Real-space investigation of short-range magnetic correlations in fluoride pyrochlores NaCaCo2_2F7_7 and NaSrCo2_2F7_7 with magnetic pair distribution function analysis

We present time-of-flight neutron total scattering and polarized neutron scattering measurements of the magnetically frustrated compounds NaCaCo$_2$F$_7$ and NaSrCo$_2$F$_7$, which belong to a class of recently discovered pyrochlore compounds based on transition metals and fluorine. The magnetic pair distribution function (mPDF) technique is used to analyze and model the total scattering data in real space. We find that a previously-proposed model of short-range XY-like correlations with a length scale of 10-15 \AA, combined with nearest-neighbor collinear antiferromagnetic correlations, accurately describes the mPDF data at low temperature, confirming the magnetic ground state in these materials. This model is further verified by the polarized neutron scattering data. From an analysis of the temperature dependence of the mPDF and polarized neutron scattering data, we find that short-range correlations persist on the nearest-neighbor length scale up to 200 K, approximately two orders of magnitude higher than the spin freezing temperatures of these compounds. These results highlight the opportunity presented by these new pyrochlore compounds to study the effects of geometric frustration at relatively high temperatures, while also advancing the mPDF technique and providing a novel opportunity to investigate a genuinely short-range-ordered magnetic ground state directly in real space

Breathing Pyrochlore Lattice Realized in <em>A</em>-Site Ordered Spinel Oxides LiGaCr₄O₈ and LiInCr₄O₈

A unique type of frustrated lattice is found in two A-site ordered spinel oxides, LiGaCr4O8 and LiInCr4O8. Because of the large size mismatch between Li+ and Ga3+/In3+ ions at the A site, the pyrochlore lattice, made up of Cr3+ ions carrying spin 3/2, becomes an alternating array of small and large tetrahedra, i.e., a "breathing" pyrochlore lattice. We introduce a parameter, the breathing factor Bf, which quantifies the degree of frustration in the pyrochlore lattice: Bf is defined as J'/J, where J' and J are nearest-neighbor magnetic interactions in the large and small tetrahedra, respectively. LiGaCr4O8 with Bf ~ 0.6 shows magnetic susceptibility similar to that of conventional Cr spinel oxides such as ZnCr2O4. In contrast, LiInCr4O8 with a small Bf ~ 0.1 exhibits a spin-gap behavior in its magnetic susceptibility, suggesting a proximity to an exotic singlet ground state. Magnetic long-range order occurs at 13.8 and 15.9 K for LiGaCr4O8 and LiInCr4O8, respectively, in both cases likely owing to the coupling to structural distortions.Comment: 5 pages, 5 figures, accepted for publication in Phys. Rev. Let

Phase diagram of multiferroic KCu3_3As2_2O7_7(OD)3_3

The layered compound KCu$_3$As$_2$O$_7$(OD)$_3$, comprising distorted kagome planes of $S=1/2$ Cu$^{2+}$ ions, is a recent addition to the family of type-II multiferroics. Previous zero field neutron diffraction work has found two helically ordered regimes in \kns, each showing a distinct coupling between the magnetic and ferroelectric order parameters. Here, we extend this work to magnetic fields up to $20$~T using neutron powder diffraction, capacitance, polarization, and high-field magnetization measurements, hence determining the $H-T$ phase diagram. We find metamagnetic transitions in both low temperatures phases around $\mu_0 H_c \sim 3.7$~T, which neutron powder diffraction reveals to correspond to a rotation of the helix plane away from the easy plane, as well as a small change in the propagation vector. Furthermore, we show that the sign of the ferroelectric polarization is reversible in a magnetic field, although no change is observed (or expected on the basis of the magnetic structure) due to the transition at $3.7$~T. We finally justify the temperature dependence of the polarization in both zero-field ordered phases by a symmetry analysis of the free energy expansion

Magnetic, electronic, and structural investigation of the strongly correlated Y1−x_{1-x}Smx_xCo5_5 system

