Tailing the Magnetoelectric Properties of Cr2Ge2Te6 by Engineering Covalently Bonded Cr Self-Intercalation: Ferromagnetic Half-Metal Tailing the Magnetoelectric Properties of Cr2Ge2Te6 by Engineering Covalently Bonded Cr Self-Intercalation: Ferromagnetic Half-Metal AITranslate

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DOI：https://doi.org/10.1021/acsaelm.2c01749

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Two-dimensional intrinsic ferromagnetic half-metals (HMs) are important for spintronics. Based on a systematic research of CrGeTe3 (CGT) bilayers and multilayers with the self-intercalated (SI) Cr (CrSI) atom, we find that self-intercalation can enhance interlayer magnetic coupling, which results in a super-exchange interaction between interlayers. The CGT bilayer keeps half-metallicity with the interlayer ferromagnetic (FM) order after Cr’s self-intercalation, independent of CrSI atoms’ concentration and stacking orders. Moreover, SI-CGT multilayers with interlayer FM order transform from HMs into normal spin-polarized metals, as the states at the Fermi level increase. Moreover, the magnetic anisotropy energies (MAEs) of SI-CGT-AA and SI-CGT-AB are −0.160 and −0.42 meV/f.u., respectively, which are modulated by the CrSI atoms. The MAEs of SI-CGT-AA and SI-CGT-AB are different, as the hybridization interactions between Cr’s d orbitals are different from each other. SI-CGT bilayers’ magnetic easy axis (EA) switches from the original [001] of CGT to the [100] direction, independent of the stacking orders. It is inferred that the MAE is mainly contributed by the hybridization between Te’s px and py, py and pz orbitals, and that this hybridization interaction is obviously weakened as CrSI atom is inserted. The SI-CGT bilayers and multilayers show good dynamic and thermal stability at 300 and 500 K. These findings offer a promising way to manipulate the interlayer exchange interaction and magnetoelectric properties of CGT multilayers and other vdW magnets.