Complex Magnetic Phases and Unconventional Skyrmion Thermodynamics in Magnetically Intercalated Cr$_{1+x}$Te$_2$Compounds

Abstract

Chemical intercalation provides a powerful route for tuning the electronic and magnetic properties of transition metal dichalcogenides (TMDs), enabling the emergence of magnetic phases and phenomena that are otherwise inaccessible in their pristine forms. Here, we investigate the structural, electronic, and magnetic properties of magnetically intercalated Cr$_{1+x}$Te$_2$ through a combination of scanning tunneling microscopy, angle-resolved photoemission spectroscopy, magnetization, electrical transport, and Lorentz transmission electron microscopy measurements. We uncover a rich magnetic phase diagram comprising paramagnetic, in-plane spin-fluctuation, out-of-plane ferromagnetic, and field-induced Néel-type skyrmion phases. In particular, Lorentz transmission electron microscopy directly reveals the formation of Néel-type skyrmion textures slightly below the Curie temperature, with their configurations evolving strongly with temperature and magnetic field. The skyrmions exhibit pronounced thermal hysteresis and coexist with stripe domains, indicative of a complex magnetic energy landscape arising from the competition among disorder-induced local Dzyaloshinskii-Moriya interactions, perpendicular magnetic anisotropy, and dipolar interactions. Our results demonstrate that chemical intercalation can profoundly reshape the magnetic interactions and phase behavior of TMDs, establishing Cr$_{1+x}$Te$_2$ as a versatile platform for exploring tunable magnetism, skyrmion physics, and unconventional thermodynamic phenomena in low-dimensional quantum materials.