Synthesis and crystal growth

Abstract:

Recent theoretical proposals have argued that cobaltates with edge-sharing octahedral coordination can have significant bond-dependent exchange couplings thus offering a platform in 3d ions for such physics beyond the much-explored realizations in 4d and 5d materials. Here we present high-resolution inelastic neutron scattering data within the magnetically ordered phase of the stacked honeycomb magnet CoTiO3 revealing the presence of a finite energy gap and demonstrate that this implies the presence of bond-dependent anisotropic couplings. We also show through an extensive theoretical analysis that the gap further implies the existence of a quantum orderby-disorder mechanism that, in this material, crucially involves virtual crystal field fluctuations. Our data also provide an experimental observation of a universal winding of the scattering intensity in angular scans around linear band-touching points for both magnons and dispersive spin-orbit excitons, which is directly related to the non-trivial topology of the quasiparticle wavefunction in momentum space near nodal points.

Abstract:

Recent theoretical proposals have argued that cobaltates with edge-sharing octahedral coordination can have significant bond-dependent exchange couplings thus offering a platform in 3d ions for such physics beyond the much-explored realisations in 4d and 5d materials. Here we present high-resolution inelastic neutron scattering data within the magnetically ordered phase of the stacked honeycomb magnet CoTiO₃ revealing the presence of a finite energy gap and demonstrate that this implies the presence of bond-dependent anisotropic couplings. We also show through an extensive theoretical analysis that the gap further implies the existence of a quantum order-by-disorder mechanism that, in this material, crucially involves virtual crystal field fluctuations. Our data also provide an experimental observation of a universal winding of the scattering intensity in angular scans around linear band-touching points for both magnons and dispersive spin-orbit excitons, which is directly related to the non-trivial topology of the quasiparticle wavefunction in momentum space near nodal points.

Abstract:

We characterize experimentally and theoretically the high-energy dielectric screening properties of the prototypical correlated metal SrVO3. The dynamical structure factor measured by inelastic x-ray scattering spectroscopy as a function of momentum transfer is in very good agreement with first-principles calculations in the adiabatic local-density approximation to time-dependent density-functional theory. Our results reveal the crucial importance of crystal local fields in the charge response function of correlated materials: They lead to depolarization effects for localized excitations and couple spectra from different Brillouin zones.

Abstract:

Revealing the predominant driving force behind symmetry breaking in correlated materials is sometimes a formidable task due to the intertwined nature of different degrees of freedom. This is the case for La2−xSrxNiO4+δ, in which coupled incommensurate charge and spin stripes form at low temperatures. Here, we use resonant x-ray photon correlation spectroscopy to study the temporal stability and domain memory of the charge and spin stripes in La2−xSrxNiO4+δ. Although spin stripes are more spatially correlated, charge stripes maintain a better temporal stability against temperature change. More intriguingly, charge order shows robust domain memory with thermal cycling up to 250 K, far above the ordering temperature. These results demonstrate the pinning of charge stripes to the lattice and that charge condensation is the predominant factor in the formation of stripe orders in nickelates.

Abstract:

Current industrial production of ammonia from the Haber-Bosch process and its transport concomitantly produces a large quantity of CO2. Herein, we successfully synthesize inorganic-structure-based catalysts with [Fe-S2-Mo] motifs with a connecting structure similar to that of FeMoco (a cofactor of nitrogenase) by placing iron atoms on a single molecular layer of MoS2 at various loadings. This type of new catalytic material functionally mimics the nitrogenase to convert N2 to ammonia and hydrogen in water without adding any sacrificial agent under visible-light illumination. Using the elevated temperature boosts the ammonia yield and the energy efficiency by one order of magnitude. The solar-to-NH3 energy-conversion efficiency can be up to 0.24% at 270°C, which is the highest efficiency among all reported photocatalytic systems. This method of ammonia production and the photocatalytic materials may open up an exciting possibility for the decentralization of ammonia production for fertilizer provision to local farmlands using solar illumination.