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Layered transition metal dichalcogenides (TMDCs) host a plethora ofinteresting physical phenomena ranging from charge order to superconductivity.By introducing magnetic ions into 2H-NbS$_2$, the material forms a family ofmagnetic intercalated TMDCs T$_x$NbS$_2$ (T = 3d transition metal). Recently,Fe$_{1/3+\delta}$NbS$_2$ has been found to possess intriguing resistanceswitching and magnetic memory effects coupled to the N\'{e}el temperature ofT$_N \sim 45$ K [1,2]. We present comprehensive single crystal neutrondiffraction measurements on under-intercalated ($\delta \sim -0.01$),stoichiometric, and over-intercalated ($\delta \sim 0.01$) samples. Magneticdefects are usually considered to suppress magnetic correlations and,concomitantly, transition temperatures. Instead, we observe highly tunablemagnetic long-ranged states as the Fe concentration is varied fromunder-intercalated to over-intercalated, that is from Fe vacancies to Feinterstitials. The under- and over- intercalated samples reveal distinctantiferromagnetic stripe and zig-zag orders, associated with wave vectors $k_1$= (0.5, 0, 0) and $k_2$ = (0.25, 0.5, 0), respectively. The stoichiometricsample shows two successive magnetic phase transitions for these two wavevectors with an unusual rise-and-fall feature in the intensities connected to$k_1$. We ascribe this sensitive tunability to the competing next nearestneighbor exchange interactions and the oscillatory nature of theRuderman-Kittel-Kasuya-Yosida (RKKY) mechanism. We discuss experimentalobservations that relate to the observed intriguing switching resistancebehaviors. Our discovery of a magnetic defect tuning of the magnetic structurein bulk crystals Fe$_{1/3+\delta}$NbS$_2$ provides a possible new avenue toimplement controllable antiferromagnetic spintronic devices.

Highly tunable magnetic phases in transition metal dichalcogenide Fe$_{1/3+\delta}$NbS$_2$