Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties

Autores
Gainza, Javier; Guiñazú, Orlando Nicolás; Cesped, Eva; Falcon, Horacio; Martínez, Jose Luis; Alonso, José Antonio
Año de publicación
2023
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Indium thiospinels (AIn2S4, A= transition metals) have attracted significant attention due to their potential for manipulating magnetic and optoelectronic properties through changes in chemical composition. Defined in the cubic space group Fd-3 m (No. 227), the crystal structure consists of a framework of edge-sharing InS6 octahedra (Oh symmetry), with A cations coordinated tetrahedrally (Td symmetry) to sulfur. In this study, we describe a rapid high-pressure synthetic method (3.5 GPa) to prepare MnIn2S4 polycrystalline samples, with tunable degree of inversion (λ) or Mn-In antisite, meaning that some Mn occupy the octahedral sites and some In atoms are located at the tetrahedral positions. We found that λ closely depends on the synthesis temperature. Notably, therefinement of the crystal structure from X-ray diffraction data reveals positive correlations between the inversion degree and different properties such as the band gap, expanding its spectral coverage, and the magnetic behavior, depending on the occupancy rate of the octahedral or tetrahedral sites by the strongly magnetic Mn2+ ions. Whereas the paramagnetic behavior is not affected by the inversion degree, for higher λ values (30%<λ < 38%), achieved at synthesis temperatures as high of 800ºC, the random distribution of Mn2+ ions between Td and Oh sites accounts for a spin-glass state with a clear cusp in the magnetic susceptibility (ac and dc), based on the strong short-range antiferromagnetic interactions.
Fil: Gainza, Javier. Instituto de Ciencia de Materiales de Madrid; España
Fil: Guiñazú, Orlando Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Cesped, Eva. Instituto de Ciencia de Materiales de Madrid; España
Fil: Falcon, Horacio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Martínez, Jose Luis. Instituto de Ciencia de Materiales de Madrid; España
Fil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; España
Materia
Thiospinel
InMn2S4
Inversion degree
Band gap
Magnetic interactions
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/244282
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/244282
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic propertiesGainza, JavierGuiñazú, Orlando NicolásCesped, EvaFalcon, HoracioMartínez, Jose LuisAlonso, José AntonioThiospinelInMn2S4Inversion degreeBand gapMagnetic interactionshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Indium thiospinels (AIn2S4, A= transition metals) have attracted significant attention due to their potential for manipulating magnetic and optoelectronic properties through changes in chemical composition. Defined in the cubic space group Fd-3 m (No. 227), the crystal structure consists of a framework of edge-sharing InS6 octahedra (Oh symmetry), with A cations coordinated tetrahedrally (Td symmetry) to sulfur. In this study, we describe a rapid high-pressure synthetic method (3.5 GPa) to prepare MnIn2S4 polycrystalline samples, with tunable degree of inversion (λ) or Mn-In antisite, meaning that some Mn occupy the octahedral sites and some In atoms are located at the tetrahedral positions. We found that λ closely depends on the synthesis temperature. Notably, therefinement of the crystal structure from X-ray diffraction data reveals positive correlations between the inversion degree and different properties such as the band gap, expanding its spectral coverage, and the magnetic behavior, depending on the occupancy rate of the octahedral or tetrahedral sites by the strongly magnetic Mn2+ ions. Whereas the paramagnetic behavior is not affected by the inversion degree, for higher λ values (30%<λ < 38%), achieved at synthesis temperatures as high of 800ºC, the random distribution of Mn2+ ions between Td and Oh sites accounts for a spin-glass state with a clear cusp in the magnetic susceptibility (ac and dc), based on the strong short-range antiferromagnetic interactions.Fil: Gainza, Javier. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Guiñazú, Orlando Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; ArgentinaFil: Cesped, Eva. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Falcon, Horacio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; ArgentinaFil: Martínez, Jose Luis. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; EspañaElsevier Science SA2023-12-25info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/244282Gainza, Javier; Guiñazú, Orlando Nicolás; Cesped, Eva; Falcon, Horacio; Martínez, Jose Luis; et al.; Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties; Elsevier Science SA; Journal of Alloys and Compounds; 969; 172413; 25-12-2023; 1-90925-8388CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.jallcom.2023.172413info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0925838823037167info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2026-02-06T12:31:32Zoai:ri.conicet.gov.ar:11336/244282instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982026-02-06 12:31:32.389CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties
title Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties
spellingShingle Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties
Gainza, Javier
Thiospinel
InMn2S4
Inversion degree
Band gap
Magnetic interactions
title_short Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties
