Dr Dharmalingam Prabhakaran

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.

Abstract:

Sustainable hydrogen production is attracting increasing attention and visible-light-driven water splitting is considered as one of the most promising approaches for hydrogen evolution and solar energy storage. Different materials have been screened at mild conditions in recent decades and 2-dimensional (2D) layered materials are considered good candidates for the photocatalytic water splitting reaction. 2D single layer MoS2 has shown its potential in various catalytic systems, and has also been used in photocatalytic water splitting reaction recently. However, current studies of MoS2 monolayers give low intrinsic activity, preventing it from practical applications. This is attributed to the rapid recombination of the photo-excited charge carriers at room temperature, resulting in poor quantum efficiency (QE). Herein, a state-of-the-art strategy to prolong the exciton lifetimes is reported, which is achieved by combining the 2D MoS2 nanosheets with solid state polar-faceted supports. The charge separation process can be facilitated by the strong local polarisation introduced by the polar-faceted supports, and tuned by changing the supports with different surface polarities. Polar oxide surface is the exposure of oxygen-terminated high energetic facet, which is known to give a net dipole moment perpendicular to its surface. Such variation in the surface properties of the support to the above metal would lead to a difference in metal-support interaction(s). The resulting composite structures show great enhancement toward the visible-light-driven photocatalytic water splitting reaction, giving hydrogen and oxygen evolution in a stoichiometric 2:1 ratio at elevated temperatures from pure water. Photocatalytic performances are improved by the prolonged exciton lifetimes and exceptional hydrogen evolution activity of 2977 μmol g−1 h−1 with impressive QEs are obtained over Ru-doped MoS2 nanosheets on polar ceria support, which is among the best of the reported results of similar catalytic systems to date. More excitingly, the linear relationship between the exciton lifetimes and strength of the local polarisation is also observed, indicating that the rational design of photocatalysts can be simply achieved via engineering their local polarisation by incorporation of polar-faceted materials.

Abstract:

The multiferroic perovskite rare earth manganites RMnO3 (R=Dy, Tb, Gd) are known as multiferroics exhibiting pressure-induced gigantic ferroelectric polarization. In this study, we have investigated the magnetic orderings in the pressure-induced phases for DyMnO3, by neutron diffraction and spherical neutron polarimetry (SNP) experiments up to 8.0 GPa. The magnetic ordering for Mn spins changes from the incommensurate bc-cycloid to the commensurate collinear E-type structure with kMn=0,12,0 above 4.0 GPa, which is concomitant with the appearance of a giant ferroelectric polarization. The magnetic ordering for the Dy spins has been determined to be a noncollinear spin structure with a and b spin components and kDy=(0,12,0) for the low- and high-pressure phases. The magnetic field along the a axis, Ha, affects the Dy ordering, which is seen in the changes in the k vector from kDy=(0,12,0) in Ha≤3T to kDy=(0,0,0) in Ha≥3T. Considering the lattice distortion generated by the determined magnetic orderings through the exchange striction mechanism, we conclude that the exchange striction for rare earth and Mn bonds, which is added to the uniform polarization generated by the E-type Mn ordering, is strongly related to the significant magnetic field enhancement of ferroelectric polarization in the high-pressure phase of the rare earth manganites.

Abstract:

Low-temperature thermal conductivity measurements have been conducted on an oxygen-annealed single crystal of Yb2Ti2O7 from 60 mK to 50 K and in magnetic fields up to 8 T applied in the [111] crystallographic direction. The temperature dependence of the conductivity in zero field shows a significant peak in thermal conductivity at T∼13 K and a sharp anomaly at Tc∼0.2 K suggesting that the sample's behavior is representative of the high-purity limit, with low levels of disorder. The magnetic field dependence of the thermal conductivity close to Tc reveals a reentrant magnetic phase for a field in the [111] direction. With this information, analysis of the very low magnetic field behavior of the thermal conductivity suggests the presence of significant fluctuations close to the phase line.