Low-dimensional quantum magnetism in Cu(NCS)${}_2$: A molecular framework material

Abstract

Low-dimensional magnetic materials with spin-$\frac{1}{2}$ moments can host a range of exotic magnetic phenomena due to the intrinsic importance of quantum fluctuations to their behavior. Here, we report the structure, magnetic structure and magnetic properties of copper(II) thiocyanate, Cu(NCS)${}_2$, a one-dimensional coordination polymer which displays low-dimensional quantum magnetism. Magnetic susceptibility, electron paramagnetic resonance (EPR) spectroscopy, ${}^{13}$C magic-angle spinning nuclear magnetic resonance (MASNMR) spectroscopy, and density functional theory (DFT) investigations indicate that Cu(NCS)${}_2$ behaves as a two-dimensional array of weakly coupled antiferromagnetic spin chains ($J_2=133(1)$ K, $\hat{I}\pm =J_1/J_2=0.08$). Powder neutron-diffraction measurements confirm that Cu(NCS)${}_2$ orders as a commensurate antiferromagnet below $T_{\mathrm{N}}=12$ K, with a strongly reduced ordered moment (0.3 $\hat{I}{¼}_{\mathrm{B}}$) due to quantum fluctuations.

11 pages, 7 figures