Reinhard K. Kremer, Walter Schnelle, Roland Eger, Arndt Simon, P. Jane Brown, Bachir Ouladdiaf, Klaus-Ulrich Neumann
{"title":"受挫稀土链系统 M2Cl3(M = 钆、铽)中的反铁磁有序性","authors":"Reinhard K. Kremer, Walter Schnelle, Roland Eger, Arndt Simon, P. Jane Brown, Bachir Ouladdiaf, Klaus-Ulrich Neumann","doi":"10.1021/acs.chemmater.4c01317","DOIUrl":null,"url":null,"abstract":"The magnetic properties of the two isostructural rare-earth condensed octahedral-cluster chain compounds M<sub>2</sub>Cl<sub>3</sub> (M = Gd, Tb) have been investigated by magnetization, heat capacity, and single-crystal neutron diffraction experiments. Both compounds exhibit antiferromagnetic order below ∼23 and ∼43 K for Gd<sub>2</sub>Cl<sub>3</sub> and Tb<sub>2</sub>Cl<sub>3</sub>, respectively. For Gd<sub>2</sub>Cl<sub>3</sub>, the large negative Curie–Weiss temperature of ∼−209 K indicates substantial magnetic frustration. The magnetic moments of Gd at the two different crystallographic atom positions are aligned along the chains. Whereas at ∼14.5 K the magnetic moments at the shared edge approach the theoretically expected spin-only value of ∼7 μ<sub>B</sub>, the moments at the geometrically frustrated apical position of the octahedra are significantly reduced. In Tb<sub>2</sub>Cl<sub>3</sub>, the magnetic moments lie in the plane perpendicular to the chains and are inclined with respect to each other. The Tb cations in the shared edges have a magnetic moment of 9.3 μ<sub>B</sub>, slightly exceeding the maximum value of 9 μ<sub>B</sub> that is expected for Tb<sup>3+</sup> with <i>J</i> = 6 for the Russell–Saunders ground state. Neutron scattering with polarization analysis on a Tb<sub>2</sub>Cl<sub>3</sub> crystal in a magnetic field reveals enhanced polarizability of the Tb moments at the frustrated apical octahedral sites.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Antiferromagnetic Ordering in the Frustrated Rare-Earth Chain Systems M2Cl3 (M = Gd, Tb)\",\"authors\":\"Reinhard K. Kremer, Walter Schnelle, Roland Eger, Arndt Simon, P. Jane Brown, Bachir Ouladdiaf, Klaus-Ulrich Neumann\",\"doi\":\"10.1021/acs.chemmater.4c01317\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The magnetic properties of the two isostructural rare-earth condensed octahedral-cluster chain compounds M<sub>2</sub>Cl<sub>3</sub> (M = Gd, Tb) have been investigated by magnetization, heat capacity, and single-crystal neutron diffraction experiments. Both compounds exhibit antiferromagnetic order below ∼23 and ∼43 K for Gd<sub>2</sub>Cl<sub>3</sub> and Tb<sub>2</sub>Cl<sub>3</sub>, respectively. For Gd<sub>2</sub>Cl<sub>3</sub>, the large negative Curie–Weiss temperature of ∼−209 K indicates substantial magnetic frustration. The magnetic moments of Gd at the two different crystallographic atom positions are aligned along the chains. Whereas at ∼14.5 K the magnetic moments at the shared edge approach the theoretically expected spin-only value of ∼7 μ<sub>B</sub>, the moments at the geometrically frustrated apical position of the octahedra are significantly reduced. In Tb<sub>2</sub>Cl<sub>3</sub>, the magnetic moments lie in the plane perpendicular to the chains and are inclined with respect to each other. The Tb cations in the shared edges have a magnetic moment of 9.3 μ<sub>B</sub>, slightly exceeding the maximum value of 9 μ<sub>B</sub> that is expected for Tb<sup>3+</sup> with <i>J</i> = 6 for the Russell–Saunders ground state. Neutron scattering with polarization analysis on a Tb<sub>2</sub>Cl<sub>3</sub> crystal in a magnetic field reveals enhanced polarizability of the Tb moments at the frustrated apical octahedral sites.\",\"PeriodicalId\":33,\"journal\":{\"name\":\"Chemistry of Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2024-07-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemistry of Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.chemmater.4c01317\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemistry of Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acs.chemmater.4c01317","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Antiferromagnetic Ordering in the Frustrated Rare-Earth Chain Systems M2Cl3 (M = Gd, Tb)
The magnetic properties of the two isostructural rare-earth condensed octahedral-cluster chain compounds M2Cl3 (M = Gd, Tb) have been investigated by magnetization, heat capacity, and single-crystal neutron diffraction experiments. Both compounds exhibit antiferromagnetic order below ∼23 and ∼43 K for Gd2Cl3 and Tb2Cl3, respectively. For Gd2Cl3, the large negative Curie–Weiss temperature of ∼−209 K indicates substantial magnetic frustration. The magnetic moments of Gd at the two different crystallographic atom positions are aligned along the chains. Whereas at ∼14.5 K the magnetic moments at the shared edge approach the theoretically expected spin-only value of ∼7 μB, the moments at the geometrically frustrated apical position of the octahedra are significantly reduced. In Tb2Cl3, the magnetic moments lie in the plane perpendicular to the chains and are inclined with respect to each other. The Tb cations in the shared edges have a magnetic moment of 9.3 μB, slightly exceeding the maximum value of 9 μB that is expected for Tb3+ with J = 6 for the Russell–Saunders ground state. Neutron scattering with polarization analysis on a Tb2Cl3 crystal in a magnetic field reveals enhanced polarizability of the Tb moments at the frustrated apical octahedral sites.
期刊介绍:
The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.