Spontaneous Enhancement of Dzyaloshinskii-Moriya Interaction via Field-Cooling-Induced Interface Engineering in 2D van der Waals Ferromagnetic ternary Tellurides

The emergence of two-dimensional (2D) van der Waals (vdW) ferromagnets has opened new avenues for exploring topological spin textures and their applications in next-generation spintronics. Among these materials, Fe3GaTe2 (FGaT) emerges as a model system due to its room-temperature skyrmion phases, which are stabilized by strong Dzyaloshinskii-Moriya interaction (DMI). However, the atomistic origins of DMI in centrosymmetric vdW lattices remain elusive. Here, we report a spontaneous DMI enhancement mechanism driven by FC in FGaT and its analog Fe3GeTe2 (FGeT). Combining Raman spectroscopy and scanning transmission electron microscopy (STEM), we have observed the irreversible precipitation of FeTe2 in annealed FGaT. The resulting FeTe2/FGaT heterostructure is considered to break the symmetry and significantly enhance the DMI. Furthermore, similar phenomenon has been observed in the family ferromagnetic material FGeT as well. Additionally, the precipitation of FeTe2 varies significantly with different thicknesses of FGaT, aligning closely with the reported behavior of skyrmions. This discovery provides new insights into the mechanisms behind the origin of the DMI in ternary tellurides, paving the way for advanced spintronic applications.