Our estimates of the interactions creating the noncollinear spin structures only provide an initial understanding. Future measurements will give access to more precise quantification of the underlying origin of this phenomenon: allowing us to measure the relevant higher-order interactions directly. Inelastic neutron scattering measurements, whether on single crystals or powders, would provide precise measurements of the magnetic excitations and hence J Cl , J L , J vdW and D, together with indications of deviations from these terms. High field EPR and single-crystal magnetometry measurements would accurately measure D and E. Calculations using dynamical mean-field theory (DMFT) and multiconfigurational methods (e.g. CASSCF) would allow for appropriate treatment of the electron correlation and spinorbit contributions (respectively). Our model suggests that the noncollinearity in these materials can be enhanced through further desymmetrisation of the ligand field environment: replacing the N-heterocycle with a stronger field ligand or the bridging halide with a weaker field should increase the canting angle. Equally, the geometry of the organic ligand can be used to control the noncollinearity, and a ligand that tilts the metal halide chains more would produce a larger canting angle. In particular, we note that the tilt angle for pym is 32 • : if this angle can be increased to ϕ = 45 • , a tetrastable state would be realisable. This strategy for realising noncollinear magnetism can be generalised to other metal-organic magnets where single ion anisotropy orientation can be anticipated.