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Metal-organic magnets (MOMs), modular magnetic materials where metal atomsare connected by organic linkers, are promising candidates for next-generationquantum technologies. MOMs readily form low-dimensional structures, and so areideal systems to realise physical examples of key quantum models, including theHaldane phase, where a topological excitation gap occurs in integer-spinantiferromagnetic (AFM) chains. Thus far the Haldane phase has only beenidentified for $S=1$, with $S \geq 2$ still unrealised because the larger spinimposes more stringent requirements on the magnetic interactions. Here, wereport the structure and magnetic properties of CrCl$_2$(pym) (pym=pyrimidine),a new quasi-1D $S=2$ AFM MOM. We show, using X-ray and neutron diffraction,bulk property measurements, density-functional theory calculations andinelastic neutron spectroscopy (INS) that CrCl$_2$(pym) consists of AFMCrCl$_2$ spin chains ($J_1=-1.13(4)\;$meV) which are weakly ferromagneticallycoupled through bridging pym ($J_2=0.10(2)\;$meV), with easy-axis anisotropy($D=-0.15(3)\;$meV). We find that although small compared to $J_1$, theseadditional interactions are sufficient to prevent observation of the Haldanephase in this material. Nevertheless, the proximity to the Haldane phasetogether with the modularity of MOMs suggests that layered Cr(II) MOMs are apromising family to search for the elusive $S=2$ Haldane phase.

Low-dimensional metal-organic magnets as a route towards the S=2 Haldane phase