Synthesis and Anisotropic Magnetic Properties of LiCrTe$_2$ Single Crystals with a Triangular-Lattice Antiferromagnetic Structure

Abstract: We report on the synthesis of LiCrTe$2$ single crystals and on their anisotropic magnetic properties. We have obtained these single crystals by employing a Te/Li-flux synthesis method. We find LiCrTe$_2$ to crystallize in a TlCdS$_2$ -type structure with cell parameters of $a$ = 3.9512(5) \r{A} and $c$ = 6.6196(7) \r{A} at $T$ = 175 K. The content of lithium in these crystals was determined to be near stoichiometric by means of neutron diffraction. We find a pronounced magnetic transition at $T^{\rm ab}{\rm N}$ = 144 K and $T^{\rm c}{\rm N}$ = 148 K, respectively. These transition temperatures are substantially higher than earlier reports on polycrystalline samples. We have performed neutron powder diffraction measurements that reveal that the long-range low-temperature magnetic structure of single crystalline LiCrTe$_2$ is an A-type antiferromagnetic (AFM) structure. Our DFT calculations are in good agreement with these experimental observations. We find the system to be easy axis with moments oriented along the $c$-direction experimentally as well as in our calculations. Thereby, the magnetic Hamiltonian can be written as $H = H{\rm Heisenberg} + \sum_i K_c (S_i^z)^2$ with $K_c=-0.34K$ (where $|S^z|=\frac{3}{2}$). We find LiCrTe$2$ to be highly anisotropic, with a pronounced metamagnetic transition for $H \perp ab$ with a critical field of $\mu H{MM}$(5 K) $\approx$ 2.5 T. Using detailed orientation-dependent magnetization measurements, we have determined the magnetic phase diagram of this material. Our findings suggest that LiCrTe$_2$ is a promising material for exploring the interplay between crystal structure and magnetism, and could have potential applications in spin-based 2D devices.