An in-depth study of the metal-organic magnet $\mathrm{Ni}{\left(\mathrm{TCNQ}\right)}_2$ was conducted where the deuterated form was synthesised both to attempt to alter the magnetic properties of the material and to be advantageous in techniques such as neutron scattering and muon spectroscopy. Deuteration saw a 3 K increase in $T_C$ with magnetization and heat capacity measurements demonstrating a spin wave contribution at low temperatures confirming the 3D nature of the ferromagnetic state shown by $\mathrm{Ni}{(\mathrm{TCNQ}-{\mathrm{D}}_4)}_2$. AC susceptibility results suggest there is a glassy component associated with the magnetically ordered state, though muon spectroscopy measurements did not support the presence of a spin glass state. Instead muon spectroscopy at zero magnetic field indicated the presence of two magnetic transitions, one at 20 K and another below 6 K; the latter is likely due to the system entering a quasistatic regime, similar to what one might expect of a superspin or cluster glass. Neutron diffraction measurements further supported this by revealing very weak magnetic Bragg peaks suggesting that the magnetism may have a short coherence length and be confined to small grains or clusters. The separation of the ferromagnetic and glassy magnetic components of the material's properties suggest that this system may show promise as a metal-organic magnet which is easily modified to change its magnetic properties, providing larger grain sizes can be synthesized.

• Received 24 February 2015
• Revised 15 October 2015

DOI:https://doi.org/10.1103/PhysRevB.92.184431