H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations

We report neutron-diffraction investigations of the quasi-2D Mn-II(dca)(2)(pym)(H2O) (pym = N2C4H4) compound, where high-spin Mn-II ions are bridged by dicyanamide anions, [N(CN)(2)](-) (herein abbreviated dca). Inside the layers, Mn2+ ions are connected by single or double dca bridges. The magnetic...

Descripción completa

Detalles Bibliográficos
Autores: Gillon, Beatrice, Hammerschmied, Albert, Gukasov, Arsen, Cousson, Alain, Cauchy, Thomas, Ruiz Sabín, Eliseo, Schlueter, John A., Manson, Jamie L.
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2018
País:España
Institución:Universidad de Barcelona
Repositorio:Dipòsit Digital de la UB
OAI Identifier:oai:diposit.ub.edu:2445/154801
Acceso en línea:https://hdl.handle.net/2445/154801
Access Level:acceso abierto
Palabra clave:Lligands
Estructura cristal·lina (Sòlids)
Teoria del funcional de densitat
Propietats magnètiques
Metalls de transició
Ligands
Layer structure (Solids)
Density functionals
Magnetic properties
Transition metals
id ES_11d9f620eb06f6cc9f03bca2864fafeb
oai_identifier_str oai:diposit.ub.edu:2445/154801
network_acronym_str ES
network_name_str España
repository_id_str
spelling H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculationsGillon, BeatriceHammerschmied, AlbertGukasov, ArsenCousson, AlainCauchy, ThomasRuiz Sabín, EliseoSchlueter, John A.Manson, Jamie L.LligandsEstructura cristal·lina (Sòlids)Teoria del funcional de densitatPropietats magnètiquesMetalls de transicióLigandsLayer structure (Solids)Density functionalsMagnetic propertiesTransition metalsWe report neutron-diffraction investigations of the quasi-2D Mn-II(dca)(2)(pym)(H2O) (pym = N2C4H4) compound, where high-spin Mn-II ions are bridged by dicyanamide anions, [N(CN)(2)](-) (herein abbreviated dca). Inside the layers, Mn2+ ions are connected by single or double dca bridges. The magnetic phase diagram was established by neutron diffraction on a single crystal. In the low-field phase, the Mn-II ions are antiferromagnetically ordered in the layers, with moments nearly parallel to the c axis, and the layers are antiferromagnetically coupled. The spin-flop phase corresponds to ferromagnetic coupling between the antiferromagnetic layers, in which the Mn-II moments are nearly perpendicular to the c axis. The induced spin-density distribution in the paramagnetic phase, determined by polarized neutron diffraction, visualizes the superexchange pathways through the dca ligands within the layers and through H bonding between neighboring layers. The theoretical spin density obtained by bidimensional periodic DFT calculations is compared with the experimental results. Furthermore, quantum Monte Carlo simulations have been performed to compare the DFT results with experimental susceptibility measurements.Wiley-VCH2018info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionapplication/pdfhttps://hdl.handle.net/2445/154801Articles publicats en revistes (Química Inorgànica i Orgànica)reponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaInglésVersió postprint del document publicat a: https://doi.org/10.1002/ejic.201700971European Journal of Inorganic Chemistry, 2018, num. 3-4, p. 278-288https://doi.org/10.1002/ejic.201700971(c) Wiley-VCH, 2018info:eu-repo/semantics/openAccessoai:diposit.ub.edu:2445/1548012026-05-27T06:46:51Z
dc.title.none.fl_str_mv H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations
title H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations
spellingShingle H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations
Gillon, Beatrice
Lligands
Estructura cristal·lina (Sòlids)
Teoria del funcional de densitat
Propietats magnètiques
Metalls de transició
Ligands
Layer structure (Solids)
Density functionals
Magnetic properties
Transition metals
title_short H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations
title_full H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations
title_fullStr H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations
title_full_unstemmed H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations
title_sort H-Mediated magnetic interactions between layers in a 2D Mn-II-dicyanamide polymer: neutron diffraction, DFT, and quantum Monte Carlo calculations
dc.creator.none.fl_str_mv Gillon, Beatrice
Hammerschmied, Albert
Gukasov, Arsen
Cousson, Alain
Cauchy, Thomas
Ruiz Sabín, Eliseo
Schlueter, John A.
Manson, Jamie L.
author Gillon, Beatrice
author_facet Gillon, Beatrice
Hammerschmied, Albert
Gukasov, Arsen
Cousson, Alain
Cauchy, Thomas
Ruiz Sabín, Eliseo
Schlueter, John A.
Manson, Jamie L.
author_role author
author2 Hammerschmied, Albert
Gukasov, Arsen
Cousson, Alain
Cauchy, Thomas
Ruiz Sabín, Eliseo
Schlueter, John A.
Manson, Jamie L.
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Lligands
Estructura cristal·lina (Sòlids)
Teoria del funcional de densitat
Propietats magnètiques
Metalls de transició
Ligands
Layer structure (Solids)
Density functionals
Magnetic properties
Transition metals
topic Lligands
Estructura cristal·lina (Sòlids)
Teoria del funcional de densitat
Propietats magnètiques
Metalls de transició
Ligands
Layer structure (Solids)
Density functionals
Magnetic properties
Transition metals
description We report neutron-diffraction investigations of the quasi-2D Mn-II(dca)(2)(pym)(H2O) (pym = N2C4H4) compound, where high-spin Mn-II ions are bridged by dicyanamide anions, [N(CN)(2)](-) (herein abbreviated dca). Inside the layers, Mn2+ ions are connected by single or double dca bridges. The magnetic phase diagram was established by neutron diffraction on a single crystal. In the low-field phase, the Mn-II ions are antiferromagnetically ordered in the layers, with moments nearly parallel to the c axis, and the layers are antiferromagnetically coupled. The spin-flop phase corresponds to ferromagnetic coupling between the antiferromagnetic layers, in which the Mn-II moments are nearly perpendicular to the c axis. The induced spin-density distribution in the paramagnetic phase, determined by polarized neutron diffraction, visualizes the superexchange pathways through the dca ligands within the layers and through H bonding between neighboring layers. The theoretical spin density obtained by bidimensional periodic DFT calculations is compared with the experimental results. Furthermore, quantum Monte Carlo simulations have been performed to compare the DFT results with experimental susceptibility measurements.
publishDate 2018
dc.date.none.fl_str_mv 2018
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/154801
url https://hdl.handle.net/2445/154801
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Versió postprint del document publicat a: https://doi.org/10.1002/ejic.201700971
European Journal of Inorganic Chemistry, 2018, num. 3-4, p. 278-288
https://doi.org/10.1002/ejic.201700971
dc.rights.none.fl_str_mv (c) Wiley-VCH, 2018
info:eu-repo/semantics/openAccess
rights_invalid_str_mv (c) Wiley-VCH, 2018
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Wiley-VCH
publisher.none.fl_str_mv Wiley-VCH
dc.source.none.fl_str_mv Articles publicats en revistes (Química Inorgànica i Orgànica)
reponame:Dipòsit Digital de la UB
instname:Universidad de Barcelona
instname_str Universidad de Barcelona
reponame_str Dipòsit Digital de la UB
collection Dipòsit Digital de la UB
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869403587126231040
score 15,300719

Similares en LA Referencia