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Intermediate Range Order in Metal–Ammonia Solutions: Pure and Na-Doped Ca-NH(3)

[Image: see text] The local and intermediate range ordering in Ca–NH(3) solutions in their metallic phase is determined through H/D isotopically differenced neutron diffraction in combination with empirical potential structure refinements. For both low and high relative Ca concentrations, the Ca ion...

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Autores principales: Nicholas, Thomas C., Headen, Thomas F., Wasse, Jonathan. C., Howard, Christopher. A., Skipper, Neal. T., Seel, Andrew G.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2021
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8389892/
https://www.ncbi.nlm.nih.gov/pubmed/34212732
http://dx.doi.org/10.1021/acs.jpcb.1c03843
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author Nicholas, Thomas C.
Headen, Thomas F.
Wasse, Jonathan. C.
Howard, Christopher. A.
Skipper, Neal. T.
Seel, Andrew G.
author_facet Nicholas, Thomas C.
Headen, Thomas F.
Wasse, Jonathan. C.
Howard, Christopher. A.
Skipper, Neal. T.
Seel, Andrew G.
author_sort Nicholas, Thomas C.
collection PubMed
description [Image: see text] The local and intermediate range ordering in Ca–NH(3) solutions in their metallic phase is determined through H/D isotopically differenced neutron diffraction in combination with empirical potential structure refinements. For both low and high relative Ca concentrations, the Ca ions are found to be octahedrally coordinated by the NH(3) solvent, and these hexammine units are spatially correlated out to lengthscales of ∼7.4–10.3 Å depending on the concentration, leading to pronounced ordering in the bulk liquid. We further demonstrate that this liquid order can be progressively disrupted by the substitution of Ca for Na, whereby a distortion of the average ion primary solvation occurs and the intermediate range ion–ion correlations are disrupted.
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spelling pubmed-83898922021-08-31 Intermediate Range Order in Metal–Ammonia Solutions: Pure and Na-Doped Ca-NH(3) Nicholas, Thomas C. Headen, Thomas F. Wasse, Jonathan. C. Howard, Christopher. A. Skipper, Neal. T. Seel, Andrew G. J Phys Chem B [Image: see text] The local and intermediate range ordering in Ca–NH(3) solutions in their metallic phase is determined through H/D isotopically differenced neutron diffraction in combination with empirical potential structure refinements. For both low and high relative Ca concentrations, the Ca ions are found to be octahedrally coordinated by the NH(3) solvent, and these hexammine units are spatially correlated out to lengthscales of ∼7.4–10.3 Å depending on the concentration, leading to pronounced ordering in the bulk liquid. We further demonstrate that this liquid order can be progressively disrupted by the substitution of Ca for Na, whereby a distortion of the average ion primary solvation occurs and the intermediate range ion–ion correlations are disrupted. American Chemical Society 2021-07-02 2021-07-15 /pmc/articles/PMC8389892/ /pubmed/34212732 http://dx.doi.org/10.1021/acs.jpcb.1c03843 Text en © 2021 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Nicholas, Thomas C.
Headen, Thomas F.
Wasse, Jonathan. C.
Howard, Christopher. A.
Skipper, Neal. T.
Seel, Andrew G.
Intermediate Range Order in Metal–Ammonia Solutions: Pure and Na-Doped Ca-NH(3)
title Intermediate Range Order in Metal–Ammonia Solutions: Pure and Na-Doped Ca-NH(3)
title_full Intermediate Range Order in Metal–Ammonia Solutions: Pure and Na-Doped Ca-NH(3)
title_fullStr Intermediate Range Order in Metal–Ammonia Solutions: Pure and Na-Doped Ca-NH(3)
title_full_unstemmed Intermediate Range Order in Metal–Ammonia Solutions: Pure and Na-Doped Ca-NH(3)
title_short Intermediate Range Order in Metal–Ammonia Solutions: Pure and Na-Doped Ca-NH(3)
title_sort intermediate range order in metal–ammonia solutions: pure and na-doped ca-nh(3)
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8389892/
https://www.ncbi.nlm.nih.gov/pubmed/34212732
http://dx.doi.org/10.1021/acs.jpcb.1c03843
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