The Dzyaloshinskii-Moriya interaction (DMI), which originates from spin-orbit coupling and relies on broken inversion symmetry, is recognized as a key ingredient in forming magnetic skyrmions. However, most two-dimensional (2D) magnets exhibit inversion symmetry; therefore, the DMI is suppressed. Here, we propose a strategy to induce large DMI via lithium absorption on the surface of 2D magnets, an experimentally feasible approach. Using first-principles and atomistic spin simulations, we predict the formation of nanoscale skyrmions in lithium-decorated monolayer ${\mathrm{Fe}}_3{\mathrm{GeTe}}_2$ by imposing small out-of-plane magnetic fields ($B_z$). Notably, we find very large skyrmion energy barriers of more than 300 meV at $B_z=0.4\mathrm{T}$, comparable to those observed in ferromagnet/heavy-metal interfaces. The origin of these unique skyrmions is attributed to the competition between strong DMI, exchange frustration, and small magnetocrystalline anisotropy energy. We further show that the lifetimes of metastable skyrmions exceed 1 h for temperatures up to 75 K.

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• Electronic structure
• First-principles calculations
• Magnetic interactions
• Magnetism
• Skyrmions
• Magnetic systems
• Nanostructures
• Multiscale modeling