Multicomposition EPSR: toward transferable potentials to model chalcogenide glass structures

The structure of xAs40Se60–(1 – x)As40S60 glasses, where x = 1.000, 0.667, 0.500, 0.333, 0.250, and 0.000, is investigated using a combination of neutron and X-ray diffraction coupled with computational modeling using multicomposition empirical potential structure refinement (MC-EPSR). Traditional E...

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Main Authors: Towey, James J., Barney, Emma R.
Format: Article
Published: American Chemical Society 2016
Online Access:https://eprints.nottingham.ac.uk/39455/
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author Towey, James J.
Barney, Emma R.
author_facet Towey, James J.
Barney, Emma R.
author_sort Towey, James J.
building Nottingham Research Data Repository
collection Online Access
description The structure of xAs40Se60–(1 – x)As40S60 glasses, where x = 1.000, 0.667, 0.500, 0.333, 0.250, and 0.000, is investigated using a combination of neutron and X-ray diffraction coupled with computational modeling using multicomposition empirical potential structure refinement (MC-EPSR). Traditional EPSR (T-EPSR) produces a set of empirical potentials that drive a structural model of a particular composition to agreement with diffraction experiments. The work presented here establishes the shortcomings in generating such a model for a ternary chalcogenide glass composition. In an enhancement to T-EPSR, MC-EPSR produces a set of pair potentials that generate robust structural models across a range of glass compositions. The structures obtained vary with composition in a much more systematic way than those taken from T-EPSR. For example, the average arsenic–sulfur bonding distances vary between 2.28 and 2.46 Å in T-EPSR but are 2.29 ± 0.02 Å in MC-EPSR. Similarly, the arsenic–selenium bond lengths from T-EPSR vary between 2.28 and 2.43 Å but are consistently 2.40 ± 0.02 Å in the MC-EPSR results. Analysis of these models suggests that the average separation of the chalcogen (S or Se) atoms is the structural origin of the changes in nonlinear refractive index with glass composition.
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spelling nottingham-394552020-05-04T18:27:29Z https://eprints.nottingham.ac.uk/39455/ Multicomposition EPSR: toward transferable potentials to model chalcogenide glass structures Towey, James J. Barney, Emma R. The structure of xAs40Se60–(1 – x)As40S60 glasses, where x = 1.000, 0.667, 0.500, 0.333, 0.250, and 0.000, is investigated using a combination of neutron and X-ray diffraction coupled with computational modeling using multicomposition empirical potential structure refinement (MC-EPSR). Traditional EPSR (T-EPSR) produces a set of empirical potentials that drive a structural model of a particular composition to agreement with diffraction experiments. The work presented here establishes the shortcomings in generating such a model for a ternary chalcogenide glass composition. In an enhancement to T-EPSR, MC-EPSR produces a set of pair potentials that generate robust structural models across a range of glass compositions. The structures obtained vary with composition in a much more systematic way than those taken from T-EPSR. For example, the average arsenic–sulfur bonding distances vary between 2.28 and 2.46 Å in T-EPSR but are 2.29 ± 0.02 Å in MC-EPSR. Similarly, the arsenic–selenium bond lengths from T-EPSR vary between 2.28 and 2.43 Å but are consistently 2.40 ± 0.02 Å in the MC-EPSR results. Analysis of these models suggests that the average separation of the chalcogen (S or Se) atoms is the structural origin of the changes in nonlinear refractive index with glass composition. American Chemical Society 2016-12-06 Article PeerReviewed Towey, James J. and Barney, Emma R. (2016) Multicomposition EPSR: toward transferable potentials to model chalcogenide glass structures. Journal of Physical Chemistry B . ISSN 1520-5207 http://pubs.acs.org/doi/abs/10.1021/acs.jpcb.6b08793 doi:10.1021/acs.jpcb.6b08793 doi:10.1021/acs.jpcb.6b08793
spellingShingle Towey, James J.
Barney, Emma R.
Multicomposition EPSR: toward transferable potentials to model chalcogenide glass structures
title Multicomposition EPSR: toward transferable potentials to model chalcogenide glass structures
title_full Multicomposition EPSR: toward transferable potentials to model chalcogenide glass structures
title_fullStr Multicomposition EPSR: toward transferable potentials to model chalcogenide glass structures
title_full_unstemmed Multicomposition EPSR: toward transferable potentials to model chalcogenide glass structures
title_short Multicomposition EPSR: toward transferable potentials to model chalcogenide glass structures
title_sort multicomposition epsr: toward transferable potentials to model chalcogenide glass structures
url https://eprints.nottingham.ac.uk/39455/
https://eprints.nottingham.ac.uk/39455/
https://eprints.nottingham.ac.uk/39455/