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    Stoichiometry-controlled structural order and tunable antiferromagnetism in FexNbSe2 (0.05≤x≤0.38)

    Xiaotong Xu1, Bei Jiang1, Runze Wang1, Zhibin Qiu2,3, Shu Guo2,3, Baiqing Lv1,4,5, and Ruidan Zhong1,5,*

    • *Contact author: rzhong@sjtu.edu.cn

    Phys. Rev. B 113, 134420 – Published 13 April, 2026

    DOI: https://doi.org/10.1103/c87z-wrhj

    Abstract

    Transition metal dichalcogenides (TMDs) enable magnetic property engineering via intercalation, but stoichiometry-structure-magnetism correlations remain poorly defined for Fe-intercalated NbSe2. Here, we report a systematic study of FexNbSe2 across an extended composition range 0.05≤x≤0.38, synthesized via chemical vapor transport and verified by rigorous energy-dispersive x-ray spectroscopy (EDS) microanalysis. X-ray diffraction, magnetic, and transport measurements reveal an intrinsic correlation between Fe content, structural ordering, and magnetic ground states. With increasing x, the system undergoes a successive transition from paramagnetism to a spin-glass state, then to long-range antiferromagnetism (AFM), and ultimately to a reentrant spin-glass phase, with the transition temperatures exhibiting a nonmonotonic dependence on Fe content. The maximum Néel temperature (TN=175K) and strongest AFM coupling occur at x=0.25, where Fe atoms form a well-ordered 2a0×2a0 superlattice within van der Waals gaps. Beyond x=0.25, the superlattice transforms or disorders, weakening Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions and significantly reducing TN. Electrical transport exhibits distinct anomalies at magnetic transition temperatures, corroborating the magnetic state evolution. Our work extends the compositional boundary of Fe-intercalated NbSe2, establishes precise stoichiometry-structure-magnetism correlations, and identifies structural ordering as a key tuning parameter for AFM. These findings provide a quantitative framework for engineering altermagnetic or switchable antiferromagnetic states in van der Waals materials.

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