ASbMnO (A = K or Rb): New Mn-Based 2D Magnetoplumbites with Geometric and Magnetic Frustration.

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.

Interlayer Ions Control Spin Canting in Low-Dimensional Manganese Trimers in 12R-BaMnO ( = Ce, Pr) Layered Perovskites.

To synthetically target a specific material with select performance, the underlying relationship between structure and function must be understood. For targeting magnetic properties, such understanding is underdeveloped for a relatively new class of layered hexagonal perovskites, the 12R-BaMnO family. Here, we perform a detailed magnetostructural study of the layered hexagonal perovskite materials 12R-BaMnO, where = diamagnetic Ce or paramagnetic ≈ 1/2 Pr.

Discovering Classical Spin Liquids by Topological Search of High Symmetry Nets.

Spin liquids are a paradigmatic example of a nontrivial state of matter. The search for new spin liquids is a key interdisciplinary challenge. Geometrical frustration-where the geometry of the net that the spins occupy precludes the generation of a simple ordered state-is a particularly fruitful way to generate these intrinsically disordered states.

Controlling Noncollinear Ferromagnetism in van der Waals Metal-Organic Magnets.

Van der Waals (vdW) magnets both allow exploration of fundamental 2D physics and offer a route toward exploiting magnetism in next generation information technology, but vdW magnets with complex, noncollinear spin textures are currently rare. We report here the syntheses, crystal structures, magnetic properties and magnetic ground states of four bulk vdW metal-organic magnets (MOMs): FeCl(pym), FeCl(btd), NiCl(pym), and NiCl(btd), pym = pyrimidine and btd = 2,1,3-benzothiadiazole. Using a combination of neutron diffraction and bulk magnetometry we show that these materials are noncollinear magnets.

Spinteract: a program to refine magnetic interactions to diffuse scattering data.

Magnetic diffuse scattering-the broad magnetic scattering features observed in neutron-diffraction data above a material's magnetic ordering temperature-provides a rich source of information about the material's magnetic Hamiltonian. However, this information has often remained under-utilised due to a lack of available computer software that can fit values of magnetic interaction parameters to such data. Here, an open-source computer program, Spinteract, is presented, which enables straightforward refinement of magnetic interaction parameters to powder and single-crystal magnetic diffuse scattering data.

Line-Graph Approach to Spiral Spin Liquids.

Competition among exchange interactions is able to induce novel spin correlations on a bipartite lattice without geometrical frustration. A prototype example is the spiral spin liquid, which is a correlated paramagnetic state characterized by subdimensional degenerate propagation vectors. Here, using spectral graph theory, we show that spiral spin liquids on a bipartite lattice can be approximated by a further-neighbor model on the corresponding line-graph lattice that is nonbipartite, thus broadening the space of candidate materials that may support the spiral spin liquid phases.

Geometric Frustration on the Trillium Lattice in a Magnetic Metal-Organic Framework.

In the dense metal-organic framework Na[Mn(HCOO)_{3}], Mn^{2+} ions (S=5/2) occupy the nodes of a "trillium" net. We show that the system is strongly magnetically frustrated: the Néel transition is suppressed well below the characteristic magnetic interaction strength; short-range magnetic order persists far above the Néel temperature; and the magnetic susceptibility exhibits a pseudo-plateau at 1/3-saturation magnetization. A simple model of nearest-neighbor Heisenberg antiferromagnetic and dipolar interactions accounts quantitatively for all observations, including an unusual 2-k magnetic ground state.

Scattering Signatures of Bond-Dependent Magnetic Interactions.

Bond-dependent magnetic interactions can generate exotic phases such as Kitaev spin-liquid states. Experimentally determining the values of bond-dependent interactions is a challenging but crucial problem. Here, I show that each symmetry-allowed nearest-neighbor interaction on triangular and honeycomb lattices has a distinct signature in paramagnetic neutron-diffraction data, and that such data contain sufficient information to determine the spin Hamiltonian unambiguously via unconstrained fits.

Sample Dependence of Magnetism in the Next-Generation Cathode Material LiNiMnCoO.

We present a structural and magnetic study of two batches of polycrystalline LiNiMnCoO (commonly known as Li NMC 811), a Ni-rich Li ion battery cathode material, using elemental analysis, X-ray and neutron diffraction, magnetometry, and polarized neutron scattering measurements. We find that the samples, labeled S1 and S2, have the composition LiNiMnCoO, with = 0.025(2), = 0.

Cluster Frustration in the Breathing Pyrochlore Magnet LiGaCr_{4}S_{8}.

We present a comprehensive neutron scattering study of the breathing pyrochlore magnet LiGaCr_{4}S_{8}. We observe an unconventional magnetic excitation spectrum with a separation of high- and low-energy spin dynamics in the correlated paramagnetic regime above a spin-freezing transition at 12(2) K. By fitting to magnetic diffuse-scattering data, we parametrize the spin Hamiltonian.

