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

TL;DR

This study investigates the low-dimensional quantum magnetic properties of Cu(NCS)$_2$, revealing its structure, magnetic behavior, and quantum fluctuations through various experimental and theoretical methods.

Contribution

It provides the first detailed characterization of Cu(NCS)$_2$ as a two-dimensional antiferromagnetic system with quantum fluctuations, combining experimental and computational insights.

Findings

Cu(NCS)$_2$ behaves as a 2D array of weakly coupled antiferromagnetic spin chains.

The material orders antiferromagnetically below 12 K with a reduced magnetic moment.

Quantum fluctuations significantly suppress the ordered magnetic moment.

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, $\alpha = J_1/J_2 = 0.08$). 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 $\mu_\mathrm{B}$) due to quantum fluctuations.