Raman fingerprints of spin-phonon coupling and magnetic transition in an organic molecule intercalated Cr2Ge2Te6
arxiv(2023)
摘要
The manipulation of spin-phonon coupling in both formations and explorations
of magnetism in two-dimensional van der Waals ferromagnetic semiconductors
facilitates unprecedented prospects for spintronics devices. The interlayer
engineering tunes spin-phonon coupling significantly and holds the promise for
controllable magnetism via organic cation intercalation. Here, we present
spectroscopic evidence to reveal the intercalation effect on intrinsic magnetic
and electronic transitions in quasi-two-dimensional Cr2Ge2Te6 using tetrabutyl
ammonium as the intercalant. The temperature-evolution of Raman modes E_g^3 and
A_g^1, along with the magnetization measurements, unambiguously captures the
enhancement of the ferromagnetic Curie temperature in the intercalated
heterostructure. Moreover, the E_g^4 mode highlighted the increased effect of
spin-phonon interaction in magnetic order-induced lattice distortion. Combined
with the first-principle calculations, we observed a substantial number of
electrons transferred from TBA+ to Cr through the interface. These results
provide the interplay between spin-phonon coupling and magnetic ordering in van
der Waals magnets where Raman fingerprints would be highly beneficial for
further understanding the manipulation of magnetism in layered
heterostructures.
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