An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environment

Two new isostructural compounds based on 6-methyl-2-oxonicotinate (6m2onic) ligand and sodium and lanthanide(III) ions are reported. The structural and chemical characterization reveals the following chemical formula: {[Ln(6m2onic)2(μ-6m2onic)2Na(H2O)3]·8H2O}n [where Ln(III) = Dy (1Dy) and Er (2Er)]...

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Autores: Razquin Bobillo, Laura, Pajuelo Corral, Oier, Zabala Lekuona, Andoni, Rodríguez Diéguez, Antonio, Cepeda Ruiz, Javier
Formato: artículo
Fecha de publicación:2022
País:España
Recursos:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/65832
Acesso em linha:http://hdl.handle.net/10810/65832
Access Level:acceso abierto
Palavra-chave:SMM
lanthanide
6-methyl-2-oxonicotinate
square antiprism
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spelling An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environmentRazquin Bobillo, LauraPajuelo Corral, OierZabala Lekuona, AndoniRodríguez Diéguez, AntonioCepeda Ruiz, JavierSMMlanthanide6-methyl-2-oxonicotinatesquare antiprismTwo new isostructural compounds based on 6-methyl-2-oxonicotinate (6m2onic) ligand and sodium and lanthanide(III) ions are reported. The structural and chemical characterization reveals the following chemical formula: {[Ln(6m2onic)2(μ-6m2onic)2Na(H2O)3]·8H2O}n [where Ln(III) = Dy (1Dy) and Er (2Er)]. These compounds crystallize in the form of one-dimensional arrays held together into a hydrogenbonded structure, in which 6m2onic ligands establish four O,O’ chelating rings with the lanthanide to render a distorted square antiprism (SAPR) geometry. Magnetic dc and ac susceptibility measurements confirm that 1Dy and 2Er behave as SIMs. Magnetic dilutions using Y(III) matrices have been made to achieve a Dy(III) counterpart (1Y/Dy) that presents slow magnetic relaxation under zero dc field. Under an optimized Hdc field (of 1000 Oe and 1500 Oe for 1Y/Dy and 2Y/Er, respectively), 1Y/Dy reveals the occurrence of two well-separated maxima, attributed to SR (Ueff = 65.2 K (45.3 cm−1) and τ0 = 2.76 × 10−9 s) and FR processes (Ueff = 23.2 K (16.1 cm−1) and τ0 = 1.40 × 10−8 s), whereas 2Y/Er shows a multiple relaxation pathway that considers quantum tunnelling of the magnetization (QTM), Orbach, Raman and direct mechanisms. Ab initio calculations have been carried out to support the experimental evidence and to explain the lanthanide ion-dependent behaviour deepen the understanding of the magneto-structural relationship of the SAPR environment.This work has been funded by the Spanish Ministry of Science, Innovation and Universities (MCIU/AEI/FEDER, UE) (PGC2018- 102052-A-C22, PGC2018-102052-B-C21), University of the Basque Country (GIU20/028), Gobierno Vasco/Eusko Jaurlaritza (IT1755-22), and Junta de Andalucía (FQM-394 and B-FQM-734- UGR2). OPC thanks his predoctoral fellowship to UPV/EHU202420242022info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10810/65832reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoInglésinfo:eu-repo/grantAgreement/MCIU/PGC2018- 102052-A-C22/info:eu-repo/grantAgreement/MCIU/PGC2018-102052-B-C21/https://pubs.rsc.org/en/content/articlelanding/2022/dt/d2dt02401binfo:eu-repo/semantics/openAccess© 2022 The Royal Society of Chemistryoai:addi.ehu.eus:10810/658322026-06-18T09:23:17Z
dc.title.none.fl_str_mv An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environment
title An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environment
spellingShingle An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environment
Razquin Bobillo, Laura
SMM
lanthanide
6-methyl-2-oxonicotinate
square antiprism
title_short An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environment
title_full An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environment
title_fullStr An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environment
title_full_unstemmed An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environment
title_sort An experimental and theoretical study of the magnetic relaxation in heterometallic coordination polymers based on 6-methyl-2-oxonicotinate and lanthanide(III) ions with square antriprismatic environment
dc.creator.none.fl_str_mv Razquin Bobillo, Laura
Pajuelo Corral, Oier
Zabala Lekuona, Andoni
Rodríguez Diéguez, Antonio
Cepeda Ruiz, Javier
author Razquin Bobillo, Laura
author_facet Razquin Bobillo, Laura
Pajuelo Corral, Oier
Zabala Lekuona, Andoni
Rodríguez Diéguez, Antonio
Cepeda Ruiz, Javier
author_role author
author2 Pajuelo Corral, Oier
Zabala Lekuona, Andoni
Rodríguez Diéguez, Antonio
Cepeda Ruiz, Javier
author2_role author
author
author
author
dc.subject.none.fl_str_mv SMM
lanthanide
6-methyl-2-oxonicotinate
square antiprism
topic SMM
lanthanide
6-methyl-2-oxonicotinate
square antiprism
description Two new isostructural compounds based on 6-methyl-2-oxonicotinate (6m2onic) ligand and sodium and lanthanide(III) ions are reported. The structural and chemical characterization reveals the following chemical formula: {[Ln(6m2onic)2(μ-6m2onic)2Na(H2O)3]·8H2O}n [where Ln(III) = Dy (1Dy) and Er (2Er)]. These compounds crystallize in the form of one-dimensional arrays held together into a hydrogenbonded structure, in which 6m2onic ligands establish four O,O’ chelating rings with the lanthanide to render a distorted square antiprism (SAPR) geometry. Magnetic dc and ac susceptibility measurements confirm that 1Dy and 2Er behave as SIMs. Magnetic dilutions using Y(III) matrices have been made to achieve a Dy(III) counterpart (1Y/Dy) that presents slow magnetic relaxation under zero dc field. Under an optimized Hdc field (of 1000 Oe and 1500 Oe for 1Y/Dy and 2Y/Er, respectively), 1Y/Dy reveals the occurrence of two well-separated maxima, attributed to SR (Ueff = 65.2 K (45.3 cm−1) and τ0 = 2.76 × 10−9 s) and FR processes (Ueff = 23.2 K (16.1 cm−1) and τ0 = 1.40 × 10−8 s), whereas 2Y/Er shows a multiple relaxation pathway that considers quantum tunnelling of the magnetization (QTM), Orbach, Raman and direct mechanisms. Ab initio calculations have been carried out to support the experimental evidence and to explain the lanthanide ion-dependent behaviour deepen the understanding of the magneto-structural relationship of the SAPR environment.
publishDate 2022
dc.date.none.fl_str_mv 2022
2024
2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10810/65832
url http://hdl.handle.net/10810/65832
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/MCIU/PGC2018- 102052-A-C22/
info:eu-repo/grantAgreement/MCIU/PGC2018-102052-B-C21/
https://pubs.rsc.org/en/content/articlelanding/2022/dt/d2dt02401b
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
© 2022 The Royal Society of Chemistry
eu_rights_str_mv openAccess
rights_invalid_str_mv © 2022 The Royal Society of Chemistry
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:Addi. Archivo Digital para la Docencia y la Investigación
instname:Universidad del País Vasco
instname_str Universidad del País Vasco
reponame_str Addi. Archivo Digital para la Docencia y la Investigación
collection Addi. Archivo Digital para la Docencia y la Investigación
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,301603

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