Professor Stephen Blundell

Abstract:

Strong hydrogen bonds such as F···H···F offer new strategies to fabricate molecular architectures exhibiting novel structures and properties. Along these lines and, to potentially realize hydrogen-bond mediated superexchange interactions in a frustrated material, we synthesized [H2F]2[Ni3F6(Fpy)12][SbF6]2 (Fpy = 3-fluoropyridine). It was found that positionally-disordered H2F+ ions link neutral NiF2(Fpy)4 moieties into a kagome lattice with perfect 3-fold rotational symmetry. Detailed magnetic investigations combined with density-functional theory (DFT) revealed weak antiferromagnetic interactions (J ~ 0.4 K) and a large positive-D of 8.3 K with ms = 0 lying below ms = ±1. The observed weak magnetic coupling is attributed to bond-disorder of the H2F+ ions which leads to disrupted Ni-F···H-F-H···F-Ni exchange pathways. Despite this result, we argue that networks such as this may be a way forward in designing tunable materials with varying degrees of frustration.

Abstract:

The synthesis of the first 4d transition metal oxide-hydride, LaSr3 NiRuO4 H4 , is prepared via topochemical anion exchange. Neutron diffraction data show that the hydride ions occupy the equatorial anion sites in the host lattice and as a result the Ru and Ni cations are located in a plane containing only hydride ligands, a unique structural feature with obvious parallels to the CuO2 sheets present in the superconducting cuprates. DFT calculations confirm the presence of S=1/2  Ni+ and S=0, Ru2+ centers, but neutron diffraction and μSR data show no evidence for long-range magnetic order between the Ni centers down to 1.8 K. The observed weak inter-cation magnetic coupling can be attributed to poor overlap between Ni 3dz2 and H 1s in the super-exchange pathways.

Abstract:

LiOsO3 is the first example of a new class of material called a ferroelectric metal. We performed zero-field and longitudinal-field μSR, along with a combination of electronic structure and dipole field calculations, to determine the magneticground state of LiOsO3. We find that the sample contains both static Li nuclear moments and dynamic Os electronic moments. Below ≈0.7 K, the fluctuations of the Os moments slow down, though remain dynamic down to 0.08 K. We expect this could result in a frozen-out, disordered ground state at even lower temperatures.

Abstract:

We report the results of a muon-spin rotation ($\mu$SR) experiment to determine the superconducting ground state of the iron-based superconductor $CsCa_2Fe_4As_4F_2$ with $T_{\rm c} \approx 28.3\,K$. This compound is related to the fully-gapped superconductor $CaCsFe_4As_4$, but here the Ca-containing spacer layer is replaced with one containing $Ca_2F_2$. The temperature evolution of the penetration depth strongly suggests the presence of line nodes and is best modelled by a system consisting of both an $s-$ and a $d-$wave gap. We also find a potentially magnetic phase which appears below $\approx 10\,K$ but does not appear to compete with the superconductivity. This compound contains the largest alkali atom in this family of superconductors and our results yield a value for the in-plane penetration depth of $\lambda_{ab}(T=0)=423(5)\,nm$.