Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite

8 pags., 2 figs., 1 tab.-- Published as part of the special collection of articles derived from the 11th Congress on Electronic Structure: Principles and Applications (ESPA-2018)

Detalhes bibliográficos
Autores: Colmenero, Francisco, Cobos, Joaquín, Timón, Vicente
Tipo de documento: artigo
Estado:Versión aceptada para publicación
Data de publicação:2019
País:España
Recursos:Consejo Superior de Investigaciones Científicas (CSIC)
Repositório:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:dnet:digitalcsic_::c019203ba5b56cf81d206af3924046c9
Acesso em linha:http://hdl.handle.net/10261/208212
Access Level:Acceso aberto
Palavra-chave:Spent nuclear fuel
Becquerelite
Density functional theory
Raman spectroscopy
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spelling Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquereliteColmenero, FranciscoCobos, JoaquínTimón, VicenteSpent nuclear fuelBecquereliteDensity functional theoryRaman spectroscopy8 pags., 2 figs., 1 tab.-- Published as part of the special collection of articles derived from the 11th Congress on Electronic Structure: Principles and Applications (ESPA-2018)Raman spectroscopy is one of the main analytic techniques used to identify uranyl-containing minerals. However, the assignment of the Raman spectra of these minerals is usually performed by using empirical arguments leading to unreliable assignments. In this paper, the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite, Ca(UO2)6O4(OH)6·8H2O, was studied by means of rigorous theoretical solid-state calculations. The computations were carried out using periodic density functional theory with plane waves and pseudopotentials. The theoretical determination of this Raman spectrum was possible due to the previous development of a high-quality norm-conserving relativistic pseudopotential specific for the uranium atom and the recent optimization of the full crystal structure of this mineral, including the position of all hydrogen atoms in the corresponding unit cell. These two pieces of knowledge were formerly used in order to study the structural, mechanical, and thermodynamic properties of this mineral, but due to the very large size of the unit cell, the determination of the vibrational spectra was not possible. The corresponding results for the Raman spectrum, resulting from an intensive computational work, are reported here. The calculated Raman spectrum was compared with the experimental spectrum, and the results were found to be in very good agreement. Therefore, a normal mode analysis of the theoretical spectra was performed to assign the main bands of the Raman spectrum. This assignment improved significantly the current empirical assignment of the bands of the Raman spectrum of becquerelite mineral.s Supercomputer time by the CTI-CSIC center is greatly acknowledged. This work has been carried out in the context of a CSIC–CIEMAT collaboration agreement: “Caracterización experimental y teórica de fases secundarias y óxidos de uranio formados en condiciones de almacenamiento de combustible nuclear.” VT acknowledges the support of the Ministry of Science, Innovation and Universities under project FIS2016-77726-C3-1-CP.Springer NatureCSIC - Centro Técnico de Informática (CTI)Consejo Superior de Investigaciones Científicas (España)Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas (España)Ministerio de Economía y Competitividad (España)Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]2020202020192020info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/208212reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/FIS2016-77726-C3-1-Phttp://dx.doi.org/10.1007/s00214-019-2437-ySíinfo:eu-repo/semantics/openAccessoai:dnet:digitalcsic_::c019203ba5b56cf81d206af3924046c92026-05-22T06:33:51Z
dc.title.none.fl_str_mv Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite
title Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite
spellingShingle Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite
Colmenero, Francisco
Spent nuclear fuel
Becquerelite
Density functional theory
Raman spectroscopy
title_short Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite
title_full Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite
title_fullStr Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite
title_full_unstemmed Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite
title_sort Periodic density functional theory study of the Raman spectrum of the hydrated uranyl oxyhydroxide mineral becquerelite
dc.creator.none.fl_str_mv Colmenero, Francisco
Cobos, Joaquín
Timón, Vicente
author Colmenero, Francisco
author_facet Colmenero, Francisco
Cobos, Joaquín
Timón, Vicente
author_role author
author2 Cobos, Joaquín
Timón, Vicente
author2_role author
author
dc.contributor.none.fl_str_mv CSIC - Centro Técnico de Informática (CTI)
Consejo Superior de Investigaciones Científicas (España)
Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas (España)
Ministerio de Economía y Competitividad (España)
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Spent nuclear fuel
Becquerelite
Density functional theory
Raman spectroscopy
topic Spent nuclear fuel
Becquerelite
Density functional theory
Raman spectroscopy
description 8 pags., 2 figs., 1 tab.-- Published as part of the special collection of articles derived from the 11th Congress on Electronic Structure: Principles and Applications (ESPA-2018)
publishDate 2019
dc.date.none.fl_str_mv 2019
2020
2020
2020
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Postprint
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/208212
url http://hdl.handle.net/10261/208212
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/FIS2016-77726-C3-1-P
http://dx.doi.org/10.1007/s00214-019-2437-y
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Springer Nature
publisher.none.fl_str_mv Springer Nature
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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