SmCo$_5$ and YCo$_5$ are isostructural compounds both showing large magnetocrystalline anisotropy, where the former originates mainly from the crystal-electric field and magnetic interactions. We investigate the contribution of both interactions by partially substituting Y by Sm in as-cast polycrystalline Y$_{1-x}$Sm$_{x}$Co$_5$ (with $x$=0, 0.1, 0.2, 0.3, and 0.4) and measuring their structural, magnetic, and electrical properties through X-ray diffraction, magnetization, and electrical transport measurements. Our results suggest an interplay between microstructure strain in as-cast samples and the electronic and magnetic interactions

Realizing square and diamond lattice S =1/2 Heisenberg antiferromagnet models in the α and β phases of the coordination framework, KTi(C2O4)2⋅xH2O

Provision of a PhD studentship to A.H.A. by the University of Liverpool and the Science and Technology Facilities Council (STFC) is gratefully acknowledged. The work of T.L. was funded by the University of St Andrews and China Scholarship Council (CSC) joint scholarship (201606280032). A.T. was funded by the Federal Ministry of Education and Research through the Sofja Kovalevskaya Award of Alexander von Humboldt Foundation. Work at St Andrews was supported by the Leverhulme Trust (RPG-2013-343).We report the crystal structures and magnetic properties of two pseudopolymorphs of the S=1/2 Ti3+ coordination framework, KTi(C2O4)2⋅xH2O. Single-crystal x-ray and powder neutron diffraction measurements on α−KTi(C2O4)2⋅xH2O confirm its structure in the tetragonal I4/mcm space group with a square planar arrangement of Ti3+ ions. Magnetometry and specific heat measurements reveal weak antiferromagnetic interactions, with J1≈7 K and J2/J1=0.11 indicating a slight frustration of nearest- and next-nearest-neighbor interactions. Below 1.8 K, α−KTi(C2O4)2⋅xH2O undergoes a transition to G-type antiferromagnetic order with magnetic moments aligned along the c axis of the tetragonal structure. The estimated ordered moment of Ti3+ in α−KTi(C2O4)2⋅xH2O is suppressed from its spin-only value to 0.62(3) μB, thus verifying the two-dimensional nature of the magnetic interactions within the system. β−KTi(C2O4)2⋅2H2O, on the other hand, realizes a three-dimensional diamondlike magnetic network of Ti3+ moments within a hexagonal P6222 structure. An antiferromagnetic exchange coupling of J≈54 K—an order of magnitude larger than in α−KTi(C2O4)2⋅xH2O—is extracted from magnetometry and specific heat data. β−KTi(C2O4)2⋅2H2O undergoes Néel ordering at TN=28 K, with the magnetic moments aligned within the ab plane and a slightly reduced ordered moment of 0.79 μB per Ti3+. Through density-functional theory calculations, we address the origin of the large difference in the exchange parameters between the α and β pseudopolymorphs. Given their observed magnetic behaviors, we propose α−KTi(C2O4)2⋅xH2O and β−KTi(C2O4)2⋅2H2O as close to ideal model S =1/2 Heisenberg square and diamond lattice antiferromagnets, respectively.PostprintPeer reviewe

One dimensional magnetism in synthetic Pauflerite, β\beta-VOSO4_4

We have synthesized single-crystal samples of $\beta$-VOSO$_4$ and fully characterized their magnetic properties. Our magnetic susceptibility, high field magnetization and powder inelastic neutron scattering results are in excellent agreement with theoretical expressions for a one-dimensional spin-1/2 Heisenberg chain with an exchange parameter of $3.83(2)$\,meV. Ab-initio calculations identify the superexchange pathway, revealing that the spin-chain does not run along the expected crystallographic chain $a$-direction but instead between V$^{4+}$O$_{6}$ octahedra that are linked via SO$_{4}$ tetrahedra along the $b$-axis. We do not detect any phase transition to a long-range magnetic order within our experimental conditions, indicating $\beta$-VOSO$_4$ is very close to an ideal one-dimensional magnetic system