Solvothermal synthesis was used to create a low-dimensional iron(II)-chloride-formate compound, NH4FeCl2(HCOO), that exhibits interesting magnetic properties. NH4FeCl2(HCOO) crystallizes in the monoclinic space group C2/c (No. 15) with a = 7.888(1) Å, b = 11.156(2) Å, c = 6.920(2) Å, and β = 108.066(2)°. The crystal structure consists of infinite zig-zag chains of distorted Fe2+-centered octahedra linked by μ2-Cl and syn-syn formate bridges, with inter-chain hydrogen bonding through NH4+ cations holding the chains together. The unique Fe2+ site is coordinated by four equatorial chlorides at a distance of 2.50 Å and two axial oxygens at a distance of 2.08 Å. Magnetic measurements performed on powder and oriented single crystal samples show complex anisotropic magnetic behavior dominated by antiferromagnetic interactions (TN = 6 K) with a small ferromagnetic component in the direction of chain propagation. An anisotropic metamagnetic transition was observed in the ordered state at 2 K in an applied magnetic field of 0.85-3 T. 57Fe Mössbauer spectroscopy reveals mixed hyperfine interactions below the ordering temperature with strong electric field gradients and complex non-collinear arrangement of the magnetic moments.
An isostructural series of transition metalformate-chloride-hydrate compounds, M 3 (OOCH) 5 Cl(OH 2 ) (M = Fe, Co, Ni), have been synthesized using a solvothermal method. These compounds crystallize in the chiral and polar space group P3 1 and are comprised of three different types of helical chains of edge-sharing M 2+ -centered octahedra. All three compounds undergo 3D ferrimagnetic ordering at low temperature, and the iron and cobalt analogues exhibit fieldinduced metamagnetic transitions. The magnetic structure was determined by neutron powder diffraction, revealing ferromagnetic intrachain coupling and antiferromagnetic interchain interactions, with the three chains arranged in a two-up/onedown triangular lattice. As all three chains contain one type of metal in the same spin state, these compounds are rare examples of homospin topological ferrimagnets.
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