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Chiral magnetic states in two-dimensional (2D) layered noncentrosymmetricmagnets, which are promising advanced spintronic materials, are usuallyattributed to Dzyaloshinskii-Moriya interactions (DMI). However, the role ofunderlying higher-order spin couplings in determining the properties of chiralspin textures has much less reported. In this work, taking thelithium-decorated monolayer CrTe$_{2}$ (monolayer LiCrTe$_{2}$) as an example,we develop a first-principles-based comprehensive spin model constructed byusing the symmetry-adapted cluster expansion method. Based on this spin model,we identify the ground state of monolayer LiCrTe$_{2}$ as a chiral spin spiralstate, which can further assemble macroscopic chiral labyrinth domains (LD)under zero-field conditions as well as evolve into skyrmions under a finitemagnetic field. Moreover, higher-order biquadratic and three-site interactionsare identified to be responsible for modulating both the size and the fieldstability of the spin spiral state. Our study sheds light on complex magneticcouplings in 2D magnets.

Chiral magnetism in lithium-decorated monolayer CrTe$_{2}$: Interplay between Dzyaloshinskii-Moriya interaction and higher-order interactions