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Two-dimensional intrinsic ferromagnetic half-metal (HM) are important for thespintronics. Manipulating the interlayer magnetic coupling of van der Waalsmagnetic materials is an important method to control magnetoelectricproperties, which is especially useful for the spintronics. Here, based onsystematical research of CrGeTe3 (CGT) bilayer and multilayers with s ofself-intercalated (SI) Cr atom, we find that self-intercalation can enhance theinterlayer magnetic coupling. The super-exchange interaction still dominatesinterlayer magnetic exchange interaction, which results in ferromagneticcoupling between neighboring vdW layers. CGT bilayer keeps HM with FM orderafter Cr self-intercalation, independent of self-intercalated Cr (CrSI) atoms'concentration. Most importantly, self-intercalated CrGeTe3 (SI-CGT) bilayersshow ferromagnetic HM, independent of stacking orders. Moreover, SI-CGTmultilayers keep FM order, independent of films' thickness. However, SI-CGTmultilayers transform from HM into normal spin-polarized metal, as the statesat the Fermi-level increases. Moreover, magnetic anisotropy energy (MAE) ofSI-CGT-AA and SI-CGT-AB are -0.160 and -0.42 meV/.f.u., which are modulated byCrSI atoms. The MAE of SI-CGT-AA and SI-CGT-AB are different, as thehybridization interaction between Cr's d orbitals is different. SI-CGTmultilayers' magnetic easy axis (EA) switches from [001] of CGT to [100]direction, independent of stacking orders. It origins that MAE mainlycontributed by hybridization between Te atoms' px and py, py and pz orbitals isobvious weakened as CrSI is introduced. SI-CGT multilayers show good dynamical,thermal, and magnetic stability at 300 and 500 K. These findings find apromising way to manipulate interlayer exchange interaction and magnetoelectricproperties of CGT multilayers and other vdW magnets.

Tailing Magnetoelectric properties of Cr2Ge2Te6 by Engineering Covalently bonded Cr Self-intercalation: Ferromagnetic Half-metal