Synthesis and physical properties of low dimensional quantum magnets

Strong electron correlation lies at the root of many quantum collective phenomena observed in solids, including high Tc superconductivity. Theoretically, the problem of many interacting electrons is difficult to treat, however, and a microscopic understanding of strongly correlated systems remains one of the foremost challenges in modern physics. A particularly clean realisation of this general problem is found in magnetic systems, where theory and experiment are both well developed and complementary. The role of the chemist in this endeavour is to provide model experimental systems to both inspire new developments in theory and to confirm existing predictions. This thesis aims to demonstrate aspects of both synthesis and physical characterisation of such model systems, with particular emphasis on materials which exhibit unusual quantum ground states due to a combination of reduced dimensionality, low spin, and geometric frustration. Four materials are considered: The first among these is a new material, KTi(SO4)2·(H2O), which was prepared using a hydrothermal route, and characterised by magnetic susceptibility, specific heat, and high field magnetisation measurements. Fitting exact diagonalisation and series expansion results to these data imply that KTi(SO4)2·(H2O)is a long-sought experimental realization of the S = 1/2 Heisenberg frustrated (J1 − J2) chain model in the dimerised regime of the phase diagram. The anhydrous analogue of KTi(SO4)2·(H2O), KTi(SO4)2, was also investigated, and found by magnetic neutron scattering to exemplify the S = 1/2 Heisenberg anisotropic triangular lattice model in the 1D chain limit. The final two materials discussed are the naturally occurring minerals volborthite and herbertsmithite, both thought to realise the S = 1/2 Heisenberg kagome antiferromagnet model. Diffuse and inelastic magnetic neutron scattering experiments, however, indicate that the kagome physics are partially destroyed by defects in the former and lattice distortion in the latter

Polarized neutron powder diffraction studies of antiferromagnetic order in bulk and nanoparticle NiO

In many materials it remains a challenge to reveal the nature of magnetic correlations, including antiferromagnetism and spin disorder. Revealing the spin structure in magnetic nanoparticles is further complicated by the large incoherent neutron scattering cross section from water adsorbed at the particle surfaces and by the broadening of diffraction peaks due to the finite crystallite size. Moreover, the spin structure in magnetic nanoparticles may deviate significantly from that of the corresponding bulk material because of the low-symmetry surroundings of surface atoms and the large relative surface contribution to the magnetic anisotropy. Here we explore the potential use of polarized neutron diffraction to reveal the magnetic structure in NiO bulk and nanoparticle powders by applying the XYZ-polarization analysis method. Our investigations address in particular the spin orientation in bulk NiO and platelet-shaped NiO nanoparticles with thickness from greater than 200 nm down to 2.0 nm. The advantage of the applied method is that it is able to clearly separate the structural, the magnetic, and the spin-incoherent scattering signals for all particle sizes. For platelet-shaped particles with thickness from greater than 200 nm down to 2.2 nm we find that the spin orientation deviates about 16 degrees from the primary (111) plane of the platelet-shaped particles. In the smallest particles (2.0 nm thick) we find the spins are oriented with a 30 degrees. average angle to the primary (111) plane of the particles. The results show that polarization analyzed neutron powder diffraction is a viable method to investigate magnetic order in powders of antiferromagnetic nanoparticles

SHERPA: A Spectrometer with High Energy Resolution and Polarisation Analysis

SHERPA is a proposed quasielastic neutron spectrometer with polarisation analysis, intended to replace the ageing Iris instrument at the ISIS neutron and muon source. In this paper we present a concept of the instrument along with Monte-Carlo simulations and analysis of possible instrument location. We expect greatly increased count rate compared to Iris (expected from 49 to 660 × Iris) in unpolarised mode and dedicated polarisation analysis capabilities at a more modest count rate increase (~5-70 × Iris). This huge gain in the count rate would be achieved from the combination of three factors: modern neutron guide with high-m coating, and prismatic effect and larger solid angle coverage at the energy analyser. Such an instrument would be the first of its kind and has incredible potential to revolutionise quasielastic neutron scattering technique through the separation of the coherent and incoherent scattering contributions