Magnetic Ordering in the Frustrated Heisenberg Chain System Cupric Chloride, CuCl₂

We report a detailed examination the magnetic structure of anhydrous cupric chloride CuCl2 carried out by powder neutron diffraction, magnetic susceptibility and specific heat measurements on polycrystalline and single crystal samples as well as an evaluation of the spin exchange interactions by first principles density functional theory (DFT) calculations. Anhydrous CuCl2 shows one dimensional antiferromagnetic behavior and long range antiferromagnetic ordering below a Neel temperature of 23.9 K. Neutron powder and single crystal diffraction reveal that, below 23.9K, CuCl2 undergoes a phase transition into an incommensurate magnetic structure (propagation vector (1,0.2257,0.5) with a spin-spiral propagating along b and the moments confined in the bc crystallographic plane. Our DFT calculations show that the spin-spiral results from competing ferromagnetic nearest neighbor and antiferromagnetic next-nearest neighbor spin-exchange interaction along the spin chains. Implications for possible multiferroic behavior of CuCl2 are discussed.