Chen Jianyi, Calder Stuart, Paddison Joseph A M, Angelo Gina, Klivansky Liana, Zhang Jian, Cao Huibo, Gui Xin
Department of Chemistry, University of Pittsburgh, Pittsburgh, PA, 15260, USA.
Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
Adv Mater. 2025 Mar;37(10):e2417906. doi: 10.1002/adma.202417906. Epub 2024 Dec 31.
Magnetoplumbites are one of the most broadly studied families of hexagonal ferrites, typically with high magnetic ordering temperatures, making them excellent candidates for permanent magnets. However, magnetic frustration is rarely observed in magnetoplumbites. Herein, the discovery, synthesis, and characterization of the first Mn-based magnetoplumbite, as well as the first magnetoplumbite involving pnictogens (Sb), ASbMnO (A = K or Rb) are reported. The Mn (S = 2) cations, further confirmed by DC magnetic susceptibility and X-ray photoelectron spectroscopy, construct three geometrically frustrated sublattices, including Kagome, triangular, and puckered honeycomb lattices. Magnetic properties measurements revealed strong antiferromagnetic spin-spin coupling as well as multiple low-temperature magnetic features. Heat capacity data does not show any prominent λ-anomaly, suggesting minimal associated magnetic entropy. Moreover, neutron powder diffraction (NPD) implied the absence of long-range magnetic ordering in KSbMnO down to 3 K. However, several magnetic peaks are observed in RbSbMnO at 3 K, corresponding to an incommensurate magnetic structure. Interestingly, strong diffuse scattering is seen in the NPD patterns of both compounds at low angles and is analyzed by reverse Monte Carlo refinements, indicating short-range spin ordering related to frustrated magnetism as well as 2D magnetic correlations in ASbMnO (A = K or Rb).
磁铅石是研究最为广泛的六方铁氧体家族之一,通常具有较高的磁有序温度,这使其成为永磁体的理想候选材料。然而,在磁铅石中很少观察到磁阻挫现象。在此,报道了首例基于锰的磁铅石以及首例含有氮族元素(锑)的磁铅石ASbMnO(A = K或Rb)的发现、合成与表征。通过直流磁化率和X射线光电子能谱进一步证实,Mn(S = 2)阳离子构建了三个几何阻挫亚晶格,包括 Kagome晶格、三角形晶格和褶皱蜂窝晶格。磁性测量结果显示出强反铁磁自旋 - 自旋耦合以及多个低温磁性特征。热容数据未显示任何明显的λ异常,表明相关磁熵极小。此外,中子粉末衍射(NPD)表明,在KSbMnO中直至3 K都不存在长程磁有序。然而,在3 K时,在RbSbMnO中观察到几个磁峰,对应于非公度磁结构。有趣的是,在两种化合物的NPD图谱的低角度处都观察到强漫散射,并通过反向蒙特卡罗精修进行分析,表明存在与阻挫磁性相关的短程自旋有序以及ASbMnO(A = K或Rb)中的二维磁关联。