Metal–organic magnets (MOMs), modular magnetic
materials
where metal atoms are connected by organic linkers, are promising
candidates for next-generation quantum technologies. MOMs readily
form low-dimensional structures and so are ideal systems to realize
physical examples of key quantum models, including the Haldane phase,
where a topological excitation gap occurs in integer-spin antiferromagnetic
(AFM) chains. Thus, far the Haldane phase has only been identified
for S = 1, with S ≥ 2 still
unrealized because the larger spin imposes more stringent requirements
on the magnetic interactions. Here, we report the structure and magnetic
properties of CrCl2(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,
and inelastic neutron spectroscopy (INS), that CrCl2(pym)
consists of AFM CrCl2 spin chains (J
1 = −1.13(4) meV) which are weakly ferromagnetically
coupled 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, these additional interactions are sufficient to prevent
observation of the Haldane phase in this material. Nevertheless, the
proximity to the Haldane phase together with the modularity of MOMs
suggests that layered Cr(II) MOMs are a promising family to search
for the elusive S = 2 Haldane phase.