dynamics simulations based on density functional theory are employed for a comparative study of structural and bonding properties of two stoichiometrically identical chalcogenide glasses, GeSe{sub 4} and GeS{sub 4}. Two periodic cells of 120 and 480 atoms are adopted. Both glasses feature a coexistence of Ge-centered tetrahedra and Se(S) homopolar connections. Results obtained for N = 480 indicate substantial differences at the level of the Se(S) environment, since Ge–Se–Se connections are more frequent than the corresponding Ge–S–S ones. The presence of a more prominent first sharp diffraction peak in the total neutron structure factor of glassy GeS{sub 4} is rationalized in terms of a higher number of large size rings, accounting for extended Ge–Se correlations. Both the electronic density of states and appropriate electronic localization tools provide evidence of a higher ionic character of Ge–S bonds when compared to Ge–Se bonds. An interesting byproduct of these investigations is the occurrence of discernible size effects that affect structural motifs involving next nearest neighbor distances, when 120 or 480 atoms are used.},
doi = {10.1063/1.4926830},
url = {https://www.osti.gov/biblio/22489729}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 3,
volume = 143,
place = {United States},
year = {Tue Jul 21 00:00:00 EDT 2015},
month = {Tue Jul 21 00:00:00 EDT 2015}
}