UC Berkeley

Recent experiments on the antiferromagnetic intercalated transition metal dichalcogenide Fe1/3NbS2 have demonstrated reversible resistivity switching by application of orthogonal current pulses below its magnetic ordering temperature, making Fe1/3NbS2 promising for spintronics applications. Here, we perform density functional theory calculations with Hubbard U corrections of the magnetic order, electronic structure, and transport properties of crystalline Fe1/3NbS2, clarifying the origin of the different resistance states. The two experimentally proposed antiferromagnetic ground states, corresponding to in-plane stripe and zigzag ordering, are computed to be nearly degenerate. In-plane cross sections of the calculated Fermi surfaces are anisotropic for both magnetic orderings, with the degree of anisotropy sensitive to the Hubbard U value. The in-plane resistance, computed within the Kubo linear response formalism using a constant relaxation time approximation, is also anisotropic, supporting a hypothesis that the current-induced resistance changes are due to a repopulating of antiferromagnetic domains. Our calculations indicate that the transport anisotropy of Fe1/3NbS2 in the zigzag phase is reduced relative to stripe, consistent with the relative magnitudes of resistivity changes in experiment. Finally, our calculations reveal the likely directionality of the current-domain response, specifically, which domains are energetically stabilized for a given current direction.