Predicting from first principles the chemical evolution of crystalline compounds due to radioactive decay: The case of the transformation of CsCl to BaCl

In this Brief Report, we use density functional theory to predict the existence of a heretofore unobservedcrystalline compound, BaCl, and additionally predict it to be isostructural with NaCl (rocksalt). Due to the chemistry of Ba, which strongly prefers a 2+ charge state, compounds where Ba nominal...

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Main Authors: Jiang, C., Stanek, C., Marks, Nigel, Sickafus, K., Uberuaga, B.
Format: Journal Article
Published: American Physical Society 2009
Online Access:http://hdl.handle.net/20.500.11937/18123
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author Jiang, C.
Stanek, C.
Marks, Nigel
Sickafus, K.
Uberuaga, B.
author_facet Jiang, C.
Stanek, C.
Marks, Nigel
Sickafus, K.
Uberuaga, B.
author_sort Jiang, C.
building Curtin Institutional Repository
collection Online Access
description In this Brief Report, we use density functional theory to predict the existence of a heretofore unobservedcrystalline compound, BaCl, and additionally predict it to be isostructural with NaCl (rocksalt). Due to the chemistry of Ba, which strongly prefers a 2+ charge state, compounds where Ba nominally exhibits a +1 charge (e.g., BaCl) are unlikely to be synthesized via conventional solid-state approaches. However, in considering the chemical evolution of 137Cs to 137Ba via B- radioactive decay in a model nuclear waste form CsCl, we find that BaCl may be indeed relevant. The mechanical stability of this surprising structure is confirmed through examination of its elastic constants and phonon-dispersion relations. We have also analyzed the chemical bonding of rocksalt BaCl and found it to exhibit a complex mixture of ionic, metallic, and covalent characters. From our results, we demonstrate that the chemical evolution of crystalline structures due to radioactive decay may be a viable synthesis route for unforeseen materials with interesting properties.
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institution Curtin University Malaysia
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publishDate 2009
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spelling curtin-20.500.11937-181232017-02-28T01:28:38Z Predicting from first principles the chemical evolution of crystalline compounds due to radioactive decay: The case of the transformation of CsCl to BaCl Jiang, C. Stanek, C. Marks, Nigel Sickafus, K. Uberuaga, B. In this Brief Report, we use density functional theory to predict the existence of a heretofore unobservedcrystalline compound, BaCl, and additionally predict it to be isostructural with NaCl (rocksalt). Due to the chemistry of Ba, which strongly prefers a 2+ charge state, compounds where Ba nominally exhibits a +1 charge (e.g., BaCl) are unlikely to be synthesized via conventional solid-state approaches. However, in considering the chemical evolution of 137Cs to 137Ba via B- radioactive decay in a model nuclear waste form CsCl, we find that BaCl may be indeed relevant. The mechanical stability of this surprising structure is confirmed through examination of its elastic constants and phonon-dispersion relations. We have also analyzed the chemical bonding of rocksalt BaCl and found it to exhibit a complex mixture of ionic, metallic, and covalent characters. From our results, we demonstrate that the chemical evolution of crystalline structures due to radioactive decay may be a viable synthesis route for unforeseen materials with interesting properties. 2009 Journal Article http://hdl.handle.net/20.500.11937/18123 American Physical Society restricted
spellingShingle Jiang, C.
Stanek, C.
Marks, Nigel
Sickafus, K.
Uberuaga, B.
Predicting from first principles the chemical evolution of crystalline compounds due to radioactive decay: The case of the transformation of CsCl to BaCl
title Predicting from first principles the chemical evolution of crystalline compounds due to radioactive decay: The case of the transformation of CsCl to BaCl
title_full Predicting from first principles the chemical evolution of crystalline compounds due to radioactive decay: The case of the transformation of CsCl to BaCl
title_fullStr Predicting from first principles the chemical evolution of crystalline compounds due to radioactive decay: The case of the transformation of CsCl to BaCl
title_full_unstemmed Predicting from first principles the chemical evolution of crystalline compounds due to radioactive decay: The case of the transformation of CsCl to BaCl
title_short Predicting from first principles the chemical evolution of crystalline compounds due to radioactive decay: The case of the transformation of CsCl to BaCl
title_sort predicting from first principles the chemical evolution of crystalline compounds due to radioactive decay: the case of the transformation of cscl to bacl
url http://hdl.handle.net/20.500.11937/18123