The Duel of Magnetic Interactions & Structural Instabilities: Itinerant Frustration in the Triangular Lattice Compound LiCrSe$_2$

The recent synthesis of the chromium selenide compound LiCrSe$_2$ constitutes a valuable addition to the ensemble of two-dimensional triangular lattice antiferromagnets (2D-TLA). In this work we present the very first comprehensive study of the combined low temperature nuclear and magnetic structure established in this material. Details on the connection between Li-ion dynamics and structural changes are also presented along with a direct link between atomic structure and spin order via a strong magnetoelastic coupling. LiCrSe$_2$ was found to undergo a first order structural transition from a trigonal crystal system with space group $P\bar{3}m1$ to a monoclinic one with space group $C2/m$ at $T_{\rm s}=30$~K. Such restructuring of the lattice is accompanied by a magnetic transition at $T_{\rm N}=30$~K, with the formation of a complex spin arrangement for the Cr$^{3+}$ moments. Refinement of the magnetic structure with neutron diffraction data and complementary muon spin rotation analysis reveal the presence of two incommensurate magnetic domains with a up-up-down-down arrangement of the spins with ferromagnetic (FM) double chains coupled antiferromagnetically (AFM). In addition to this unusual arrangement, the spin axial vector is modulated both in direction and modulus, resulting in a spin density wave-like order with periodic suppression of the Cr moment along the chains. This behavior is believed to appear as a result of strong competition between direct exchange AFM and superexchange FM couplings established between both nearest neighbor and next nearest neighbor Cr$^{3+}$ ions. We finally conjecture that the resulting magnetic order is stabilized via subtle vacancy/charge order within the Li layers, potentially causing a mix of two different magnetic phases within the sample.