Professor Stephen Blundell

Abstract:

We present an investigation of the effect of randomizing exchange coupling strengths in the S=1/2 square lattice quasi-two-dimensional quantum Heisenberg antiferromagnet (QHAF) (QuinH)2Cu(ClxBr1-x)4·2H2O (QuinH = Quinolinium, C9H8N+), with 0≤x≤1. Pulsed-field magnetization measurements allow us to estimate an effective in-plane exchange strength J in a regime where exchange fosters short-range order, while the temperature TN at which long-range order (LRO) occurs is found using muon-spin relaxation, allowing us to construct a phase diagram for the series. We evaluate the effectiveness of disorder in suppressing TN and the ordered moment size, and we find an extended disordered phase in the region 0.4≲x≲0.8 where no magnetic order occurs. The observed critical substitution levels are accounted for by an energetics-based competition between different local magnetic orders. Furthermore, we demonstrate experimentally that the ground-state disorder is driven by quantum effects of the exchange randomness, which is a feature that has been predicted theoretically and has implications for other disordered quasi-two-dimensional QHAFs.

Abstract:

We report magnetic, transport, neutron diffraction, and muon spin rotation data showing that Pb2CoOsO6, a metallic double-perovskite with a centrosymmetric space group at room temperature exhibits a continuous second-order phase transition at 45 K to a magnetically ordered state with a noncentrosymmetric space group. The absence of inversion symmetry is very uncommon in metals, particularly metallic oxides. In contrast to the recently reported ferroelectriclike structural transition in LiOsO3, the phase transition in Pb2CoOsO6 is driven by a long-range collinear antiferromagnetic order, with propagation vector k=(12,0,12), which relieves the frustration associated with the symmetry of the magnetic exchanges. This magnetically driven loss of inversion symmetry represents another frontier in the search for novel metallic behavior.

Abstract:

© 2020 authors. We report on a comprehensive characterization of the newly synthesized Cu2+-based molecular magnet [Cu(pz)2(2-HOpy)2](PF6)2 (CuPOF), where pz=C4H4N2 and 2-HOpy=C5H4NHO. From a comparison of theoretical modeling to results of bulk magnetometry, specific heat, μ+SR, ESR, and NMR spectroscopy, this material is determined as an excellent realization of the two dimensional square-lattice S=12 antiferromagnetic Heisenberg model with a moderate intraplane nearest-neighbor exchange coupling of J/kB=6.80(5) K, and an extremely small interlayer interaction of about 1 mK. At zero field, the bulk magnetometry reveals a temperature-driven crossover of spin correlations from isotropic to XY type, caused by the presence of a weak intrinsic easy-plane anisotropy. A transition to long-range order, driven by the low-temperature XY anisotropy under the influence of the interlayer coupling, occurs at TN=1.38(2) K, as revealed by μ+SR. In applied magnetic fields, our H1-NMR data reveal a strong increase of the magnetic anisotropy, manifested by a pronounced enhancement of the transition temperature to commensurate long-range order at TN=2.8 K and 7 T.