$\left[{{(}^i{C}_3{H}_7)}_{2}N{H}_2\right]\left[C{r}_{8}Ni{F}_9{\left(O_{2}CCMe\right)}_{18}\right]$, or $C{r}_{8}Ni$, is a prominent example of an odd-membered antiferromagnetic “wheel.” A detailed characterization of the magnetic properties of $C{r}_{8}Ni$ has been conducted. Inelastic neutron scattering (INS) is used to investigate the energy and momentum transfer dependence of the low-lying spin excitations, including excited states inaccessible by other experimental techniques. The richness of the INS data, in conjunction with microscopic spin Hamiltonian simulations, enables an accurate characterization of the magnetic properties of $C{r}_{8}Ni$. Nearest-neighbor exchange constants of $J_{\mathrm{CrCr}}$ = 1.31 meV and $J_{\mathrm{CrNi}}$ = 3.22 meV are determined, and clear evidence of axial single-ion anisotropy is found. The parameters determined by INS are shown to fit magnetic susceptibility. The spectroscopic identification of several successive $S=1$ excited total spin states and lowest spin band excitations show that the rotational band picture, valid for bipartite AFM wheels, breaks down for this odd-numbered wheel. The exchange constants determined here differ from previous efforts based on bulk measurements, and possible reasons are discussed. The large $J_{\mathrm{CrNi}}/J_{\mathrm{CrCr}}$ ratio in $C{r}_{8}Ni$ puts this wheel into a regime with strong quantum fluctuations in which the ground state can be described with a valence bond solid state picture.

• Received 11 May 2012

DOI:https://doi.org/10.1103/PhysRevB.86.064405