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Register a new userA new family of disorder-free Rare-Earth-based kagome lattice magnets: structure and magnetic characterizations of RE3BWO9 (RE=Pr, Nd, Gd-Ho) Boratotungstates
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Authors
Malik Ashtar
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Exploration of rare-earth (RE)-based Kagome lattice magnets with spin-orbital entangled jeff=1/2 moments will provide new platform for investigating the exotic magnetic phases. Here, we report a new family of RE3BWO9 (RE=Pr,Nd,Gd-Ho) boratotungstates with magnetic RE3+ ions arranged on Kagome lattice, and perform its structure and magnetic characterizations. This serial compounds crystallize in hexagonal coordinated structure with space group P63 (No.173), where magnetic RE3+ ions have distorted Kagome lattice connections within the ab plane and stacked in a AB-type fashion along c axis. The interlayer RE-RE separation is comparable with that of intralayer distance, forming 3-dimensional (3D) exchange coupled magnetic framework of RE3+ ions. The magnetic susceptibility data of RE3BWO9 (RE=Pr, Nd, Gd-Ho) reveal dominant antiferromagnetic interactions between magnetic RE3+ ions, but without visible magnetic ordering down to 2 K. The magnetization analyses for different RE3+ ions show diverse anisotropic behaviors, make RE3BWO9 as an appealing Kagome-lattice antiferromagnet to explore exotic magnetic phases.
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Rare-earth (RE) based frustrated magnets as typical systems of combining strong spin-orbit coupling, geometric frustration and anisotropic exchange interactions, can give rise to diverse exotic magnetic ground states such as quantum spin liquid (QSL). The discovery of new RE-based frustrated materials is crucial for exploring the exotic magnetic phases. Herein, we report the synthesis, structure and magnetic properties of a family of melilite-type RE2Be2GeO7 (RE = Pr, Nd, Gd-Yb) compounds crystallized in a tetragonal structure, where magnetic RE3+ ions lay out on Shastry-Sutherland lattice (SSL) within ab-plane and are well separated by nonmagnetic GeBe2O7 polyhedrons along c-axis. Temperature-dependent susceptibilities and isothermal magnetization M(H) measurements reveal that most RE2Be2GeO7 compounds except RE=Tb show no magnetic ordering down to 2 K despite the dominant antiferromagnetic (AFM) interactions, where Tb2Be2GeO7 undergoes AFM transition with Neel temperature TN~ 2.5 K and field-induced spin flop behaviors (T< TN). In addition, the calculated magnetic entropy change from the isothermal M(H) curves reveal a viable magnetocaloric effect (MCE) for RE2Be2GeO7 (RE =Gd, Dy) in liquid helium temperature regimes, Gd2Be2GeO7 shows maximum Sm up to 54.8 J K-1 Kg-1 at H= 7 T and Dy2Be2GeO7 has largest value Sm=16.1 J K-1 kg-1 at H= 2 T in this family. More excitingly, rich diversity of RE ions in this family enables an archetype for exploring exotic quantum magnetic phenomena with large variability of spin located on SSL lattice.
We present a systematic study of the structural and magnetic properties of two branches of the rare earth Tripod Kagome Lattice (TKL) family A$_{2}$RE$_{3}$Sb$_{3}$O$_{14}$ (A = Mg, Zn; RE = Pr, Nd, Gd, Tb, Dy, Ho, Er, Yb; here, we use abbreviation textit{A-RE}, as in textit{MgPr} for Mg$_{2}$Pr$_{3}$Sb$_{3}$O$_{14}$), which complements our previously reported work on textit{MgDy}, textit{MgGd}, and textit{MgEr} cite{TKL}. The present susceptibility ($chi_{dc}$, $chi_{ac}$) and specific heat measurements reveal various magnetic ground states, including the non-magnetic singlet state for textit{MgPr}, textit{ZnPr}; long range orderings (LROs) for textit{MgGd}, textit{ZnGd}, textit{MgNd}, textit{ZnNd}, and textit{MgYb}; a long range magnetic charge ordered state for textit{MgDy}, textit{ZnDy}, and potentially for textit{MgHo}; possible spin glass states for textit{ZnEr}, textit{ZnHo}; the absence of spin ordering down to 80 mK for textit{MgEr}, textit{MgTb}, textit{ZnTb}, and textit{ZnYb} compounds. The ground states observed here bear both similarities as well as striking differences from the states found in the parent pyrochlore systems. In particular, while the TKLs display a greater tendency towards LRO, the lack of LRO in textit{MgHo}, textit{MgTb} and textit{ZnTb} can be viewed from the standpoint of a balance among spin-spin interactions, anisotropies and non-Kramers nature of single ion state. While substituting Zn for Mg changes the chemical pressure, and subtly modifies the interaction energies for compounds with larger RE ions, this substitution introduces structural disorder and modifies the ground states for compounds with smaller RE ions (Ho, Er, Yb).
