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 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. The deposited data package contains neutron powder diffraction and single crystal inelastic neutron scattering data to probe the magnetic ordering and dynamics. The zip archive contains the data in the format of multi-column ASCII files, a README.txt that explains the content of all the files and matlab code to plot the data in all the files, together with relevant RGB colourmap.

Abstract:

We explore the magnetic excitations of the spin-1/2 triangular antiferromagnet Ba3CoSb2O9 in its 120 degree ordered phase using single-crystal high-resolution inelastic neutron scattering. Sharp magnons with no decay are observed throughout reciprocal space, with a strongly renormalized dispersion and multiple soft modes compared to linear spin wave theory. We propose an empirical parametrization that can quantitatively capture the complete dispersions in the three-dimensional Brillouin zone and explicitly show that the dispersion renormalizations have the direct consequence that one to two magnon decays are avoided throughout reciprocal space, whereas such decays would be allowed for the unrenormalized dispersions. At higher energies, we observe a very strong continuum of excitations with highly-structured intensity modulations extending up at least 4x the maximum one-magnon energy. The one-magnon intensities decrease much faster upon increasing energy than predicted by linear spin wave theory and the higher-energy continuum contains much more intensity than can be accounted for by a two-magnon cross-section, suggesting a significant transfer of spectral weight from the high-energy magnons into the higher-energy continuum states. We attribute the strong dispersion renormalizations and substantial transfer of spectral weight to continuum states to the effect of quantum fluctuations and interactions beyond the spin wave approximation, and make connections to theoretical approaches that might capture such effects. Finally, through measurements in a strong applied magnetic field, we find evidence for magnetic domains with opposite senses for the spin rotation in the 120 degree ordered ground state, as expected in the absence of Dzyaloshinskii-Moriya interactions, when the sense of spin rotation is selected via spontaneous symmetry breaking.