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Published: 2011
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We nave measured the high-field magnetization of a number of Ni-based metal-organic molecular magnets. These materials are self-assembly coordination polymers formed from transition metal ions and organic ligands. The chemistry of the compounds is versatile allowing many structures with different magnetic properties to be formed. These studies follow on from previous measurements of the Cu-based analogues in which we showed it was possible to extract the exchange parameters of low-dimensional magnets using pulsed magnetic fields. In our recent experiments we have investigated the compound (Ni(HF2)(pyz)2)PF6, where pyz = pyrazine, and the Ni-ions are linked in a quasi-two-dimensional (Q2D) square lattice via the pyrazine molecules, with the layers held together by HF2 ligands. We also investigated Ni(NCS)2(pyzdo)2, where pyzdo = pyrazine dioxide. The samples are grown at Eastern Washington University using techniques described elsewhere. Measurements are performed at the pulsed magnetic field laboratory in Los Alamos. The magnetization of powdered samples is determined using a compensated coil magnetometer in a 65 T short pulse magnet. Temperatures as low as 500 mK are achievable using a 3He cryostat. The main figure shows the magnetization of the spin-1 [Ni(HF2)(pyz)2]PF6 compound at 1.43 K. The magnetization rises slowly at first, achieving a rounded saturation whose midpoint is around 19 T.A small anomaly is also seen in the susceptibility at low fields (≈3 T), which might be attributed to a spin-flop transition. In contrast, the spin-1/2 [Cu(HF2)(pyz)2]PF6 measured previously has a saturation magnetization of 35.5 T and a strongly concave form of M(B) below this field. This latter compound was shown to be a good example of a Q2D Heisenberg antiferromagnet with the strong exchange coupling (J{sub 2D} = 12.4 K, J{sub {perpendicular}}/J{sub 2D} ≈ 10−2) directed along the Cu-pyz-Cu directions. The structure of the two compounds is similar, but in the case of the Cu-compound the Cu-Cu pathways are linear, whereas in the Ni-compound they are kinked. The pulsed-field data combined with information from temperature-dependent susceptibility, muon-spin rotation, electron-spin resonance and ligand-field calculations suggest that, far from being magnetically Q2D, the Ni-compound is fairly one-dimensional with the dominant exchange (J{sub 1D} = 3.1 K and J{sub {perpendicular}}/J{sub 1D} = 0.63) directed along the Ni-FHF-Ni direction. Ni(NCS)2(pyzdo)2 was also investigated. Previous ultra-high field measurements using the 100 T magnet have shown that this compound has a saturation field close to 80 T. The purpose of the present studies is to map out the phase diagram of this material at mid-range fields. The data are shown in the inset to the figure. This continuing project probes the ability of organic ligands to mediate magnetic exchange, the link between structure, dimensionality and bulk magnetic properties, as well as the role of spin number in quantum magnets. Ultimately the investigations aim to determine to what extent it is possible to produce self-assembly molecular materials with tailor-made magnetic characteristics.
