Two-dimensional overdamped fluctuations of the soft perovskite lattice in CsPbBr3.

Lead halide perovskites exhibit structural instabilities and large atomic fluctuations thought to impact their optical and thermal properties, yet detailed structural and temporal correlations of their atomic motions remain poorly understood. Here, these correlations are resolved in CsPbBr3 crystals using momentum-resolved neutron and X-ray scattering measurements as a function of temperature, complemented with first-principles simulations. We uncover a striking network of diffuse scattering rods, arising from the liquid-like damping of low-energy Br-dominated phonons, reproduced in our simulations of the anharmonic phonon self-energy. These overdamped modes cover a continuum of wave vectors along the edges of the cubic Brillouin zone, corresponding to two-dimensional sheets of correlated rotations in real space, and could represent precursors to proposed two-dimensional polarons. Further, these motions directly impact the electronic gap edge states, linking soft anharmonic lattice dynamics and optoelectronic properties. These results provide insights into the highly unusual atomic dynamics of halide perovskites, relevant to further optimization of their optical and thermal properties.

Dynamical ground state in the XY pyrochlore Yb2GaSbO7.

The magnetic ground state of the pyrochlore Yb2GaSbO7 has remained an enigma for nearly a decade. The persistent spin fluctuations observed by muon spin relaxation measurements at low temperatures have not been adequately explained for this material using existing theories for quantum magnetism. Here we report on the synthesis and characterisation of Yb2GaSbO7 to elucidate the central physics at play. Through DC and AC magnetic susceptibility, heat capacity, and neutron scattering experiments, we observe evidence for a dynamical ground state that makes Yb2GaSbO7 a promising candidate for disorder-induced spin-liquid or spin-singlet behaviour. This state is quite fragile, being tuned to a splayed ferromagnet in a modest magnetic field µ0Hc∼1.5T.

Magnetic ordering and structural distortion in a PrFeAsO single crystal studied by neutron and x-ray scattering.

We report the magnetic ordering and structural distortion in PrFeAsO crystals, the basis compound for one of the oxypnictide superconductors, using high-resolution x-ray diffraction, neutron diffraction, and x-ray resonant magnetic scattering (XRMS). We find the structural tetragonal-to-orthorhombic phase transition at TS=147K, the AFM phase transition of the Fe moments at TFe=72K, and the Pr AFM phase transition at TPr=21K. Combined high-resolution neutron diffraction and XRMS show unambiguously that the Pr moments point parallel to the longer orthorhombic a axis and order antiferromagnetically along the a axis but ferromagnetically along the b and c directions in the stripelike AFM order. The temperature-dependent magnetic order parameter of the Pr moments shows no evidence for a reorientation of moments.

Extended anharmonic collapse of phonon dispersions in SnS and SnSe.

The lattice dynamics and high-temperature structural transition in SnS and SnSe are investigated via inelastic neutron scattering, high-resolution Raman spectroscopy and anharmonic first-principles simulations. We uncover a spectacular, extreme softening and reconstruction of an entire manifold of low-energy acoustic and optic branches across a structural transition, reflecting strong directionality in bonding strength and anharmonicity. Further, our results solve a prior controversy by revealing the soft-mode mechanism of the phase transition that impacts thermal transport and thermoelectric efficiency. Our simulations of anharmonic phonon renormalization go beyond low-order perturbation theory and capture these striking effects, showing that the large phonon shifts directly affect the thermal conductivity by altering both the phonon scattering phase space and the group velocities. These results provide a detailed microscopic understanding of phase stability and thermal transport in technologically important materials, providing further insights on ways to control phonon propagation in thermoelectrics, photovoltaics, and other materials requiring thermal management.

Competing Magnetic Interactions in the Antiferromagnetic Topological Insulator MnBi_{2}Te_{4}.

The antiferromagnetic (AFM) compound MnBi_{2}Te_{4} is suggested to be the first realization of an AFM topological insulator. We report on inelastic neutron scattering studies of the magnetic interactions in MnBi_{2}Te_{4} that possess ferromagnetic triangular layers with AFM interlayer coupling. The spin waves display a large spin gap and pairwise exchange interactions within the triangular layer are long ranged and frustrated by large next-nearest neighbor AFM exchange. The degree of frustration suggests proximity to a variety of magnetic phases, potentially including skyrmion phases, which could be accessed in chemically tuned compounds or upon the application of symmetry-breaking fields.

Structural features associated with multiferroic behavior in the RX3(BO3)4 system.

The magnetoelectric effect in the RX3(BO3)4 system (R = Ho, Eu, Sm, Nd, Gd; X = Fe, Al) varies significantly with the cation R despite very similar structural arrangements. Our structural studies reveal a symmetry reducing tilting of the BO3 planes and of the FeO6 polyhedra in the systems exhibiting low magnetic field induced electric polarization. Neutron scattering measurements reveal a lack of magnetic ordering indicating the primary importance of the atomic structure in the multiferroic behavior of this system.

Spin Stripe Order in a Square Planar Trilayer Nickelate.

Trilayer nickelates, which exhibit a high degree of orbital polarization combined with an electron count (d^{8.67}) corresponding to overdoped cuprates, have been identified as a promising candidate platform for achieving high-T_{c} superconductivity. One such material, La_{4}Ni_{3}O_{8}, undergoes a semiconductor-insulator transition at ∼105 K, which was recently shown to arise from the formation of charge stripes. However, an outstanding issue has been the origin of an anomaly in the magnetic susceptibility at the transition and whether it signifies the formation of spin stripes akin to single layer nickelates. Here we report single crystal neutron diffraction measurements (both polarized and unpolarized) that establish that the ground state is indeed magnetic. The ordering is modeled as antiferromagnetic spin stripes that are commensurate with the charge stripes, the magnetic ordering occurring in individual trilayers that are essentially uncorrelated along the crystallographic c axis. A comparison of the charge and spin stripe order parameters reveals that, in contrast to single-layer nickelates such as La_{2-x}Sr_{x}NiO_{4} as well as related quasi-2D oxides including manganites, cobaltates, and cuprates, these orders uniquely appear simultaneously, thus demonstrating a stronger coupling between spin and charge than in these related low-dimensional correlated oxides.

Disordered Route to the Coulomb Quantum Spin Liquid: Random Transverse Fields on Spin Ice in Pr_{2}Zr_{2}O_{7}.

Inelastic neutron scattering reveals a broad continuum of excitations in Pr_{2}Zr_{2}O_{7}, the temperature and magnetic field dependence of which indicate a continuous distribution of quenched transverse fields (Δ) acting on the non-Kramers Pr^{3+} crystal field ground state doublets. Spin-ice correlations are apparent within 0.2 meV of the Zeeman energy. A random phase approximation provides an excellent account of the data with a transverse field distribution ρ(Δ)∝(Δ^{2}+Γ^{2})^{-1}, where Γ=0.27(1) meV. Established during high temperature synthesis due to an underlying structural instability, it appears disorder in Pr_{2}Zr_{2}O_{7} actually induces a quantum spin liquid.