The design and synthesis of targeted functional materials have been a long-term goal for material scientists. Although a universal design strategy is difficult to generate for all types of materials, however, it is still helpful for a typical family of materials to have such design rules. Herein, we incorporated several significant chemical and physical factors regarding magnetism, such as structure type, atom distance, spin-orbit coupling, and successfully synthesized a new rare-earth-free ferromagnet, MnPt5As, for the first time. MnPt5As can be prepared by using high-temperature pellet methods. According to X-ray diffraction results, MnPt5As crystallizes in a tetragonal unit cell with the space group P4/mmm (Pearson symbol tP7). Magnetic measurements on MnPt5As confirm ferromagnetism in this phase with a Curie temperature of ~301 K and a saturated moment of 3.5 uB per formula. Evaluation by applying the Stoner Criterion also indicates that MnPt5As is susceptible to ferromagnetism. Electronic structure calculations using the WIEN2k program with local spin density approximation imply that the spontaneous magnetization of this phase arises primarily from the hybridization of d orbitals on both Mn and Pt atoms. The theoretical assessments are consistent with the experimental results. Moreover, the spin-orbit coupling effects heavily influence on magnetic moments in MnPt5As. MnPt5As is the first high-performance magnetic material in this structure type. The discovery of MnPt5As offers a platform to study the interplay between magnetism and structure.
Exploration of the topological quantum materials with electron correlation is at the frontier of physics, as the strong interaction may give rise to new topological phases and transitions. Here we report that a family of kagome magnets RMn$_6$Sn$_6$ manifest the quantum transport properties analogical to those in the quantum-limit Chern magnet TbMn$_6$Sn$_6$. The topological transport in the family, including quantum oscillations with nontrivial Berry phase and large anomalous Hall effect arising from Berry curvature field, points to the existence of massive Dirac fermions. Our observation demonstrates a close relationship between rare-earth magnetism and topological electron structure, indicating the rare-earth elements can effectively engineer the Chern quantum phase in kagome magnets.
We present the crystal structures and magnetic properties of RE3Sb3Mg2O14 (La3Sb3Mg2O14, Pr3Sb3Mg2O14, Sm3Sb3Mg2O14, Eu3Sb3Mg2O14, Tb3Sb3Mg2O14, and Ho3Sb3Mg2O14), a family of novel materials based on a perfect geometry 2D rare earth Kagome lattice. Structure refinements were performed by the Rietveld method using X-ray diffraction data, indicating that the layered compounds are fully structurally ordered. The compounds crystallize in a rhombohedral supercell of the cubic pyrochlore structure, in the space group R-3m. As indicated by magnetic susceptibility measurements, they exhibit predominantly antiferromagnetic interactions between rare earth moments. Except for possibly Pr3Sb3Mg2O14 and Eu3Sb3Mg2O14, none of the compounds show any signs of magnetic ordering above 2 K. This RE3Sb3Mg2O14 family of compounds is similar to that of RE3Sb3Zn2O14, except the series reported here features a fully ordered distribution of cations in both the nonmagnetic antimony and magnesium sites and the magnetic rare earth kagome sites. The compounds appear to be relatively defect-free and are therefore model systems for investigating magnetic frustration on an ideal 2D rare earth Kagome lattice.
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