Strengthening the Magnetic Interactions in Pseudobinary First-Row Transition Metal Thiocyanates, M(NCS).

Understanding the effect of chemical composition on the strength of magnetic interactions is key to the design of magnets with high operating temperatures. The magnetic divalent first-row transition metal (TM) thiocyanates are a class of chemically simple layered molecular frameworks. Here, we report two new members of the family, manganese(II) thiocyanate, Mn(NCS), and iron(II) thiocyanate, Fe(NCS).

Quantum Versus Classical Spin Fragmentation in Dipolar Kagome Ice HoMgSbO.

A promising route to realize entangled magnetic states combines geometrical frustration with quantum-tunneling effects. Spin-ice materials are canonical examples of frustration, and Ising spins in a transverse magnetic field are the simplest many-body model of quantum tunneling. Here, we show that the tripod-kagome lattice material HoMgSbO unites an icelike magnetic degeneracy with quantum-tunneling terms generated by an intrinsic splitting of the Ho ground-state doublet, which is further coupled to a nuclear spin bath.

Ultrafast calculation of diffuse scattering from atomistic models.

Diffuse scattering is a rich source of information about disorder in crystalline materials, which can be modelled using atomistic techniques such as Monte Carlo and molecular dynamics simulations. Modern X-ray and neutron scattering instruments can rapidly measure large volumes of diffuse-scattering data. Unfortunately, current algorithms for atomistic diffuse-scattering calculations are too slow to model large data sets completely, because the fast Fourier transform (FFT) algorithm has long been considered unsuitable for such calculations [Butler & Welberry (1992).

Orbital Dimer Model for the Spin-Glass State in Y_{2}Mo_{2}O_{7}.

The formation of a spin glass generally requires that magnetic exchange interactions are both frustrated and disordered. Consequently, the origin of spin-glass behavior in Y_{2}Mo_{2}O_{7}-in which magnetic Mo^{4+} ions occupy a frustrated pyrochlore lattice with minimal compositional disorder-has been a longstanding question. Here, we use neutron and x-ray pair-distribution function (PDF) analysis to develop a disorder model that resolves apparent incompatibilities between previously reported PDF, extended x-ray-absorption fine structure spectroscopy, and NMR studies, and provides a new and physical explanation of the exchange disorder responsible for spin-glass formation.

Spin correlations in the dipolar pyrochlore antiferromagnet GdSnO.

We investigate spin correlations in the dipolar Heisenberg antiferromagnet GdSnO using polarised neutron-scattering measurements in the correlated paramagnetic regime. Using Monte Carlo methods, we show that our data are sensitive to weak further-neighbour exchange interactions of magnitude  ∼0.5% of the nearest-neighbour interaction, and are compatible with either antiferromagnetic next-nearest-neighbour interactions, or ferromagnetic third-neighbour interactions that connect spins across hexagonal loops.

Encoding complexity within supramolecular analogues of frustrated magnets.

The solid phases of gold(I) and/or silver(I) cyanides are supramolecular assemblies of inorganic polymer chains in which the key structural degrees of freedom-namely, the relative vertical shifts of neighbouring chains-are mathematically equivalent to the phase angles of rotating planar ('XY') spins. Here, we show how the supramolecular interactions between chains can be tuned to mimic different magnetic interactions. In this way, the structures of gold(I) and/or silver(I) cyanides reflect the phase behaviour of triangular XY magnets.

Hidden order in spin-liquid Gd₃Ga₅O₁₂.

Frustrated magnetic materials are promising candidates for new states of matter because lattice geometry suppresses conventional magnetic dipole order, potentially allowing "hidden" order to emerge in its place. A model of a hidden-order state at the atomic scale is difficult to deduce because microscopic probes are not directly sensitive to hidden order. Here, we develop such a model of the spin-liquid state in the canonical frustrated magnet gadolinium gallium garnet (Gd3Ga5O12).

SPINVERT: a program for refinement of paramagnetic diffuse scattering data.

We present a program (spinvert; http://spinvert.chem.ox.

Emergent frustration in co-doped β-Mn.

We investigate low-temperature spin correlations in the metallic frustrated magnet β-Mn1-xCox. Single-crystal polarized-neutron scattering experiments reveal the persistence of highly structured magnetic diffuse scattering and the absence of periodic magnetic order to T=0.05  K.

Empirical magnetic structure solution of frustrated spin systems.

Frustrated magnetism plays a central role in the phenomenology of exotic quantum states. However, since the magnetic structures of frustrated systems are often aperiodic, there has been the problem that they cannot be determined by using traditional crystallographic techniques. Here we show that the magnetic component of powder neutron scattering data is actually sufficiently information-rich to drive magnetic structure solution for frustrated systems, including spin ices, spin liquids, and molecular magnets.