Dynamical electronic correlation and chiral magnetism in van der Waals magnet Fe4GeTe2

Among the quasi-2D van der Waals magnetic systems, Fe4GeTe2 imprints a profound impact due to its near-room temperature ferromagnetic behaviour and the complex magnetothermal phase diagram exhibiting multiple phase transformations, as observed from magnetization and magnetotransport measurements. A complete analysis of these phase transformations in the light of electronic correlation and its impact on the underlying magnetic interactions remain unattended in the existing literature. Using first-principles methodologies, incorporating the dynamical nature of electron correlation, we have analysed the interplay of the direction of magnetization in the easy-plane and easy-axis manner with the underlying crystal symmetry, which reveals the opening of a pseudogap feature beyond the spin-reorientation transition (SRT) temperature. The impact of dynamical correlation on the calculated magnetic circular dichroism and x-ray absorption spectrum of the L-edge of the Fe atoms compared well with the existing experimental observations. The calculated intersite Heisenberg exchange interactions display a complicated nature, depending upon the pairwise interactions among the two inequivalent Fe sites, indicating a RKKY-like behaviour of the magnetic interactions. We noted the existence of significant anisotropic and antisymmetric exchanges interactions, resulting into a chirality in the magnetic behaviour of the system. Subsequent investigation of the dynamical aspects of magnetism in Fe4GeTe2 and the respective magnetothermal phase diagram reveal that the dynamical nature of spins and the decoupling of the magnetic properties for both sites of Fe is crucial to explain all the experimentally observed phase transformations.