Molecular magnets based on ${\left[{\mathrm{Mo}}_3\right]}^{11+}$ units with one unpaired electron per trimer have attracted recent interest due to the identification of quantum spin liquid candidacy in some family members. Here, we present comprehensive measurements on polycrystalline samples of ${\mathrm{ZnScMo}}_3{\mathrm{O}}_8$, ${\mathrm{MgScMo}}_3{\mathrm{O}}_8$, and ${\mathrm{Na}}_3{\mathrm{Sc}}_2{\mathrm{Mo}}_5{\mathrm{O}}_{16}$ with the same ${\mathrm{Mo}}_3{\mathrm{O}}_{13}$ magnetic building blocks. The crystal structures are characterized with x-ray or neutron powder diffraction and the magnetic ground states are determined by performing ac and dc susceptibility, specific heat, neutron powder diffraction, and muon spin relaxation measurements. Our work indicates that ${\mathrm{ZnScMo}}_3{\mathrm{O}}_8$ and ${\mathrm{MgScMo}}_3{\mathrm{O}}_8$ have ferromagnetic Curie-Weiss temperatures of 18.5 and 11.9 K, ordered ground states with net moments (low-moment ferromagnetism or canted antiferromagnetism), and zero field ordering temperatures of $T_c=$ 6 K and $T_c<$ 2 K, respectively. On the other hand, ${\mathrm{Na}}_3{\mathrm{Sc}}_2{\mathrm{Mo}}_5{\mathrm{O}}_{16}$ hosts a dynamical magnetic ground state with no evidence for magnetic ordering or spin freezing down to 20 mK despite an antiferromagnetic Curie-Weiss temperature of $-36.2$ K, and therefore is a candidate for quantum spin liquid behavior. By comparing the present results to past work on the same family of materials, we construct a phase diagram which illustrates that the magnetic ground states of these Mo-based molecular magnets are very sensitive to small changes in the nearest-neighbor Mo-Mo distance.

• Received 4 March 2022
• Accepted 5 April 2022

DOI:https://doi.org/10.1103/PhysRevMaterials.6.044414