Interplay of Coordination Environment and Magnetic Behavior of Layered Co(II) Hydroxichlorides: A DFT+U Study

In this work we present a systematic computational study of the structural and magnetic properties of a layered family of Co(II) hydroxichlorides, obeying to the general formula Co(OH)2-xClx(H2O)y. This solid contains both octahedral and tetrahedral cobalt ions, displaying a complex magnetic order a...

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Autores principales:	Hunt, D., Jobbagy, M., Scherlis, D.A.
Formato:	JOUR
Acceso en línea:	http://hdl.handle.net/20.500.12110/paper_00201669_v57_n9_p4989_Hunt
Aporte de:	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) de Universidad de Buenos Aires

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spelling	todo:paper_00201669_v57_n9_p4989_Hunt2023-10-03T14:17:11Z Interplay of Coordination Environment and Magnetic Behavior of Layered Co(II) Hydroxichlorides: A DFT+U Study Hunt, D. Jobbagy, M. Scherlis, D.A. In this work we present a systematic computational study of the structural and magnetic properties of a layered family of Co(II) hydroxichlorides, obeying to the general formula Co(OH)2-xClx(H2O)y. This solid contains both octahedral and tetrahedral cobalt ions, displaying a complex magnetic order arising from the particular coupling between the two kinds of metallic centers. Here, supercells representing concentrations of 12, 20, and 40% of tetrahedral sites were modeled consistently with the compositions reported experimentally. Our simulations show that the two types of cobalt ions tend to couple antiferromagnetically, giving rise to a net magnetic moment slightly out of the plane of the layers. The band gap reaches its minimum value of 1.4 eV for the most diluted fraction of tetrahedral Co(II) sites, going up to 2.2 eV when the content is 40%. Moreover, our results suggest that the presence of interlayer water stabilizes the material and at the same time strongly modifies the electronic environment of tetrahedral Co(II), leading to a further drop of the band gap. To our knowledge, this is the first theoretical investigation of this material. © 2018 American Chemical Society. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_00201669_v57_n9_p4989_Hunt
institution	Universidad de Buenos Aires
institution_str	I-28
repository_str	R-134
collection	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA)
description	In this work we present a systematic computational study of the structural and magnetic properties of a layered family of Co(II) hydroxichlorides, obeying to the general formula Co(OH)2-xClx(H2O)y. This solid contains both octahedral and tetrahedral cobalt ions, displaying a complex magnetic order arising from the particular coupling between the two kinds of metallic centers. Here, supercells representing concentrations of 12, 20, and 40% of tetrahedral sites were modeled consistently with the compositions reported experimentally. Our simulations show that the two types of cobalt ions tend to couple antiferromagnetically, giving rise to a net magnetic moment slightly out of the plane of the layers. The band gap reaches its minimum value of 1.4 eV for the most diluted fraction of tetrahedral Co(II) sites, going up to 2.2 eV when the content is 40%. Moreover, our results suggest that the presence of interlayer water stabilizes the material and at the same time strongly modifies the electronic environment of tetrahedral Co(II), leading to a further drop of the band gap. To our knowledge, this is the first theoretical investigation of this material. © 2018 American Chemical Society.
format	JOUR
author	Hunt, D. Jobbagy, M. Scherlis, D.A.
spellingShingle	Hunt, D. Jobbagy, M. Scherlis, D.A. Interplay of Coordination Environment and Magnetic Behavior of Layered Co(II) Hydroxichlorides: A DFT+U Study
author_facet	Hunt, D. Jobbagy, M. Scherlis, D.A.
author_sort	Hunt, D.
title	Interplay of Coordination Environment and Magnetic Behavior of Layered Co(II) Hydroxichlorides: A DFT+U Study
title_short	Interplay of Coordination Environment and Magnetic Behavior of Layered Co(II) Hydroxichlorides: A DFT+U Study
title_full	Interplay of Coordination Environment and Magnetic Behavior of Layered Co(II) Hydroxichlorides: A DFT+U Study
title_fullStr	Interplay of Coordination Environment and Magnetic Behavior of Layered Co(II) Hydroxichlorides: A DFT+U Study
title_full_unstemmed	Interplay of Coordination Environment and Magnetic Behavior of Layered Co(II) Hydroxichlorides: A DFT+U Study
title_sort	interplay of coordination environment and magnetic behavior of layered co(ii) hydroxichlorides: a dft+u study
url	http://hdl.handle.net/20.500.12110/paper_00201669_v57_n9_p4989_Hunt
work_keys_str_mv	AT huntd interplayofcoordinationenvironmentandmagneticbehavioroflayeredcoiihydroxichloridesadftustudy AT jobbagym interplayofcoordinationenvironmentandmagneticbehavioroflayeredcoiihydroxichloridesadftustudy AT scherlisda interplayofcoordinationenvironmentandmagneticbehavioroflayeredcoiihydroxichloridesadftustudy
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Interplay of Coordination Environment and Magnetic Behavior of Layered Co(II) Hydroxichlorides: A DFT+U Study

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