title_full Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties
title_fullStr Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties
title_full_unstemmed Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties
title_sort Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties
dc.creator.none.fl_str_mv Gainza, Javier
Guiñazú, Orlando Nicolás
Cesped, Eva
Falcon, Horacio
Martínez, Jose Luis
Alonso, José Antonio
author Gainza, Javier
author_facet Gainza, Javier
Guiñazú, Orlando Nicolás
Cesped, Eva
Falcon, Horacio
Martínez, Jose Luis
Alonso, José Antonio
author_role author
author2 Guiñazú, Orlando Nicolás
Cesped, Eva
Falcon, Horacio
Martínez, Jose Luis
Alonso, José Antonio
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Thiospinel
InMn2S4
Inversion degree
Band gap
Magnetic interactions
topic Thiospinel
InMn2S4
Inversion degree
Band gap
Magnetic interactions
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Indium thiospinels (AIn2S4, A= transition metals) have attracted significant attention due to their potential for manipulating magnetic and optoelectronic properties through changes in chemical composition. Defined in the cubic space group Fd-3 m (No. 227), the crystal structure consists of a framework of edge-sharing InS6 octahedra (Oh symmetry), with A cations coordinated tetrahedrally (Td symmetry) to sulfur. In this study, we describe a rapid high-pressure synthetic method (3.5 GPa) to prepare MnIn2S4 polycrystalline samples, with tunable degree of inversion (λ) or Mn-In antisite, meaning that some Mn occupy the octahedral sites and some In atoms are located at the tetrahedral positions. We found that λ closely depends on the synthesis temperature. Notably, therefinement of the crystal structure from X-ray diffraction data reveals positive correlations between the inversion degree and different properties such as the band gap, expanding its spectral coverage, and the magnetic behavior, depending on the occupancy rate of the octahedral or tetrahedral sites by the strongly magnetic Mn2+ ions. Whereas the paramagnetic behavior is not affected by the inversion degree, for higher λ values (30%<λ < 38%), achieved at synthesis temperatures as high of 800ºC, the random distribution of Mn2+ ions between Td and Oh sites accounts for a spin-glass state with a clear cusp in the magnetic susceptibility (ac and dc), based on the strong short-range antiferromagnetic interactions.
Fil: Gainza, Javier. Instituto de Ciencia de Materiales de Madrid; España
Fil: Guiñazú, Orlando Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Cesped, Eva. Instituto de Ciencia de Materiales de Madrid; España
Fil: Falcon, Horacio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
Fil: Martínez, Jose Luis. Instituto de Ciencia de Materiales de Madrid; España
Fil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; España
description Indium thiospinels (AIn2S4, A= transition metals) have attracted significant attention due to their potential for manipulating magnetic and optoelectronic properties through changes in chemical composition. Defined in the cubic space group Fd-3 m (No. 227), the crystal structure consists of a framework of edge-sharing InS6 octahedra (Oh symmetry), with A cations coordinated tetrahedrally (Td symmetry) to sulfur. In this study, we describe a rapid high-pressure synthetic method (3.5 GPa) to prepare MnIn2S4 polycrystalline samples, with tunable degree of inversion (λ) or Mn-In antisite, meaning that some Mn occupy the octahedral sites and some In atoms are located at the tetrahedral positions. We found that λ closely depends on the synthesis temperature. Notably, therefinement of the crystal structure from X-ray diffraction data reveals positive correlations between the inversion degree and different properties such as the band gap, expanding its spectral coverage, and the magnetic behavior, depending on the occupancy rate of the octahedral or tetrahedral sites by the strongly magnetic Mn2+ ions. Whereas the paramagnetic behavior is not affected by the inversion degree, for higher λ values (30%<λ < 38%), achieved at synthesis temperatures as high of 800ºC, the random distribution of Mn2+ ions between Td and Oh sites accounts for a spin-glass state with a clear cusp in the magnetic susceptibility (ac and dc), based on the strong short-range antiferromagnetic interactions.
publishDate 2023
dc.date.none.fl_str_mv 2023-12-25
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/244282
Gainza, Javier; Guiñazú, Orlando Nicolás; Cesped, Eva; Falcon, Horacio; Martínez, Jose Luis; et al.; Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties; Elsevier Science SA; Journal of Alloys and Compounds; 969; 172413; 25-12-2023; 1-9
0925-8388
CONICET Digital
CONICET
url http://hdl.handle.net/11336/244282
identifier_str_mv Gainza, Javier; Guiñazú, Orlando Nicolás; Cesped, Eva; Falcon, Horacio; Martínez, Jose Luis; et al.; Tunable inversion degree of MnIn2S4 thiospinels prepared by high-pressure synthesis, and its implication in the optical and magnetic properties; Elsevier Science SA; Journal of Alloys and Compounds; 969; 172413; 25-12-2023; 1-9
0925-8388
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.jallcom.2023.172413
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0925838823037167
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science SA
publisher.none.fl_str_mv Elsevier Science SA
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.106097

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